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Review
Novel advances in metal-based solar absorber for photothermal vapor generation
Zhengtong Li, Chengbing Wang
2020, 31(9): 2159-2166  doi: 10.1016/j.cclet.2019.09.030
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摘要:
Access to safe drinking water has become an extremely urgent research topic worldwide. In recent years, the technology of solar vapor generation has been extensively explored as a potential and effective strategy of transforming elements content in seawater. In this review, the basic concepts and theories of metal-based photothermal vapor generation device (PVGD) with excellent optical and thermal regulatory are introduced. In the view of optical regulation, how to achieve high-efficiency localized evaporation in different evaporation system (i.e., volumetric solar heating and interface solar heating) is discussed; from the aspect of thermal regulation, the importance of selective absorption surface for interfacial PVGD is analyzed. Based on the above discussion and analysis, we summarize the challenges of metal-based desalination device.
Progress on multiphase layered transition metal oxide cathodes of sodium ion batteries
Qi Wang, Shiyong Chu, Shaohua Guo
2020, 31(9): 2167-2176  doi: 10.1016/j.cclet.2019.12.008
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As one of the most promising secondary batteries in large-scale energy storage, sodium ion batteries (SIBs) have attracted wide attention due to the abundant raw materials and low cost. Layered transition metal oxides are one kind of popular cathode material candidates because of its easy synthesis and large theoretical specific capacity. Yet, the most common P2 and O3 phases show distinct structural characteristics respectively. O3 phase can serve as a sodium reservoir, but it usually suffers from serious phase transition and sluggish kinetics. For the P2 phase, it allows the fast sodium ion migration in the bulk and the structure can maintain stable, but it is lack of sodium, showing a great negative effect on Coulombic efficiency in full cell. Thus, single phase structure almost cannot achieve satisfied comprehensive sodium storage performances. Under these circumstances, exploiting novel multiphase cathodes showing synergetic effect may give solution to these problems. In this review, we summarize the recent development of multiphase layered transition metal oxide cathodes of SIBs, analyze the mechanism and prospect the future potential research directions.
Research progress on transition metal oxide based electrode materials for asymmetric hybrid capacitors
Meizhen Dai, Depeng Zhao, Xiang Wu
2020, 31(9): 2177-2188  doi: 10.1016/j.cclet.2020.02.017
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In the past few years, the increasing energy consumption of traditional fossil fuels has posed a huge threat to human health. It is very imperious to develop the sustainable and renewable energy storage and conversion devices with low cost and environment friendly features. Hybrid supercapacitors are emerging as one of the promising energy devices with high power density, fast charge-discharge process and excellent cycle stability. However, morphology and structure of the electrode materials exert serious effect on their electrochemical performances. In this review, we summarized recent progresses in transition metal oxide based electrode materials for supercapacitors. Different synthesis routes and electrochemical performances of electrode materials and storage mechanisms of supercapacitor devices have been presented in details. The future developing trends of supercapacitor based on metal oxide electrode materials are also proposed.
Metal-organic framework membranes: From synthesis to electrocatalytic applications
Xiaobang Liu, Ting Yue, Kai Qi, Yubing Qiu, Bao Yu Xia, Xingpeng Guo
2020, 31(9): 2189-2201  doi: 10.1016/j.cclet.2019.12.009
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Metal-organic frameworks (MOFs), as an emerging family of porous inorganic-organic crystal materials, exhibit widely applications in gas storage and separation, drug release, sensing, and catalysis, owing to easily adjustable pore sizes, uniformly distributed metal centers, high surface areas, and tunable functionalities. However, MOF crystal powders are usually difficult to be directly applied into specific devices because of their brittleness, insolubility and low compatibility. Therefore, to expand versatile MOF membranes with robustness and operational flexibility is urgent to satisfy practical applications. Although numerous reports have reviewed the synthesis and applications of MOF membranes, relatively few reports the electrocatalytic properties based on MOF membranes. Herein, this mini-review provides an overview of preparation of MOF membranes, including directed synthesis, secondary growth and electrochemical deposition method. Meanwhile, fabrication of ultrathin 2D MOF nanosheets those can be also defined as a kind of nanoscale MOF membranes is also mentioned. Electrocatalytic performance of oxygen reduction reaction (ORR), oxygen evolution reaction (OER), hydrogen evolution reaction (HER) and CO2 reduction reaction (CO2RR) for diverse MOF membranes/nanosheets and their derivatives are introduced.
Chemical protein synthesis-assisted high-throughput screening strategies for D-peptides in drug discovery
Ying Li, Xiuxiu Cao, Changlin Tian, Ji-Shen Zheng
2020, 31(9): 2365-2374  doi: 10.1016/j.cclet.2020.04.015
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D-peptides are recognized as a new class of synthetic chemical drugs and they possess many interesting advantages such as high enzymatic stability, improved oral bioavailability, as well as high binding affinity and specificity. Recently, D-peptide drugs have been attracting increasing attention in both academic and industrial researches over recent years. One D-peptide etelcalcetide has even entered the market that targets the calcium (Ca2+)-sensing receptor (CaSR) to fight secondary hyperparathyroidism. Effective discovery and optimization of D-peptide ligands that can bind to various disease-related targets with high specificity and potency is of great importance for the development of D-peptide drugs. This review surveys the recent method development in this area especially the chemical protein synthesis-assisted high-throughput screening strategies for D-peptide ligands and their application in drug discovery.
Energetic materials based on poly furazan and furoxan structures
Junlin Zhang, Jing Zhou, Fuqiang Bi, Bozhou Wang
2020, 31(9): 2375-2394  doi: 10.1016/j.cclet.2020.01.026
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Furazan and furoxan represent fascinating explosophoric units with intriguing structures and unique properties. Compared with other nitrogen-rich heterocycles, most poly furazan and furoxan-based heterocycles demonstrate superior energetic performances due to the higher enthalpy of formation and density levels. A large variety of advanced energetic materials have been achieved based on the combination of furazan and furoxan moieties with different kinds of linkers and this review provides an overview of the development of energetic poly furazan and furoxan structures during the past decades, with their physical properties and detonation characteristics summarized and compared with traditional energetic materials. Various synthetic strategies towards these compact energetic structures are highlighted by covering the most important cyclization methods for construction of the hetercyclic scaffolds and the following modifications such as nitrations and oxidations. Given the synthetic availabilities and outstanding properties, energetic materials based on poly furazan and furoxan structures are undoubtedly listed as a promising candidate for the development of new-generation explosives, propellants and pyrotechnics.
Continuous-flow photochemistry: An expanding horizon of sustainable technology
Jingli Xie, Dongyuan Zhao
2020, 31(9): 2395-2400  doi: 10.1016/j.cclet.2020.03.022
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Understanding the unique characteristics of continuous-flow photochemistry will lead to a paradigm shift in the way we enhance sustainability and wellbeing. In this mini-review, we first provide a succinct overview of working principles of this technique and discuss several recent synthetic protocols. Then, emphasis is given to those representative examples which address environmental issues such as indoor air pollutants and water contamination. Finally, recent progress made using this technique to deal with rising CO2 emission, solar energy utilization and biomedical equipment is described. It is believed that this mini-review could inspire more chemists to utilize this technique in their research, either in the academic or industrial field.
Fluorine-containing drugs approved by the FDA in 2019
Haibo Mei, Attila Márió Remete, Yupiao Zou, Hiroki Moriwaki, Santos Fustero, Lorand Kiss, Vadim A. Soloshonok, Jianlin Han
2020, 31(9): 2401-2413  doi: 10.1016/j.cclet.2020.03.050
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Eleven new fluorine-containing FDA-approved drugs have been profiled and details of their discovery and preparation are discussed. Therapeutic areas include schizophrenia, migraine, multiple sclerosis, insomnia, rheumatoid arthritis, anti-tuberculosis, breast cancer, lymphoma kinase inhibitor, serotonin receptor antagonist. New pharmaceuticals feature four examples of aromatic fluorine, three aromatic CF3 group, three aliphatic CF3 and one compound with aromatic CF3O group. Furthermore, among the new compounds, six are chiral and seven are derived from tailor-made amino acids.
Ionic current rectification in asymmetric nanofluidic devices
Yue Zhou, Xuewei Liao, Jing Han, Tingting Chen, Chen Wang
2020, 31(9): 2414-2422  doi: 10.1016/j.cclet.2020.05.033
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In recent decades, the properties and behaviors of nanofluidic devices have been widely explored in varied subjects such as engineering, physics, chemistry, and biology. Among the rich properties of nanofluidics, ionic current rectification (ICR) is a unique phenomenon arising from asymmetric nanofluidic devices with electric double layer (EDL) overlapped. The ICR property is especially useful in applications including energy conversion, mass separation, sea water purification and bioanalysis. In this review, the ICR property in nanofluidics as well as the underlying mechanism is demonstrated. The influencing factors concerning to the ICR property are systematically summarized. The asymmetric geometry as well as the charge distribution is in charge of the ICR behavior occurring in nanofluidic devices. This review is aimed at readers who are interested in the fundamentals of mass transport in nanofluidics in general, as well as those who are willing to apply nanofluidics in various research fields.
Communication
Hierarchical porous nanofibers of carbon@nickel oxide nanoparticles derived from polymer/block copolymer system
Wen Shang, Huanzhou Du, Yage Wu, Jianlin Xu, Fen Ran
2020, 31(9): 2202-2206  doi: 10.1016/j.cclet.2019.10.017
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The triblock copolymer (PAA-b-PAN-b-PAA) iSs prepared by reversible addition-fragmentation chain-transfer polymerization, and then blended with polymer (PAN) and metal hydroxide (Ni(OH)2) as a precursor for heat-treatment. A composite material of hierarchical porous nanofibers and nickel oxide nanoparticles (HPCF@NiO) is prepared by electrospinning combined with high-temperature carbonization. The effects of the ratio of PAA and PAA-b-PAN-b-PAA on the internal structure of nanofibers and their electrochemical properties as positive electrode materials are investigated. The experimental results show that when the ratio of PAA to PAA-b-PAN-b-PAA is 1.3 to 0.4, it has good pore structure and excellent electrochemical performance. At the current density of 1 A/g, the specific capacitance is 188.7 F/g and the potential window is -1 V to 0.37 V. The asymmetric supercapacitor assembled with activated carbon as the negative electrode materials has a specific capacitance of 21.2 F/g in 2 mol/L KOH and a capacitance retention of 85.7% after 12, 500 cycles at different current density.
Nanoreactors derived from silica-protection-assisted metal-organic framework
Ling Jin, Xiaxia Li, Chunsen Liu, Huan Pang
2020, 31(9): 2207-2210  doi: 10.1016/j.cclet.2019.08.044
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The construction of highly stable and regular nanoreactors is a major challenge. In this work, we use a facile template protection method to obtain ZIF-67@SiO2 (JS) and to encapsulate metal oxide nanoparticles (Co3O4) into nanoreactors (SiO2). ZIF-67 crystals provide a cobalt species; SiO2 was first used as a protective layer of ZIF-67 and then as a nanoreactor for metastable metal oxide nanoparticles. On this basis, Co3O4@SiO2 with dodecahedron morphology were synthesized by calcining JS at different temperatures, followed by a hydrothermal reaction to obtain Co3(OH)4Si2O5. Subsequently, CoSx and CoPSiO2 were fabricated through sulfuration and phosphorization. The results in this work show that nanoreactors derived from metal-organic frameworks (MOFs) with a rational structure have broad development prospects.
A highly stable, luminescent and layered zinc(Ⅱ)-MOF: Iron(Ⅲ)/copper(Ⅱ) dual sensing and guest-assisted exfoliation
Xiu Qian, Siyu Deng, Xiang Chen, Qiang Gao, Yun-Long Hou, Aiwu Wang, Lizhuang Chen
2020, 31(9): 2211-2214  doi: 10.1016/j.cclet.2019.09.024
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A highly stable and luminescent metal-organic framework (LMOF) with layered structure, namely, C6H4N5OZn (1) has been successfully achieved and fully characterized by single crystal X-ray diffraction, powder X-ray diffractions, fluorescence titration and thermogravimetry. This blue-light emitting compound 1 exhibit outstanding stability and can detect Fe3+ and Cu2+ in water specifically, presenting potential application in the field of fluorescent probe technology. Fluorescence titration experiments indicate that the detection of Fe3+ ions by 1 is more significant than that of Cu2+ ions in terms of Ksv value. Furthermore, guest-assisted exfoliation of layered MOF 1 is efficiently carried out through ether O—H hydrogen bond or ππ interactions between the layered host structure and intercalated guest molecules (4, 4'-oxybisbenzoic acid and triphenylamine). Tyndal scattering was observed in the suspensions of obtained MOF nanosheets. This study shows that the compound 1 with unique metal ion sensing properties can be applied as a probe material in water pollution treatment field, but also opens up the opportunity for synthesizing luminescent MONs through the "bottom-up" guest intercalation methodology.
A high-performance potassium-ion capacitor based on a porous carbon cathode originated from the Aldol reaction product
Xu Yu, Mingjie Shao, Xuemei Yang, Chongxing Li, Tong Li, Danyu Li, Rutao Wang, Longwei Yin
2020, 31(9): 2215-2218  doi: 10.1016/j.cclet.2019.11.012
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Potassium-ion capacitors (KICs) emerge as a promising substitute for the well-developed lithium-ion capacitors (LICs), however, the energy density of KICs is below expectations because of lacking a suitable electrical double-layer positive electrode. Using chemical activation of the Aldol reaction product of acetone with KOH, we synthesized a porous carbon with a Brunauer-Emmett-Teller surface area of up to 2947 m2/g and a narrow pore size distribution ranging from 1 nm to 3 nm. Half-cell (versus potassium metal) test demonstrates that this porous carbon has high capacitive performance in K+ based organic electrolytes. Furthermore, a novel KIC fabricated by this porous carbon as the cathode, yields high values of energy density and power density. The processes used to make this porous carbon are readily low-cost to fabricate metal-ion capacitors.
High-performance nitrogen and sulfur co-doped nanotube-like carbon anodes for sodium ion hybrid capacitors
Yongqiang Ding, Yali Li, Junshuai Li, Xingbin Yan
2020, 31(9): 2219-2224  doi: 10.1016/j.cclet.2019.11.017
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Sodium ion hybrid capacitors are of great concern in large-scale and cost-effective electrical energy storage owing to their high energy and power densities, as well as natural abundance and wide distribution of sodium. However, it is difficult to find a well-pleasing anode material that matches the high-performance cathode materials to achieve good energy and power output for sodium ion hybrid capacitors. In this paper, nitrogen and sulfur co-doped nanotube-like carbon prepared by a simple carbonization process of high sulfur-loaded polyaniline nanotubes is introduced as the anode. The assembled sodium ion half cell based on the optimal nanotube-like carbon delivers a high reversible capacity of ~304.8 mAh/g at 0.2 A/g and an excellent rate performance of ~124.8 mAh/g at 10 A/g in a voltage window of 0.01-2.5 V (versus sodium/sodium ion). For the hybrid capacitors assembled using the optimal nanotube-like carbon as the anode and high-capacity activated carbon as the cathode, high energy densities of ~100.2 Wh/kg at 250 W/kg and ~50.69 Wh/kg at 12, 500 W/kg are achieved.
Carbon-coated Li3VO4 with optimized structure as high capacity anode material for lithium-ion capacitors
Wenjie Liu, Xiong Zhang, Chen Li, Kai Wang, Xianzhong Sun, Yanwei Ma
2020, 31(9): 2225-2229  doi: 10.1016/j.cclet.2019.11.015
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Due to the high capacity, moderate voltage platform, and stable structure, Li3VO4 (LVO) has attracted close attention as feasible anode material for lithium-ion capacitor. However, the intrinsic low electronic conductivity and sluggish kinetics of the Li+ insertion process severely impede its practical application in lithium-ion capacitors (LICs). Herein, a carbon-coated Li3VO4 (LVO/C) hierarchical structure was prepared by a facial one-step solid-state method. The synthesized LVO/C composite delivers an impressive capacity of 435 mAh/g at 0.07 A/g, remarkable rate capability, and nearly 100% capacity retention after 500 cycles at 0.5 A/g. The superior electrochemical properties of LVO/C composite materials are attributed to the improved conductivity of electron and stable carbon/LVO composite structures. Besides, the LIC device based on activated carbon (AC) cathode and optimal LVO/C as anode reveals a maximum energy density of 110 Wh/kg and long-term cycle life. These results provide a potential way for assembling the advanced hybrid lithium-ion capacitors.
Implanting Ni into N-doped puffed carbon: A new advanced electrocatalyst for oxygen evolution reaction
Feng Cao, Guoxiang Pan, Yujian Zhang, Xinhui Xia
2020, 31(9): 2230-2234  doi: 10.1016/j.cclet.2020.01.037
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Tailored design and synthesis of high-quality electrocatalysts is vital for the advancement of oxygen evolution reaction (OER). Herein, we report a powerful puffing method to fabricate hierarchical porous N-doped carbon with numerous embedded Ni nanoparticles. Interestingly, during the puffing and annealing process, rice precursor with N and Ni sources can be in-situ converted into Niembedded N-doped porous carbon (N-PC/Ni) composite. The obtained N-PC/Ni composite possesses a cross-linked porous architecture containing conductive carbon backbone and active Ni nanoparticles electrocatalysts for OER. The pore formation in N-PC/Ni composite is also proposed because of carbothermic reduction. The N-PC/Ni composite is fully studied as electrocatalysts for OER. Due to increased active surface area, enhanced electronic conductivity and reactivity, the designed N-PC/Ni composite exhibits superior OER performance with a low Tafel slope (~88 mV/dec) and a low overpotential as well as excellent long-term stability in alkaline solution. Our proposed rational design strategy may provide a new way to construct other advanced metal/heteroatom-doped composites for widespread application in electrocatalysis.
One-step synthesis of biomass derived O, N-codoped hierarchical porous carbon with high surface area for supercapacitors
Shuxian Sun, Fuqin Han, Xiaoliang Wu, Zhuangjun Fan
2020, 31(9): 2235-2238  doi: 10.1016/j.cclet.2019.11.023
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We report a convenient method to synthesize O, N-codoped hierarchical porous carbon by one-step carbonization of the mixture of KHCO3, urea and alginic acid. Benefiting from KHCO3 and urea synergistic effect, the obtained O, N-codoped hierarchical porous carbon (NPC-700) material has a well-developed interconnected porous framework with ultrahigh specific surface area (2846 m2/g) and massive heteroatoms functional groups. Consequence, such porous carbon displays high specific capacitance (324 F/g at 1 A/g), excellent rate performance (212 F/g at 30 A/g) and good electrochemical stabilization in 6 mol/L KOH solution. More importantly, the assembled NPC-700//NPC-700 symmetrical supercapacitor can achieve a high energy density of 18.8 Wh/kg and good electrochemical stabilization in 1 mol/L Na2SO4 solution. This process opens up a new way to design heteroatoms-doped hierarchical porous carbon derived from biomass materials for supercapacitors.
Nitrogen-doped carbon nanotubes by multistep pyrolysis process as a promising anode material for lithium ion hybrid capacitors
Juan Yang, Dan Xu, Ruilin Hou, Junwei Lang, Zhaoli Wang, Zhengping Dong, Jiantai Ma
2020, 31(9): 2239-2244  doi: 10.1016/j.cclet.2019.11.044
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Lithium-ion hybrid capacitors (LIHCs) is a promising electrochemical energy storage devices which combines the advantages of lithium-ion batteries and capacitors. Herein, we developed a facile multistep pyrolysis method, prepared an amorphous structure and a high-level N-doping carbon nanotubes (NCNTs), and by removing the Co catalyst, opening the port of NCNTs, and using NCNTs as anode material. It is shows good performance due to the electrolyte ions enter into the electrode materials and facilitate the charge transfer. Furthermore, we employ the porous carbon material (APDC) as the cathode to couple with anodes of NCNTs, building a LIHCs, it shows a high energy density of 173 Wh/kg at 200 W/kg and still retains 53 Wh/kg at a high power density of 10 kW/kg within the voltage window of 0-4.0 V, as well as outstanding cyclic life keep 80% capacity after 5000 cycles. This work provides an opportunity for the preparation of NCNTs, that is as a promising high-performance anode for LIHCs.
Melamine sponge derived porous carbon monoliths with NiMn oxides for high performance supercapacitor
Qianyuan Shan, Wangchen Huo, Man Shen, Chuan Jing, Yan Peng, Huayan Pu, Yuxin Zhang
2020, 31(9): 2245-2248  doi: 10.1016/j.cclet.2020.02.003
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Supercapacitors with good electrochemical performance and flexibility are in great demand. In this paper, the concept of preparing 3D porous carbon monoliths via direct calcination of melamine sponge is presented. This preparation method is simple and has good control of the structure. Porous carbon composite nickel-manganese oxides can be obtained by hydrothermal method followed with calcination. The electrochemical performances were tested and porous carbon monoliths with NiMn oxides exhibited a specific capacitance of 870 F/g in 1 mol/L KOH at a charge/discharge current density of 0.5 A/g and a capacity retention of 89.9% after 5000 times charge and discharge.
Bulk heterojunction perovskite solar cells incorporated with solution-processed TiOx nanoparticles as the electron acceptors
Tao Zhu, Yongrui Yang, Suyuan Zhou, Xiang Yao, Lei Liu, Wenping Hu, Xiong Gong
2020, 31(9): 2249-2253  doi: 10.1016/j.cclet.2020.02.004
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In the past ten years, perovskite solar cells were rapidly developed, but the intrinsic unbalanced charge carrier diffusion lengths within perovskite materials were not fully addressed by either a planar heterojunction or meso-superstructured perovskite solar cells. In this study, we report bulk heterojunction perovskite solar cells, where perovskite materials CH3NH3PbI3 is blended with solution-processed n-type TiOx nanoparticles as the photoactive layer. Studies indicate that one-step solution-processed CH3NH3PbI3:TiOx bulk-heterojunction thin film possesses enhanced and balanced charge carrier mobilities, superior film morphology with enlarged crystal sizes, and suppressed trapinduced charge recombination. Thus, bulk heterojunction perovskite solar cells by CH3NH3PbI3 mixed with 5 wt% of TiOx, which is processed by one-step method rather than typical two-step method, show a short-circuit current density of 20.93 mA/cm2, an open-circuit voltage of 0.90 V, a fill factor of 80% and with a corresponding power conversion efficiency of 14.91%, which is more than 30% enhancement as compared with that of perovskite solar cells with a planar heterojunction device structure. Moreover, bulk heterojunction perovskite solar cells possess enhanced device stability. All these results demonstrate that perovskite solar cells with a bulk heterojunction device structure are one of apparent approaches to boost device performance.
In-situ growth of hybrid NaTi8O13/NaTiO2 nanoribbons on layered MXene Ti3C2 as a competitive anode for high-performance sodium-ion batteries
Xuan Sun, Ke Tan, Yang Liu, Jinyang Zhang, Linrui Hou, Changzhou Yuan
2020, 31(9): 2254-2258  doi: 10.1016/j.cclet.2020.02.016
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In the work, we successfully explore a two-step hydrothermal method for scalable synthesis of the hybrid sodium titanate (NaTi8O13/NaTiO2) nanoribbons well in-situ formed on the multi-layered MXene Ti3C2 (designed as NTO/Ti3C2). Benefiting from the inherent structural and componential superiorities, the resulted NTO/Ti3C2 composite exhibits long-duration cycling stability and superior rate behaviors when evaluated as a hybrid anode for advanced SIBs, which delivers a reversible and stable capacity of ~82 mAh/g even after 1900 cycles at 2000 mA/g for SIBs.
Unstable Ni leaching in MOF-derived PtNi-C catalyst with improved performance for alcohols fuel electro-oxidation
Bo Fang, Zong Liu, Yufei Bao, Ligang Feng
2020, 31(9): 2259-2262  doi: 10.1016/j.cclet.2020.02.045
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Significance of unstable species leaching was for the first time demonstrated on MOF-derived catalysts by taking PtNi-C as an example, that was instructive for the relevant catalyst fabrication and performance study. PtNi-C catalyst was synthesized by combining Pt nanoparticles with Ni-BTC after annealing in the tube furnace and the unstable Ni species can be easily leached out in nitric acid, and the stable PtNi nanoparticles trapped in the graphite carbon layer were obtained. The greatly improved catalytic ability for alcohol fuels oxidation was verified by comparing the fresh and acid leached catalysts in terms of the high peak current density, specific and mass activity and rapid charge transfer kinetics and high catalytic stability. The current work guides the importance of unstable assistant promoter removal for the MOF derived catalysts.
Morphology and size controlled synthesis of Co-doped MIL-96 by different alkaline modulators for sensitively detecting alphafetoprotein
Chaonan Gu, Jingjing Li, Guang Yang, Liming Zhang, Chun-Sen Liu, Huan Pang
2020, 31(9): 2263-2267  doi: 10.1016/j.cclet.2020.02.044
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This work introduces a simple and facile approach for the morphology and size controlled synthesis of Co-doped MIL-96. By using different bases as modulators, Co-doped MIL-96 was obtained with sizes that varied from 5 μm to 300 nm, and four different morphologies, including hexagonal prism, icosahedron, hexagonal spindle and ellipsoid. Among these, nano-sized Co-doped MIL-96 with an ellipsoid morphology exhibited the highest electroactive surface area and good conductivity as well as the best electrochemical sensing performance towards α-fetoprotein.
High-performance Na1.25V3O8 nanosheets for aqueous zinc-ion battery by electrochemical induced de-sodium at high voltage
Di Xie, Fang Hu, Xin Yu, Fuhan Cui, Guihong Song, Kai Zhu
2020, 31(9): 2268-2274  doi: 10.1016/j.cclet.2020.02.052
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Aqueous rechargeable zinc-ion batteries (ARZIBs) are expected to replace organic electrolyte batteries owing to its low price, safe and environmentally friendly characteristics. Herein, we fabricated vanadium-based Na1.25V3O8 nanosheets as a cathode material for ARZIBs, which present a high performance by electrochemical de-sodium at high voltage to form Na2V6O16 phase in the first cycle: high capacity of 390 mAh/g at 0.1 A/g, high rate performance (162 mAh/g at 10 A/g) and superior cycle stability (179 mAh/g with a high capacity retention of 88.2% of the maximum capacity after 2000 cycles). In addition, the cell exhibits a high energy density of 416.9 Wh/kg at 143.6 W/kg, suggesting great potential of the as-prepared Na1.25V3O8 nanosheets for ARZIBs.
Synthesis of nickel selenide thin films for high performance all-solid-state asymmetric supercapacitors
Hao Li, Jiangfeng Gong, Jing-Chang Li, Xincheng Zhang, Chunmei Tang, Hongbing Yao, Qingping Ding
2020, 31(9): 2275-2279  doi: 10.1016/j.cclet.2020.03.010
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As a significant semiconductor, nickel selenide shows enormous potential and extensive application prospects in the field of sensor, photocatalysis and supercapacitor. In this paper, nickel selenide (Ni3Se2, NiSe) thin films were successfully fabricated on stainless-steel sheet using a facile, effective electrodeposition technique. The morphologies, microstructures and chemical compositions of the thin films are characterized systematically. Electrochemical tests exhibit that the Ni3Se2 and NiSe possess high specific capacitance of 581.1 F/g and 1644.7 F/g, respectively. A flexible, all-solid-state asymmetric supercapacitor is assembled by utilizing NiSe film as positive electrode and activated carbon as negative electrode. The solid device delivers a high areal capacitance of 27.0 mF/cm2 at the current density of 0.7 mA/cm2. The maximum volumetric energy density and power density of the NiSe//AC asymmetric SCs can achieve 0.26 mWh/cm3 and 33.35 mW/cm3, respectively. The device shows robust cycling stability with 84.6% capacitance retention after 10, 000 cycles, outstanding flexibility and satisfactory mechanical stability. Moreover, two devices in series can light up a red light-emitting diode, which displayed great potential applications for energy storage.
Design and synthesis of nitrogen-doped hexagonal NiCoO nanoplates derived from Ni-Co-MOF for high-performance electrochemical energy storage
Yan Li, Yuying Shan, Huan Pang
2020, 31(9): 2280-2286  doi: 10.1016/j.cclet.2020.03.027
[摘要]  (176) [HTML全文] (176) [PDF 5755KB] (5)
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In order to further improve the potential application of nickel-cobalt oxide (NiCoO) in supercapacitors, we use controlled calcination of different Ni-Co-MOF ([NiCo(HBTC)(4, 4'-bipy)]) composites to obtain five kinds of nickel doped NiCoO (N-NiCoO) with different Ni/Co molar ratio. These N-NiCoO materials with unique hexagonal nanoplates structure, high specific surface area and high porosity indicate high and stable electrochemical activity. In particular, N-NiCoO-2 with a Ni/Co molar ratio of 2:1 exhibits the highest 945.79 F/g specific capacitance at 1 A/g and a high cycle stability of only 6.7% attenuation after 5000 cycles. Apart from the certain percentage of NiCoO with higher conductivity, nitrogen doping provides more reactive sites and the specific porous hexagonal nanoplates structure of the product itself accelerate electron transfer and promote electrolyte diffusion can more effectively enhance the electrochemical performance. Therefore, N-NiCoO synthesized via a simple method exhibit exciting potential and can be used as an electrode material for supercapacitors with good performance.
Construction of SiO2-TiO2/g-C3N4 composite photocatalyst for hydrogen production and pollutant degradation: Insight into the effect of SiO2
Sijia Sun, Hao Ding, Lefu Mei, Ying Chen, Qiang Hao, Wanting Chen, Zhuoqun Xu, Daimei Chen
2020, 31(9): 2287-2294  doi: 10.1016/j.cclet.2020.03.026
[摘要]  (183) [HTML全文] (183) [PDF 7875KB] (4)
摘要:
Using low-cost precipitated silica (SiO2) as the carrier, a ternary SiO2-TiO2/g-C3N4 composite photocatalyst was prepared via the sol-gel method associated with a wet-grinding process. The as-prepared composite exhibits photocatalytic hydrogen production and pollutant degradation performance under solar-like irradiation. The effect of SiO2 carrier on the properties of the heterostructure between TiO2 and g-C3N4 (CN) was systematically studied. It is found that SiO2 has important effects on promoting the interaction between TiO2 and CN. The particle size of TiO2 and CN was obviously reduced during the calcination process due to the effects of SiO2. Especially, the TiO2 particles exhibit monodispersed state with particle size below 10 nm (quantum dots), resulting in the improvement of the contact area and the interaction betweenTiO2 and CN, and leading to the formation of efficient TiO2/CN Z-scheme heterostructure in SiO2-TiO2/CN. Besides, the introduction of SiO2 can increase the specific surface area and light absorption of SiO2-TiO2/CN, further promoting the photocatalytic reaction. As expected, the optimum SiO2-TiO2/CN composite exhibits 12.3, 3.1 and 2.9 times higher photocatalytic hydrogen production rate than that of SiO2-TiO2, CN and TiO2/CN under solar-like irradiation, while the photocatalytic active component in SiO2-TiO2/CN is only about 60 wt%. Moreover, the rhodamine B degradation rate of SiO2-TiO2/CN is also higher than that of SiO2-TiO2, CN and TiO2/CN.
Metal-organic framework derived Co3O4/PPy bifunctional electrocatalysts for efficient overall water splitting
Yongli Tong, Hengqi Liu, Meizhen Dai, Li Xiao, Xiang Wu
2020, 31(9): 2295-2299  doi: 10.1016/j.cclet.2020.03.029
[摘要]  (147) [HTML全文] (147) [PDF 6303KB] (2)
摘要:
In this work, we report Co3O4@PPy hybrid structured electrode materials for overall water splitting. The as-synthesized Co3O4/PPy-120 samples present excellent electrocatalytic performances for OER and HER and long durability. It only requires an operating potential of 1.67 V to deliver a current density of 10 mA/cm2 with a remarkable durability for 28 h. The superior electrocatalytic performances mainly can be attributed to the unique heterostructures and the synergistic effects between PPy and Co3O4 electrode materials.
CoP@SiO2nanoreactors: A core-shell structure for efficient electrocatalytic oxygen evolution reaction
Ling Jin, Huan Pang
2020, 31(9): 2300-2304  doi: 10.1016/j.cclet.2020.03.041
[摘要]  (132) [HTML全文] (132) [PDF 4862KB] (2)
摘要:
Metallic phosphides as a crucial class of metal-like compounds show high electric conductivity and electrochemical properties. It is of significant benefit to understanding the relationship between the electrocatalytic performance and phosphating degree of precursors. In this work, using Co3O4@SiO2 as precursor, core-shell structured CoP@SiO2 nanoreactors with outstanding oxygen evolution reaction performance were synthesized through a facile calcination method. The electrocatalytic performance of CoP@SiO2 modified electrode that treated with 500 mg NaH2PO2 was greatly enhanced. The obtained product displays a low overpotential of 280 mV at a current density of 10 mA/cm2 and a Tafel value 89 mV/dec in alkaline conditions. The easy available CoP@SiO2 with outstanding catalytic performance and stability possesses huge potential in future electrochemical applications.
3D crumbled MXene for high-performance supercapacitors
Xin Zhang, Jiawei Miao, Peng Zhang, Qizhen Zhu, Mingchi Jiang, Bin Xu
2020, 31(9): 2305-2308  doi: 10.1016/j.cclet.2020.03.040
[摘要]  (146) [HTML全文] (146) [PDF 4122KB] (3)
摘要:
MXene materials have recently attracted considerable attention in energy storage application owing to their metallic conductivity, 2D structure and tunable surface terminations. However, the restacking of 2D MXene nanosheets hinders the ion transport and accessibility to the surface, resulting in adverse effect on their electrochemical performances. Here, with the assistance of hexamethylenetetramine (C6H12N4), 2D Ti3C2Tx MXene nanosheets were fabricated into a 3D architecture with crumbled and porous structure through an electrostatic self-assembly followed by annealing. The resultant 3D structure can expose massive active sites and facilitates the ion transport, which is beneficial for sufficient utilization of the outstanding superiorities of the MXene. Therefore, as a pseudocapacitive material, the 3D crumpled and porous Ti3C2Tx MXene shows a gravimetric capacitance of 333 F/g at 1 A/g, and maintains 261 F/g and 132 F/g at ultrahigh current densities of 100 A/g and 1000 A/g, respectively, revealing promising potential for application in supercapacitors.
A conductive anionic Co-MOF cage with zeolite framework for supercapacitors
Wei Du, Yue-Ling Bai, Zhen Yang, Runlong Li, Dan Zhang, Zhiheng Ma, Anbao Yuan, Jiaqiang Xu
2020, 31(9): 2309-2313  doi: 10.1016/j.cclet.2020.04.017
[摘要]  (146) [HTML全文] (146) [PDF 3152KB] (3)
摘要:
Conductive MOFs could exhibit full potential as integrated electrode materials for supercapacitors without interference from additional conductive additives. Here we report an anionic Co-MOF cage with zeolite framework, which was balanced by the redox-active guest [Co(H2O)6]2+ and protonated [(CH3)2NH2]2+ ions. Benefit from the unique ion skeleton structure, Co-MOF exhibits a conductivity higher than most of reported MOFs with the value of 1.42×10-3 S/cm, which can be directly fabricated as electrode for supercapacitors. A maximum specific capacitance of 236.2 F/g can be achieved at a current density of 1 A/g of Co-MOF. Additionally, the electric performance and morphology of this Co-MOF can be modified by cetyltrimethylammonium bromide (CTAB) and the maximum specific capacitance could increase up to 334 F/g at 1 A/g when the ratio of ligand and CTAB is 1:6 (Co-MOF-6). Furthermore, the specific capacitance can retain at 64.04% and 77.92% of the initial value after 3000 cycles of Co-MOF and Co-CTAB-6, respectively. Obviously, the addition of CTAB further improves both capacitance and cycle stability.
Sodium-based dual-ion batteries via coupling high-capacity selenium/graphene anode with high-voltage graphite cathode
Xiankun Hou, Wenhao Li, Yingying Wang, Shaofang Li, Yunfeng Meng, Haiyue Yu, Baokuan Chen, Xinglong Wu
2020, 31(9): 2314-2318  doi: 10.1016/j.cclet.2020.04.021
[摘要]  (150) [HTML全文] (150) [PDF 9662KB] (1)
摘要:
Dual ion batteries (DIBs) exhibit broad application prospects in the field of electrical energy storage (EES) devices with excellent properties, such as high voltage, high energy density, and low cost. In the graphitebased DIBs, high voltage is needed to store enough anions with the formation of anion intercalation compound XCn (X = AlCl4-, PF6-, TFSI-, etc.). Hence, it is difficult for graphite-based DIBs to match proper anodes and electrolytes. Here, an Se/graphene composite is prepared via a convenient method, and assembled into a dual-ion full battery (DIFB) as anode with graphite cathode and 1 mol/L NaPF6 in EC: EMC (1:1, v:v). This DIFB has achieved a high discharge capacity of 75.9 mAh/g and high medium output voltage of 3.5 V at 0.1 A/g. Actually, the suitable anode materials, such as the present Se/graphene composite, are extremely important for the development and application of graphite-based DIBs. This study is enlightening for the design of future low-cost EES devices including graphite-based DIBs.
Insights into the photocatalytic mechanism of the C4N/MoS2 heterostructure: A first-principle study
Rui Zhang, Wei Jian, Zhao-Di Yang, Fu-Quan Bai
2020, 31(9): 2319-2324  doi: 10.1016/j.cclet.2020.04.055
[摘要]  (142) [HTML全文] (142) [PDF 4842KB] (1)
摘要:
Constructing heterostructures by combining COFs and TMD is a new strategy to design efficient photocatalysts for CO2 reduction reaction (CO2RR) due to their good stability, tunable band gaps and efficient charge separation. Based on the synthesis of completely novel C4N-COF in our previous reported work, a new C4N/MoS2 heterostructure was constructed and then the related structural, electronic and optical properties were also studied using first principle calculations. The interlayer coupling effect and charge transfer between the C4N and MoS2 layer are systematically illuminated. The reduced band gap of the C4N/MoS2 heterostructure is beneficial to absorb more visible light. For the formation of type-Ⅱ band alignment, a built-in electric field appears which separates the photogenerated electrons and holes into different layers efficiently and produces redox active sites. The band alignment of the heterostructure ensures its photocatalytic activities of the whole CO2 reduction reaction. Furthermore, the charge density difference and charge carrier mobility confirm the existence of the built-in electric field at the interface of the C4N/MoS2 heterostructure directly. Finally, the high optical absorption indicates it is an efficient visible light harvesting photocatalyst. Therefore, this work could provide strong insights into the internal mechanism and high photocatalytic activity of the C4N/MoS2 heterostructure and offer guiding of designing and synthesizing COF/TMD heterostructure photocatalysts.
Two-dimensional 1T-PS2 as a promising anode material for sodium-ion batteries with ultra-high capacity, low average voltage and appropriate mobility
Dawei Zhou, Chunping Li, Furong Yin, Xin Tang, Chunying Pu, Chaozheng He
2020, 31(9): 2325-2329  doi: 10.1016/j.cclet.2020.04.045
[摘要]  (141) [HTML全文] (141) [PDF 3358KB] (2)
摘要:
As electrodes, two-dimensional materials show special advantages including the infinite planar lengths, broad electrochemical window, large surface-volume ratio, and much exposed active sites. In theory, the two-dimensional materials consist of the elements with high electronegativity may absorb more Na atoms, resulting in a high battery storage capacity. Based on the above idea, we selected the two dimensional metallic PS2 with 1T-Type structure as an anode material, and explored its potential applications as an electrode material for Na-ion battery through first-principle calculations. As we expected, when two dimensional PS2 is used as an anode in Na-ion battery, it can adsorb maximum three layers of sodium atoms on both sides of the monolayer, resulting in a maximum theoretical capacity of 1692 mAh/g. Furthermore, it also possesses a rather small sodium diffusion barrier of 0.17 eV, a low average open-circuit voltage of 0.18 V, and a relatively small lattice changes within 13% during the intercalation of Na. These results suggested that the two dimensional PS2 is a potentially excellent Na-ion battery anode. Our idea of designing two-dimensional anode materials with high storage capacity may provide some references for designing the next generation anode materials of metal-ion batteries.
CeO2 quantum dots doped Ni-Co hydroxide nanosheets for ultrahigh energy density asymmetric supercapacitors
Huiyu Duan, Tong Wang, Xinyi Wu, Ziyun Su, Jing Zhuang, Suli Liu, Rongmei Zhu, Changyun Chen, Huan Pang
2020, 31(9): 2330-2332  doi: 10.1016/j.cclet.2020.06.001
[摘要]  (151) [HTML全文] (151) [PDF 3225KB] (4)
摘要:
By integrating the merits of lanthanide elements and quantum dots, we firstly design CeO2 quantum dots doped Ni-Co hydroxide nanosheet via a controllable synthetic strategy, which exhibits a large specific capacitance (1370.7 F/g at 1.0 A/g) and a good cyclic stability (90.6% retention after 4000 cycles). Moreover, we assemble an aqueous asymmetric supercapacitor with the obtained material, which has an extremely high energy density (108.9 Wh/kg at 378 W/kg) and outstanding cycle stability (retaining 88.1% capacitance at 2.0 A/g after 4000 cycles).
Multilayered structure of N-carbonenvelopediron oxide/graphene nanocomposites as an improved anode for Li-ion battery
Li Sun, Kai Wang, Ningning Li, Jun Zhang, Xiangxin Guo, Xianghong Liu
2020, 31(9): 2333-2338  doi: 10.1016/j.cclet.2020.02.006
[摘要]  (141) [HTML全文] (141) [PDF 8492KB] (2)
摘要:
Transition metal oxides with high capacity are considered a promising electrode material for lithium-ion batteries (LIBs). Nevertheless, the huge volume expansion and poor conductivity severely hamper their practical application. In this work, a carbon riveting method is reported to address the above issues by designing multilayered N-doped carbon (N-carbon) enveloped Fe3O4/graphene nanosheets. When evaluated as a negative electrode, the N-carbon/Fe3O4/graphene nanocomposites demonstrate greatly enhanced electrochemical properties compared with Fe3O4/graphene. The N-carbon/Fe3O4/graphene presents a superior reversible capacity (807 mAh/g) over Fe3O4/graphene (540 mAh/g). Furthermore, it affords a considerable capacity of 550 mAh/g at 1 A/g over 700 cycles, indicating superb cycling stability. The structure-property correlation studies reveal that the carbon riveting layer is essential for enhancing the lithium diffusion kinetics. The good electrochemical properties and effective structure design make the carbon riveting strategy quite general and reliable to manipulate high performance electrodes for future LIBs.
Integrated lithium metal anode protected by composite solid electrolyte film enables stable quasi-solid-state lithium metal batteries
Junfan Ding, Rui Xu, Chong Yan, Ye Xiao, Yeru Liang, Hong Yuan, Jiaqi Huang
2020, 31(9): 2339-2342  doi: 10.1016/j.cclet.2020.03.015
[摘要]  (146) [HTML全文] (146) [PDF 3464KB] (1)
摘要:
Lithium (Li) metal, possessing an extremely high theoretical specific capacity (3860 mAh/g) and the most negative electrode potential (-3.040 V vs. standard hydrogen electrode), is one the most favorable anode materials for future high-energy-density batteries. However, the poor cyclability and safety issues induced by extremely unstable interfaces of traditional liquid Li metal batteries have limited their practical applications. Herein, a quasi-solid battery is constructed to offer superior interfacial stability as well as excellent interfacial contact by the incorporation of Li@composite solid electrolyte integrated electrode and a limited amount of liquid electrolyte (7.5 μL/cm2). By combining the inorganic garnet Aldoped Li6.75La3Zr1.75Ta0.25O12 (LLZO) with high mechanical strength and ionic conductivity and the organic ethylene-vinyl acetate copolymer (EVA) with good flexibility, the composite solid electrolyte film could provide sufficient ion channels, sustained interfacial contact and good mechanical stability at the anode side, which significantly alleviates the thermodynamic corrosion and safety problems induced by liquid electrolytes. This innovative and facile quasi-solid strategy is aimed to promote the intrinsic safety and stability of working Li metal anode, shedding light on the development of next-generation high-performance Li metal batteries.
MnO2-directed synthesis of NiFe-LDH@FeOOH nanosheeet arrays for supercapacitor negative electrode
Qing Sun, Kexin Yao, Yuxin Zhang
2020, 31(9): 2343-2346  doi: 10.1016/j.cclet.2020.03.069
[摘要]  (150) [HTML全文] (150) [PDF 3446KB] (1)
摘要:
The complex-architectured NiFe-LDH@FeOOH negative material was first prepared by simple two-step hydrothermal method. In this study, the porous nanostructure of FeOOH nanosheets features a large number of accessible channels to electroactive sites and the two-dimensional layered structure of NiFe-LDH nanosheets have an open spatial structure with high specific surface area, which enhance the diffusion of ions in the active material. Benefited from above advantages, the excellent electrochemical properties were demonstrated. NiFe-LDH@FeOOH nanocomposites present high specific capacitance (1195 F/g at a current density of 1 A/g), lower resistance and well cycling performance (90.36% retention after 1000 cycles). Furthermore, the NiFe-LDH@MnO2//NiFe-LDH@FeOOH supercapacitor exhibits 22.68 Wh/kg energy density at 750 W/kg power density, demonstrating potential application in energy storage devices.
Bimetal-organic frameworks derived Co/N-doped carbons for lithium-sulfur batteries
Shifang Jiang, Shuo Huang, Minjie Yao, Jiacai Zhu, Lili Liu, Zhiqiang Niu
2020, 31(9): 2347-2352  doi: 10.1016/j.cclet.2020.04.014
[摘要]  (154) [HTML全文] (154) [PDF 4288KB] (1)
摘要:
Lithium-sulfur (Li-S) batteries have received extensive attention due to their high theoretical specific energy density. However, the utilization of sulfur is seriously reduced by the shuttle effect of lithium polysulfides and the low conductivity of sulfur and lithium sulfide (Li2S). Herein, we introduced bimetalorganic frameworks (Co/Zn-ZIF) derived cobalt and nitrogen-doped carbons (Co/N-C) into Li-S batteries through host design and separator modification. The Co/N-C in Li-S batteries effectively limits the shuttle effect through simultaneously serving as polysulfide traps and chemical catalyst. As a result, the Li-S batteries deliver a high reversible capacity of 1614.5 mAh/g and superior long-term cycling stability with a negligible capacity decay of only 0.04% per cycle after 1000 cycles. Furthermore, they have a high area capacity of 5.5 mAh/cm2.
S-O bond chemically constrained NiS2/rGO nanocomposite with enhanced Na-ion storage capacity
Shuyu Zhou, Xiaozhe Jin, Shengming Zhu, Qian Luo, Zhiwen Qiu, Aimin Wu, Hao Huang
2020, 31(9): 2353-2357  doi: 10.1016/j.cclet.2020.02.042
[摘要]  (145) [HTML全文] (145) [PDF 5298KB] (3)
摘要:
NiS2 has become a research hotspot of anode materials for Na-ion batteries due to its high theoretical specific capacity. However, the volume effect, the dissolution of polysulfide intermediates and the low conductivity during the charge/discharge process lead to the low specific capacity and poor cycling stability. NiS2/rGO nanocomposite was prepared by a facile two-step process: GO was prepared by modified Hummers method, and then NiS2/rGO nanocomposite was synthesized by L-cys assisted hydrothermal method. NiS2/rGO nanocomposite shows excellent cycle performance and rate performance, which could be attributed to the mesoporous structure on the graphene skeleton with high conductivity. Besides, the chemical constraint of a unique S-O bond on NiS2 could inhibit the dissolution of intermediates and the loss of irreversible capacity.
Synergetic ternary metal oxide nanodots-graphene cathode for high performance zinc energy storage
Lijun Su, Lingyang Liu, Yue Wang, Yulan Lu, Xingbin Yan
2020, 31(9): 2358-2364  doi: 10.1016/j.cclet.2020.03.014
[摘要]  (145) [HTML全文] (145) [PDF 8114KB] (1)
摘要:
Zinc-based electrochemistry energy storage with high safety and high theoretical capacity is considered to be a competitive candidate to replace lithium-ion batteries. In electrochemical energy storage, multimetal oxide cathode materials can generally provide a wider electrochemical stability window and a higher capacity compared with single metal oxides cathode. Here, a new type of cathode material, MnFe2Co3O8 nanodots/functional graphene sheets, is designed and used for aqueous hybrid Zn-based energy storage. Coupling with a hybrid electrolyte based on zinc sulfate and potassium hydroxide, the asfabricated battery was able to work with a wide electrochemical window of 0.1~1.8 V, showed a high specific capacity of 660 mAh/g, delivered an ultrahigh energy density of 1135 Wh/kg and a scalable power density of 5754 W/kg (calculated based on the cathode), and displayed a long cycling life of 1000 cycles. These are mainly attributed to the valence charge density distribution in MnFe2Co3O8 nanodots, the good structural strengthening as well as high conductivity of the cathode, and the right electrolyte. Such cathode material also exhibited high electrocatalytic activity for oxygen evolution reaction and thus could be used for constructing a Zn-air battery with an ultrahigh reversible capacity of 9556 mAh/g.
Screening of amino acids in dried blood spots by stable isotope derivatization-liquid chromatography-electrospray ionization mass spectrometry
Huaming Xiao, Ping Liu, Shujian Zheng, Xian Wang, Jun Ding, Yuqi Feng
2020, 31(9): 2423-2427  doi: 10.1016/j.cclet.2020.03.003
[摘要]  (159) [HTML全文] (159) [PDF 5239KB] (2)
摘要:
Direct infusion mass spectrometry (DIMS) is a powerful technique in clinical diagnosis for screening neonatal amino acid metabolic disorders from dried blood spots (DBS). However, DIMS sometimes generated false-positive results for analysis of amino acids. In this work, we utilized a stable isotope derivatization method, combining with liquid chromatography tandem mass spectrometry (SID-LC-MS), to improve the specificity for screening amino acids in DBS specimens. A pair of isotope reagents, p-(dimethylamino)phenyl isothiocyanate (DMAP-NCS) and 4-isothiocyanato-N, N-bis(methyl-[2H2])aniline ([2H4]DMAP-NCS), was synthesized and used to label amino acids in DBS specimens. The [2H4]DMAP-NCS labelled amino acid standards were used as internal standards to compensate the matrix effect. This method was validated by measuring linearity, recovery and accuracy. The results showed that the developed SID-LC-MS method can be used for sensitive and selective determination of 12 diagnostically important amino acids in DBS specimens.
Visual sensing of picric acid in 100% aqueous media based on supramolecular polythiophene assemblies with colorimetric and fluorescent dual response
Li Zhang, Yanan Sun, Yanping Jiang, Yining Li, Gang Song, Kunlun Huang, Zhiyi Yao
2020, 31(9): 2428-2432  doi: 10.1016/j.cclet.2020.04.003
[摘要]  (148) [HTML全文] (148) [PDF 3110KB] (1)
摘要:
A colorimetric and fluorometric dual probe based on a water-soluble polythiophene derivative (PMTPBA) was designed and synthesized. It can be applied to determination of picric acid (PA) in 100% aqueous solution. The approach relies on the formation of supramolecular polythiophene assemblies in the presence of PA through electrostatic, charge transfer and π-π stacking interactions. This probe could be utilized for the rapid and visual detection of PA both in aqueous solution and solid support with high specificity and sensitivity. The detection limit of this sensor is as low as 5.0×10-8 mol/L.
Polycyclic polyprenylated acylphloroglucinol with an unprecedented spirocyclic core from Hypericum patulum
Yansong Ye, Nana Jiang, Xianwen Yang, Gang Xu
2020, 31(9): 2433-2436  doi: 10.1016/j.cclet.2020.04.028
[摘要]  (145) [HTML全文] (145) [PDF 1828KB] (1)
摘要:
Spirohypatone A (1), a spirocyclic PPAP (polycyclic polyprenylated acylphloroglucinol) bearing an unprecedented hexahydro-1'H-spiro [cyclohexane-1, 2'-pentalene]-2, 4, 6-trione core and a new homologue (spirohypatone B, 2) were isolated from Hypericum patulum together with two known biosynthetic precursors. Compound 1 represents the first spirocyclic PPAP possessing a 5/5/6 carbon ring system, biogenetically derived from the intermediate 3 (attack from C-3 to C-12), which was differed from normal spirocyclic PPAPs (attack from C-3 to C-11). In addition, through extensive spectroscopic analysis, an interconversion mechanism of keto-enol of 1 was postulated and confirmed by its methylated reaction. The structures and absolute configurations of 1 and 2 were determined by comprehensive spectroscopic and chemical derivatized methods and X-ray crystallography. Compounds 1, 2, and 4 were tested to exhibit cytotoxic activities against several cancer cell lines.
Synthesis of highly-branched Au@AgPd core/shell nanoflowers for in situ SERS monitoring of catalytic reactions
Yujian Lai, Lijie Dong, Rui Liu, Shaoyu Lu, Zuoliang He, Wanyu Shan, Fanglan Geng, Yaqi Cai, Jingfu Liu
2020, 31(9): 2437-2441  doi: 10.1016/j.cclet.2020.04.050
[摘要]  (168) [HTML全文] (168) [PDF 4112KB] (1)
摘要:
Alloy and small size nanostructures are favorable to catalytical performance, but not to surface-enhanced Raman spectroscopy (SERS) applications. Integrating SERS and catalytic activity into the nanocrystals with both alloy and small size structures is of great interest in fabrication of SERS platform to in situ monitor catalytical reaction. Herein, we report a facile method to synthesize Au@AgPd trimetallic nanoflowers (Au@AgPd NFs) with both SERS and catalytic activities, through simultaneous selective growth of Ag and Pd on Au core to form highly-branched alloy shell. These nanocrystals have the properties of small sizes, defects abundance, and highly-dispersed alloy shell which offer superior catalytic activity, while the merits of monodisperse, excellent stability, and highly-branched shell and core/alloy-shell structure promise the enhanced SERS activity. We further studied their growth mechanisms, and found that the ratio of Ag to Pd, sizes of Au core, and surfactant cetyltrimethylammonium bromide together determine this special structure. Using this as-synthesized nanocrystals, a monolayer bifunctional platform with both SERS and catalytical activity was fabricated through selfassembly at air/water interface, and applied to in situ SERS monitoring the reaction process of Pd-catalyzed hydrogenation of 4-nitrothiophenol to 4-aminothiophenol.
Evolution of single nanobubbles through multi-state dynamics
Huihui Wang, Ting He, Ying Du, Wenhui Wang, Yangbin Shen, Shuping Li, Xiaochun Zhou, Feng Yang
2020, 31(9): 2442-2446  doi: 10.1016/j.cclet.2020.03.049
[摘要]  (148) [HTML全文] (148) [PDF 4479KB] (3)
摘要:
Nanobubble is a rising research field, which attracts more and more attentions due to its potential applications in medical science, catalysis, electrochemistry and etc. To better implement these applications, it is urgent to understand one of the most important mechanisms of nanobubbles, the evolution. However, few attentions have been paid in this aspect because of the methodology difficulties. Here we successfully used dark-field microscopy to study the evolution process of single nanobubbles generated from formic acid dehydrogenation on single Pd-Ag nanoplates. We found some of the nanobubbles in this system can exhibit three distinct states representing different sizes, which can transform among each other. These transitions are not direct but through some intermediate states. Further kinetic analysis reveals complicated mechanisms behind the evolution of single nanobubbles. The results acquired from this study can be applicable to nanobubble systems in general and provide insights into the understanding of mechanisms affecting the stability of nanobubbles and their applications.
Rapid and fine tailoring longitudinal surface plasmon resonances of gold nanorods by end-selective oxidation
Wenhan Li, Zhirui Guo, Qiuyuan Tai, Yawen Li, Yefei Zhu, Tingting Bai
2020, 31(9): 2447-2451  doi: 10.1016/j.cclet.2020.05.019
[摘要]  (136) [HTML全文] (136) [PDF 6149KB] (1)
摘要:
Facile achievement of gold nanorods (AuNRs) with controllable longitudinal surface plasmon resonance (LSPR) is of great importance for their applications in various fields. The LSPR of AuNRs is sensitive to their aspect ratio, which is still hard to be precisely tuned by direct synthesis. In this work, we report a simple approach for end-selective etching of AuNRs by a rapid oxidation process with Au(Ⅲ) in cetyltrimethylammonium bromide (CTAB) solution at a mild temperature. The LSPR wavelength and the length of AuNRs blue shifted linearly as a function of the amount of Au(Ⅲ), while the diameter of AuNRs remained nearly constant. The oxidative rate is temperature dependent, and the oxidative process for a desired LSPR can be accomplished within 15 min at 60 ℃. Further investigations indicated that Br- determine the occurrence of the oxidation between AuNRs and Au(Ⅲ), and a small amount of surfactant chain (CTA+) is crucial for stabilizing AuNRs. This method presents a quick but robust strategy for acquiring AuNRs with an arbitrary intermediate LSPR wavelength using the same starting AuNRs, and can be a powerful tool for subsequent applications.
A novel AH-D-A-type phase junction material to improve photovoltaic performance and device stability in fullerene OSCs
Lin Shao, Fei Tong, Mengbing Zhu, Hao Xia, Wenhong Peng, Hua Tan, Bin Zhang, Yu Liu, Weiguo Zhu
2020, 31(9): 2452-2458  doi: 10.1016/j.cclet.2020.03.036
[摘要]  (153) [HTML全文] (153) [PDF 10910KB] (2)
摘要:
In order to boost power conversion efficiency (PCE) and operation stability of organic solar cells (OSCs), we propose a new idea of phase junction materials (PJMs) used as a photoactive layer component to improve device performance and stability. For this purpose, a novel PJM of H-TRC8 based on rhodanine unit was designed with a conjugated AH-D-A framework. Here, AH is a hydrogen-donating electron acceptor unit, D-A is an electron donor-acceptor unit. It is found that H-TRC8 has a good carriertransporting ability, as well as definite hydrogen-bond and D-A interaction with donor/acceptor materials. While H-TRC8 is added into the PBDB-T/PC60BM blend film with 1.0 vol% DIO (1, 8-diiodooctane), the resulting blend film exhibited an enhanced absorption and improved morphology. The intermolecular hydrogen bond between H-TRC8 and PBDB-T plays an important role for them, which is confirmed via FT-IR spectra and 2D 1H NMR. As a result, the PBDB-T/PC60BM-based devices with 1.25 wt% H-TRC8 and 1.0 vol% DIO exhibit a significantly improved PCE of 8.06%, which is increased by 20.6% in comparison to that in the binary devices with 1.0 vol% DIO only (PCE = 6.68%). Furthermore, the device stability is significantly enhanced with only 43% PCE roll-off at 150 ℃ for 120 h. This work indicates that AH-D-A-type PJMs are promising photovoltaic materials used as photoactive-layer components to achieve high-performance fullerene OSCs with high device stability.
Enhancement the photovoltaic performance of conjugated polymer based on simple head-to-head alkylthio side chains engineered bithiophene
Zuoji Liu, Chengjia Bao, Guangjun Zhang, Kai Zhang, Gangtie Lei, Qiang Zhang, Qiang Peng, Yu Liu
2020, 31(9): 2459-2464  doi: 10.1016/j.cclet.2020.02.021
[摘要]  (141) [HTML全文] (141) [PDF 5101KB] (2)
摘要:
In this article, three novel and simple molecular structure with donor-acceptor (D-A) type copolymers via only head-to-head alkoxy (OR) and/or alkylthio (SR) side chains onto the bithiophene (BT) as donor units and fluorinated benzotriazole (FBTA) as acceptor unit, namely, PBTOR-FBTA, PBTOSR-FBTA and PBTSRFBTA, were successfully designed and synthesized. The impacts of sulfur-oxygen (S⋯O) or sulfur-sulfur (S⋯S) noncovalent interactions on their physicochemical properties, molecular stacking, carrier mobility, morphologies of blend films, as well as their photovoltaic performance were deeply and systematically studied. The introduction of SR side-chains suddenly lowered the highest occupied molecular orbital (HOMO) energy levels, blue-shifted absorption, enhanced π-π stacking, as well as improved morphology of the photoactive layer blends in comparison with the reference polymer without SR side-chain. Polymer solar cells (PSCs) were fabricated to estimate their photovoltaic performance of the polymers. Under an optimized blend ratio of PBTSR-FBTA:PC71BM (1:0.8, w/w), the PBTSR-FBTAbased device exhibits a higher power conversion efficiency (PCE) of 6.25%, which is about 3.34 and 1.87 folds than that of the PBTOR-FBTA and PBTOSR-FBTA-based devices, respectively. Our research results demonstrate that the modification of the simple and low-cost SR side chains is an effective strategy to improve the photovoltaic performance of the polymers.
HFIP-promoted catalyst-free cascade reactions for the synthesis of biologically relevant 3, 3-di(indolyl)indolin-2-ones from indoles and isatins
Xiaohan Yuan, Shuai Wang, Jialing Cheng, Bin Yu, Hong-Min Liu
2020, 31(9): 2465-2468  doi: 10.1016/j.cclet.2020.03.025
[摘要]  (157) [HTML全文] (157) [PDF 2569KB] (1)
摘要:
The first HFIP-promoted catalyst-free cascade reactions for the synthesis of biologically relevant 3, 3-di (indolyl)indolin-2-ones (27 examples, up to 98% yield) from readily available indoles and isatin derivatives are described. This protocol shows well tolerance of different functional groups and features mild reaction conditions such as short reaction time (~1 h), no usage of catalyst, easy operation and product isolation. Of particular interest is the formation of two C—C bonds and one all-carbon quaternary center. This protocol could serve as an alternative strategy to synthesize biologically important 3, 3-di (indolyl)indolin-2-ones for biological testing.
Nickel-iron borate coated nickel-iron boride hybrid for highly stable and active oxygen evolution electrocatalysis
Pengyu Han, Tan Tan, Fei Wu, Ping Cai, Gongzhen Cheng, Luo Wei
2020, 31(9): 2469-2472  doi: 10.1016/j.cclet.2020.03.009
[摘要]  (146) [HTML全文] (146) [PDF 2994KB] (2)
摘要:
The development of efficient and cost-effective electrocatalysts toward anodic oxygen evolution reaction (OER) is crucial for the commercial application of electrochemical water splitting. As the most promising electrocatalysts, the OER performances of nickel-iron-based materials can be further improved by introducing metalloid elements to modify their electron structures. Herein, we developed an efficient hybrid electrocatalyst with nickel-iron boride (NiFeB) as core and amorphous nickel-iron borate (NiFeBi) as shell (NiFeB@NiFeBi) via a simple aqueous reduction. The obtained NiFeB@NiFeBi exhibits a small overpotential of 237 mV at 10 mA/cm2 and Tafel slope of 57.65 mV/dec in 1.0 mol/L KOH, outperforming most of the documented precious-metal-free based electrocatalysts. Benefiting from the in situ formed amorphous NiFeBi layer, it shows excellent stability toward the oxygen evolution reaction (OER). These findings might provide a new way to design advanced precious-metal-free electrocatalysts for OER and the application of electrochemical water splitting.
Rapid pattern recognition of different types of sulphur-containing species as well as serum and bacteria discrimination using Au NCs-Cu2+ complexes
Wentao Li, Xiaomei Sun, Xuan Zhao, Wei Wang, Shenghao Xu, Xiliang Luo
2020, 31(9): 2473-2477  doi: 10.1016/j.cclet.2020.04.027
[摘要]  (150) [HTML全文] (150) [PDF 4587KB] (1)
摘要:
Discrimination of different types of sulfur-containing species not only helps us to deeply understand how sulfur affects cellular signaling, but also contribute to the early diagnosis of diseases. However, the current investigation about sulfur-containing species discrimination is mainly concentrated in biothiols, which is relatively limited for practical application. Toward circumventing this limitation, herein, a convenient sensor array consisting of three kinds of Au NCs-Cu2+ for simultaneous and rapid identification of different types of sulfur-containing species is reported. Based on the fingerprint-like fluorescence responses generated by competitive binding between Au NCs-Cu2+ and different sulfur-containing species, not only ten different types of sulfur-containing species separately but also their binary or ternary randomly selected mixtures can be well discriminated even in human urine and serum samples. It is worth noting that it only takes 2 min to obtain the best response signals for sulfur-containing species discrimination. Most importantly, serums from cancer patients (such as liver cancer and breast cancer) and healthy people as well as sulfur-oxidizing bacteria (SOB) and sulfur-free bacteria can be both effectively and rapidly identified within 2 min, respectively, making it a promising approach for point-of-care disease diagnostic.
Pt nanodendrites with (111) crystalline facet as an efficient, stable and pH-universal catalyst for electrochemical hydrogen production
Huifang Sun, Qi Zeng, Chen Ye, Yangguang Zhu, Feiyue Chen, Mingyang Yang, Li Fu, Shiyu Du, Jinhong Yu, Nan Jiang, Jianxiong Liu, Tianzhun Wu, Cheng-Te Lin
2020, 31(9): 2478-2482  doi: 10.1016/j.cclet.2020.03.032
[摘要]  (142) [HTML全文] (142) [PDF 10151KB] (1)
摘要:
High-performance nanomaterial catalysts for hydrogen evolution reaction via electrochemical water splitting are significant to the development of hydrogen energy. In this work, we report a robust and highly active catalyst fabricated through direct electrochemical deposition of Pt nanodendrites at the surface of activated carbon (Pt NDs). Owing to the large electrochemically active area and the exposed (111) facet of Pt, Pt NDs exhibits outstanding activity towards hydrogen evolution reaction with a low requiring overpotential of 0.027 V at 10 mA/cm2 and Tafel slope of ≈ 22 mV/dec in acidic media. In addition, the hydrogen yield of Pt NDs is 30%-45% larger than that of commercial Pt/C at the same Pt loadings. Moreover, Pt NDs exhibits excellent long-term durability whose hydrogen production efficiency remains unchanged after six-hour hydrogen production, while the efficiency of commercial Pt/C catalyst decayed 9% under the same circumstance. Considering the superiority of catalytic activity and stability, this Pt NDs present great potentiality towards practical hydrogen production application.
Synthesis, structure and electrocatalytic H2-evoluting activity of a dinickel model complex related to the active site of [NiFe]-hydrogenases
Dengmeng Song, Xuyun Gao, Bo Li, Jun Li, Xuzhuo Sun, Chengbo Li, Jiale Zhao, Lin Chen, Ning Wang
2020, 31(9): 2483-2486  doi: 10.1016/j.cclet.2020.01.033
[摘要]  (142) [HTML全文] (142) [PDF 3103KB] (2)
摘要:
Structural and functional biomimicking of the active site of [NiFe]-hydrogenases can provide helpful hints for designing bioinspired catalysts to replace the expensive noble metal catalysts for H2 generation and uptake. Treatment of dianion [Ni(phma)]2- [H4phma = N, N'-1, 2-phenylenebis(2-mercaptoacetamide)] with [NiCl2(dppp)] (dppp = bis(diphenylphosphino)propane) yielded a dinickel product [Ni(phma)(μ-S, S')Ni(dppp)] (1) as the model complex relevant to the active site of [NiFe]-H2ases. The structure of complex 1 has been characterized by single-crystal X-ray analysis. From cyclic voltammetry and controlled potential electrolysis studies, complex 1 was found to be a moderate electrocatalyst for the H2-evoluting reaction using ClCH2COOH as the proton source.
Fe doping promoted electrocatalytic N2 reduction reaction of 2H MoS2
Jiaojiao Guo, Tsegaye Tadesse Tsega, Ibrahim Ul Islam, Asma Iqbal, Jiantao Zai, Xuefeng Qian
2020, 31(9): 2487-2490  doi: 10.1016/j.cclet.2020.02.019
[摘要]  (138) [HTML全文] (138) [PDF 4342KB] (1)
摘要:
Electrocatalytic N2 reduction to ammonia is a fascinating alternative to Haber-Bosch process and also considered as an energy storage method. This work, Fe doped MoS2/carbon cloth (CC) has been studied on the electro-catalysis fix nitrogen indicating the doped Fe can indeed enhance the MoS2 material ability. Compared with MoS2/CC, Fe-Mo-S-3/CC not only increases 10 times in the rate of production ammonia, but also 5 times in Faraday efficiency.
High stability three-dimensional porous PtSn nano-catalyst for ethanol electro-oxidation reaction
Yue Sun, Haiyan Xiang, Huimin Li, Gang Yu, Hong Chen, Song Liu
2020, 31(9): 2491-2494  doi: 10.1016/j.cclet.2020.04.025
[摘要]  (141) [HTML全文] (141) [PDF 3158KB] (1)
摘要:
In addition to the theoretical research, direct ethanol fuel cells have great potential in practical applications. The performance of direct ethanol fuel cells largely depends on the electrocatalysts. Pt-based electrocatalysts have been promising candidates for advancing direct ethanol fuel cells for its high catalytic activity and great durability. Here, a PtSn catalyst with unique three-dimensional porous nanostructure has been designed and synthesized via a two-step liquid phase reduction reaction. Sn formed a self-supporting framework in PtSn alloy particles (~3.5 nm). In ethanol electro-oxidation reaction, the PtSn catalyst exhibited high mass activity and excellent recycling time compared with that of Pt/C. After the morphology characterization before and after potential cycling, the PtSn alloy-based nano-catalyst showed good stability. The PtSn catalysts effectively avoid structural instability due to the external carriers, and prolong the leaching time of Sn. In addition, the introduction of a certain amount of Sn can also solve the poisoning phenomenon of active sites on Pt surface. The design strategy of porous alloy nano-catalyst sheds light on its applications in direct ethanol fuel cells.
Covalent organic frameworks functionalized carbon fiber paper for the capture and detection of hydroxyl radical in the atmosphere
Zhiling Huang, Qin Xu, Xiaoya Hu
2020, 31(9): 2495-2498  doi: 10.1016/j.cclet.2020.06.017
[摘要]  (142) [HTML全文] (142) [PDF 4233KB] (3)
摘要:
Developing a fast, sensitive and convenient method for the detection of hydroxyl radicals (·OH) in the atmosphere could help us know the precursor levels of atmospheric species and control air pollution. In this work, the carbon fiber paper (CFP) functionalizing with a kind of covalent organic frameworks (COFs), formed from 1, 3, 5-triformylphloroglucinol (Tp) and benzidine (BD) (COF(TpBD)), was firstly used a new platform for ·OH trapping and detection. The COF(TpBD) modified CFP was acted as a filter to impregnate salicylic acid (SA) and a detector to detect 2, 5-dihydroxybenzoic acid (2, 5-DHBA) which was produced from the reaction between the impregnated SA and ·OH in the atmosphere. This method provided a linearity for 2, 5-DHBA from 5.0×10-14 mol/L 1.0×10-9 mol/L with a detection limit of 6.9×10-15 mol/L, which is corresponding to the amount of ·OH from 3.0×107 to 6.0×1011 molecules/cm3 with the detection limit of 4.1×106 molecules/cm3. This COF(TpBD)-CFP platform has been successfully applied for the detection of ·OH concentration under different conditions of Yangzhou when the sampling time was shortened to 30 min. This work has provided a new method for atmospheric ·OH detection with excellent sensitivity, simplicity, and high speed.
Enhanced photoluminescence and stability of ZnSe microspheres/Cs4PbBr6 microcrystals/CsPbBr3 nanocrystals composites
Chao Zhang, Tingting Li, Lei Pu, Weijia Wen, Xiangdong Luo, LijuanZ hao
2020, 31(9): 2499-2502  doi: 10.1016/j.cclet.2020.01.013
[摘要]  (146) [HTML全文] (146) [PDF 3599KB] (1)
摘要:
A ternary complex combining dual-phase perovskites - Cs4PbBr6/CsPbBr3 (DP-CPB) with ZnSe micropsheres (ZnSe-DP-CPB) was successfully prepared using supersaturated recrystallization technique at room temperature. It was showed that the DP-CPB composites were partially embedded in ZnSe microsphere composed with ZnSe NCs. The light absorption range of ZnSe-DP-CPB composites was extended from visible to near infrared light. Highly enhanced luminescence from ZnSe-DP-CPB composite was observed and the excitation power-dependent photoluminescence showed that the recombination involves excitons. The recombination lifetimes of the ternary composites increased compared with DP-CPB composite, indicating that the non-radiative combination was suppressed which may be possibly due to the decrease of both bulk and surface defects, owing to the passivation of ZnSe, as well as the suitable band alignments of these three components. The ternary complex also showed improved stability of photoluminescence (PL), which opens a new avenue for enhancing the stability of PL and optoelectronic applications for semiconductor-perovskite composites.
Synthesis, structure and magnetic properties of a decanuclear Fe(Ⅲ)/oxo cluster
Waseem Muhammad, Jie Ni, Zvonko Jagličić, Ping Cui, Linna Gao, Di Sun
2020, 31(9): 2503-2506  doi: 10.1016/j.cclet.2020.01.031
[摘要]  (142) [HTML全文] (142) [PDF 2609KB] (1)
摘要:
An iron (Ⅲ) cluster, namely [Fe10(μ3-O)8L8(NO3)6] (1), has been synthesized by treatment of Fe (NO3)3·9H2O with 3, 5-dimethyl-1-(hydroxymethyl)-pyrazole (HL) under ambient temperature. The core skeleton of {Fe10} can be regarded as a pear-like cage with eight triangular {Fe3(μ3-O)} units, in which each three Fe centers is held together by one μ3-O2- group with Fe centers as corner-sharing triangle units. Importantly, {Fe10} cluster is not only stable in solid state but also in solution, which is confirmed by powder X-ray diffraction (PXRD) pattern and electrospray ionization mass spectrometry (ESI-MS), respectively. Furthermore, 1 shows antiferromagnetic exchange behavior arising from the interactions between the iron(Ⅲ) centers.
A dense graphene monolith with poloxamer prefunctionalization enabling aqueous redispersion to obtain solubilized graphene sheets
Chen Ye, Fan Zhang, Xue Tan, Huifang Sun, Wen Dai, Ke Yang, Minghui Yang, Shiyu Du, Dan Dai, Jinhong Yu, Nan Jiang, Weitao Su, Li Fu, He Li, Jing Kong, Cheng-Te Lin
2020, 31(9): 2507-2511  doi: 10.1016/j.cclet.2020.01.021
[摘要]  (147) [HTML全文] (147) [PDF 5579KB] (2)
摘要:
The realization of good aqueous dispersibility of commercial graphene products composed of exfoliated graphene sheets is of significance for downstream applications. However, the tap density of commercial graphene powder is quite low (0.03-0.1 kg/m3), meaning that 1 kg graphene powder occupies about 10-30 m3 in volume during transportation. And, the available content of commercial graphene dispersion/slurry in aqueous medium cannot exceed 5 wt%, although the density is high (≈1050 kg/m3). In this work, a graphene monolith was prepared by oven-drying of graphene sheets prefunctionalized with poloxamer surfactants. Our graphene monoliths not only have a high density (1500 kg/m3) and high graphene content (≈10 wt%), but also a full capability to be completely redispersed (≈100%) in water by bath sonication to obtain solubilized graphene sheets, whose lateral size and thickness are unchanged compared to as-exfoliated ones. Moreover, a simple empirical method was proposed to predict the redispersion capability of graphene monoliths using different poloxamers by contact angle measurements. Our results provide a universal approach to make exfoliated graphene-based products with better downstream availability and lower transportation cost.
Highly dispersed Ru/Co catalyst with enhanced activity for catalyzing NaBH4 hydrolysis in alkaline solutions
Jiapeng Zhang, Fanzhen Lin, Lijing Yang, Hua Dong
2020, 31(9): 2512-2515  doi: 10.1016/j.cclet.2020.03.072
[摘要]  (145) [HTML全文] (145) [PDF 3574KB] (1)
摘要:
Ru and Co are highly dispersed on the surface of TiO2 nanoparticles with an easy coprecipitation method to fabricate a novel Ru-based catalyst (Ru/Co-TiO2). The fabricated Ru/Co-TiO2 catalyst exhibits superior catalytic performance for promoting NaBH4 hydrolysis in alkaline medium, showing an impressive hydrogen generation rate per gram Ru as high as 172 L min-1 gRu-1, which is better than most of recently reported Ru-based catalysts. In addition, the fabricated Ru/Co-TiO2 catalyst also shows excellent durability in cycle use, with only 2.9% activity loss after being used for 5 cycles.These advantages make the developed Ru/ Co-TiO2 catalyst a potential choice for promoting hydrogen generation from NaBH4 hydrolysis.
Photosensitizer conjugate-functionalized poly(hexamethylene guanidine) for potentiated broad-spectrum bacterial inhibition and enhanced biocompatibility
Fengfeng Xiao, Bing Cao, Liewei Wen, Yanhong Su, Meixiao Zhan, Ligong Lu, Xianglong Hu
2020, 31(9): 2516-2519  doi: 10.1016/j.cclet.2020.06.038
[摘要]  (152) [HTML全文] (152) [PDF 2998KB] (1)
摘要:
Pathogen infection is the main cause of human morbidity and death. Traditional antibiotics usually sterilize bacteria in chemical ways, which tends to develop serious antibiotic resistance. Cationic polymers exhibit good bacterial inhibition with less resistance, but often face severe cytotoxicity toward normal cells. The optimization of polymeric antimicrobials for enhanced bactericidal capacity and improved biocompatibility is quite meaningful. In addition, photodynamic therapy (PDT) is a therapeutic modality with less susceptibility to develop resistance. Herein, a typical commercial polymeric antimicrobial, polyhexamethylene guanidine (PHMG) was selected for current proof-of-concept optimization due to its excellent bactericidal capacity but moderate biocompatibility. Eosin-Y (EoS) was copolymerized to afford EoS-labeled polymer conjugates, poly(2-(dimethylamino) ethyl methacrylate-co-eosin), P(DMAEMA-co-EoS), which was conjugated with PHMG to afford a novel polymeric antimicrobial, P(DMAEMA-co-EoS)-b-PHMG-b-P(DMAEMA-co-EoS), noted as PEoS-PHMG. It could efficiently kill broad-spectrum bacteria by physical damage and photodynamic therapy. Compared with PHMG, the bacterial inhibition of PEoS-PHMG was potentiated after the functionalization. Furthermore, PEoS-PHMG exhibited low cytotoxicity and minimal hemolysis, which was demonstrated by cell viability assays toward LO2 cells and RAW 264.7 cells as well as hemolytic assays against red blood cells. These results confirmed that the resultant PEoS-PHMG could act as promising alternative antibacterial materials with excellent broad-spectrum bacterial inhibition and favorable biocompatibility.
Monitoring casein kinase Ⅱ at subcellular level via bio-bar-code-based electrochemiluminescence biosensing method
Lifen Wang, Jiajia Song, Xiaofei Wang, Honglan Qi, Qiang Gao, Chengxiao Zhang
2020, 31(9): 2520-2524  doi: 10.1016/j.cclet.2020.06.032
[摘要]  (167) [HTML全文] (167) [PDF 4364KB] (2)
摘要:
A highly sensitive electrochemiluminescence (ECL) biosensing method was developed for monitoring casein kinase Ⅱ (CK2) at subcellular level via bio-bar-code assay. A bio-bar-code probe (h-DNA/AuNPs/pDNA) prepared by conjugating phosphorylated DNA (p-DNA) and hairpin DNA (h-DNA) onto gold nanoparticles (AuNPs) was used as a carrier for ECL signal reagent (Ru(phen)32+) while a specific peptide was used as a recognition substance. A gold ultramicroelectrode with a diameter of 400 nm was fabricated and then modified with the specific peptide via self-assembly technique to obtain peptide modified gold ultramicroelectrode. The peptide on gold ultramicroelectrode was phosphorylated in the presence of CK2 and adenosine 5'-triphosphate, and then the phosphorylated peptide was integrated with the h-DNA/AuNPs/p-DNA through a process mediated by zirconium cations (Zr4+), and finally Ru(phen)32+ was intercalated into h-DNA. A "signal on" ECL method was developed for the detection of CK2 in the range of 0.005-0.2 U/mL with a detection limit of 0.001 U/mL. Additionally, combined efficient subcellular phosphorylation in vivo with bio-bar-code-based ECL biosensing method, the ECL method was further applied to monitor CK2 at subcellular level without tedious subcellular fractionation. It was found that the concentration of CK2 by inserting the peptide modified gold ultramicroelectrode into the nucleus was higher than that into cytoplasm of HeLa cells. A distinct heterogeneity among CK2 concentrations in single cells was observed for cellular heterogeneity assessment.

Reviews
The synthesis and applications of α-zirconium phosphate
Yu Cheng, Gaik Khuan Chuah
2020, 31(2): 307-310  doi: 10.1016/j.cclet.2019.04.063
[摘要]  (259) [HTML全文] (259) [PDF 2064KB] (259)
摘要:
The synthesis of α-ZrP with a range of crystallinity is of high importance due to the different requirements in various applications. Nanosized crystalline α-ZrP is typically obtained by refluxing amorphous ZrP in concentrated H3PO4 solutions. Microcrystalline α-ZrP are obtained by direct precipitation in the presence of either HF or oxalic acid which are used as complexing agents for zirconium. These larger crystals are useful as ion-exchangers in column-type applications as the back pressure can be significantly reduced. A novel minimalistic synthesis that is green, simple and fast is highlighted in this review. Both nano-sized and micro-sized α-ZrP can be prepared via this protocol to meet many potential applications. Applications of α-ZrP in ion-exchange, catalysis, lubricants, intercalation hosts, polymer fillers and fire retardants are discussed.
Recent advances in asymmetric synthesis of 2-substituted indoline derivatives
Ting-Bi Hua, Cong Xiao, Qing-Qing Yang, Jia-Rong Chen
2020, 31(2): 311-323  doi: 10.1016/j.cclet.2019.07.015
[摘要]  (265) [HTML全文] (265) [PDF 15535KB] (265)
摘要:
Enantiomerically pure 2-substituted indolines are an important class of nitrogen heterocycles that occur frequently in many alkaloid natural products and biologically active compounds. Consequently, the synthesis of such skeletons is of great significance. The past years have witnessed a number of remarkable advances in the development of efficient strategies to construct this class of chiral compounds. This review summarizes the recent advances in asymmetric synthesis of 2-substituted indoline derivatives. Due to the limitation of the length, this review only summarizes those works published from January of 2012 to January of 2019. Meanwhile, methods towards synthesis of fused and spirocyclic indolines will not be discussed in this review.
Communications
Enantioselective carboxylative cyclization of propargylic alcohol with carbon dioxide under mild conditions
Shiliang Xie, Xiaotong Gao, Feng Zhou, Haihong Wu, Jian Zhou
2020, 31(2): 324-328  doi: 10.1016/j.cclet.2019.05.060
[摘要]  (225) [HTML全文] (225) [PDF 1491KB] (225)
摘要:
An enantioselective carboxylative cyclization of propargylic alcohols and CO2 was realized under mild conditions, based on a kinetic resolution strategy, which enabled the synthesis of chiral cyclic carbonates and propargylic alcohols with promising yield and enantioselectivity simultaneously.
Divergent intramolecular reactions between phosphines and alkynes
Yanying Song, Lili Wang, Zheng Duan, François Mathey
2020, 31(2): 329-332  doi: 10.1016/j.cclet.2019.05.053
[摘要]  (230) [HTML全文] (230) [PDF 1985KB] (230)
摘要:
A divergent intramolecular reaction of phosphine tethered alkyne in protic solvent was developed. This provided a novel and simple access to a large variety of (Z)-alkenylphosphine oxides and phospholane oxides. Our preliminary studies suggested that these divergent reactions are closely related to the reaction condition and molecular structure. A possible mechanism of C-P bond cleavage of a pentacoordinated hydroxyphosphorane intermediate was proposed.
Selective and facile deacetylation of pentacyclic triterpenoid under methanolic ammonia condition and unambiguous NMR analysis
Han Wang, Renyang Xu, Shuobin Liang, Fuxiang Ran, Lihe Zhang, Yongmin Zhang, Demin Zhou, Sulong Xiao
2020, 31(2): 333-336  doi: 10.1016/j.cclet.2019.06.007
[摘要]  (220) [HTML全文] (220) [PDF 1942KB] (220)
摘要:
The acetyl ester plays an important role for protection of the hydroxyl groups in carbohydrates synthesis. In the present study, we described an efficient deprotection of acetyl group of pentacyclic triterpenoid by using methanolic ammonia in THF solution. Good selectivity for cleaving gal-C2-OAc group of 3β-hydroxy-olean-12-en-28-oic acid 28-N-2, 3, 4, 6-tetra-O-acetyl-β-D-galactopyranoside (3) was achieved in the presence of methanolic ammonia within 4 h at low temperature (-60℃) in a yield of 56%. The reaction disclosed here provides a new method for the synthesis of C2 selective modified carbohydrates, which is more useful than conventional synthesis procedure that usually requires many steps including temporary regioselective protection and deprotection. When the reaction temperature was increased from -60℃ to room temperature, the cleavage of the other three acetyl groups of galactose in an order of C4-OAc > C3-OAc > C6-OAc was observed. Based on this study, a plausible route for the deacetylation reaction has been proposed.
Visible light induced the high-efficiency spirocyclization reaction of propynamide and thiophenols via recyclable catalyst Pd/ZrO2
Nannan Zhang, Hangdong Zuo, Chen Xu, Junyi Pan, Jun Sun, Cheng Guo
2020, 31(2): 337-340  doi: 10.1016/j.cclet.2019.06.008
[摘要]  (261) [HTML全文] (261) [PDF 2648KB] (261)
摘要:
A new method for the synthesis of 3-thioazaspiro[4,5]trienones was developed using Pd nanoparticle catalysts, which are highly efficient, environmentally friendly and recyclable. Alkynes and thiophene phenols are effectively cyclized by Pd/ZrO2 catalyst under visible light irradiation. The present protocol simply utilizes visible light as the safe and ecofriendly energy source, and the Pd/ZrO2 nanocomposite as photocatalyst provides a simple and practical approach to various 3-thioazaspiro[4,5]trienones in moderate conditions to high yields
Thermodynamic favorable CO2 conversion via vicinal diols and propargylic alcohols: A metal-free catalytic method
Li-Hua Han, Jing-Yuan Li, Qing-Wen Song, Kan Zhang, Qian-Xia Zhang, Xiao-Fang Sun, Ping Liu
2020, 31(2): 341-344  doi: 10.1016/j.cclet.2019.06.030
[摘要]  (222) [HTML全文] (222) [PDF 2343KB] (222)
摘要:
Organocatalysis represents a promising field in chemical fixation of CO2. Herein, a facile metal-free strategy was reported for the one-pot preparation of cyclic carbonates and α-hydroxy ketones from vicinal diols, propargylic alcohols and CO2. Wide scope of vicinal diols and propargylic alcohols was demonstrated to be efficient under the DBU-catalyzed conditions. A plausible mechanism was proposed, which included detailed main and side reactions under the metal-free conditions.
Effects of the chemical structure of surfactants on the stability of naphthenic oil-based metalworking fluids
Yuan Xue, Jinbao Liu, Maiying Xie, Fengfei Chen, Mingan Zhou, Hualin Lin, Fan Zhang, Shizhou Liu, Zhiqiao Wu, Sheng Han
2020, 31(2): 345-348  doi: 10.1016/j.cclet.2019.06.031
[摘要]  (242) [HTML全文] (242) [PDF 730KB] (242)
摘要:
In this study, various nonionic surfactants (NS) with different ethylene oxide (EO) numbers and tail lengths and its binary blends with anionic surfactants (AS) were used as emulsifiers for naphthenic oil to form the microemulsion metalworking fluids (MWFs), and the effects of them on the stability of the emulsion system were investigated by formulation triangle method. The results indicated that binary complex surfactants of NS and AS as emulsifiers exhibited better emulsifying effect than that of single NS. NS with different EO numbers and tail lengths presented various emulsifying effects. NS (EO = 10) exhibited the greatest number of stable formulations, especially the TX-10, but no linear relationship existed between the number of stable formulations and the tail length of NS. In addition, aromatic primary alcohol ethoxylate (APAE) series surfactants containing benzene groups similar to the cycloalkanes in the naphthenic oil so that presented the best emulsifying affect and the greatest number of stable formulations. The co-surfactant of sodium dodecyl benzene sulfonate (SDBS) binary blends with NS exerted the best synergistic effect, and the stable formulations numbers were ranged from 5 to 7, next sodium stearate (SS) comes last followed by sodium dodecyl sulfate (SDS-1) and sodium dodecyl sulfonate (SDS-2).
Brønsted acid-promoted 'on-water' C(sp3)-H functionalization for the synthesis of isoindolinone/[1, 2, 4]triazolo[1, 5-a] pyrimidine derivatives targeting the SKP2-CKS1 interaction
Shuo Yuan, Sixi Wang, Min Zhao, Danqing Zhang, Jinjie Chen, Jian-Xin Li, Jingya Zhang, Yihui Song, Jinyi Wang, Bin Yu, Hongmin Liu
2020, 31(2): 349-352  doi: 10.1016/j.cclet.2019.07.019
[摘要]  (218) [HTML全文] (218) [PDF 892KB] (218)
摘要:
The isoindolinone and biaryl scaffolds are prevalent in natural products and drug molecules, which have showed broad and interesting biological activities. The efficient construction of such hybridized molecules and biological evaluation are of great interest to medicinal chemistry community. In this communication, we report an efficient Brønsted acid-promoted C(sp3)-H functionalization approach that enables the rapid construction of biologically important isoindolinone/[1,2,4]triazolo[1, 5-a]pyrimidine hybrids from 5-methyl-7-(2, 4, 6-trimethoxyphenyl)-[1,2,4]triazolo[1, 5-a]pyrimidine, 2-formylbenzoic acid and various anilines. The title compounds were generated in high to excellent yields (up to 96%) regardless of the electronic nature and steric effects of the substituents. In this reaction, an isoindolinone scaffold, one C-C single bond, and two C-N bonds were formed simultaneously with high atom economy. In this work, we have envisioned that the methyl group linked to the electron-deficient Nheterocycles could be used as a new synthetic handle for late-state diversification and may have broad applications in the field of organic and medicinal chemistry. Besides, the title compounds have exhibited promising activity against the SKP2-CKS1 interaction.
The self-assemblies of a newly designed star-shaped molecule end-capped with bromine atoms studied by scanning tunneling microscopy
Jingfei Hou, Bin Tu, Qingdao Zeng, Chuanlang Zhan, Jiannian Yao
2020, 31(2): 353-356  doi: 10.1016/j.cclet.2019.07.029
[摘要]  (208) [HTML全文] (208) [PDF 892KB] (208)
摘要:
A new star-shaped molecule StOF-Br3 containing oligofluorenes and halogen atoms (Bromine) has been synthesized and studied by Scanning Tunneling Microscopy (STM) at the highly oriented pyrolytic graphite (HOPG) surface. We have obtained the high-resolution self-assembled STM images, from which the highly ordered and closely packed non-porous arrangements of the StOF-Br3 molecular selfassemblies at the heptanoic acid/HOPG surface could be observed. The molecular models and selfassembled StOF-Br3 architectures have been given in the following text. Besides, we have also figured out the surface free energy by the density functional theory (DFT) calculation, which proved that the halogen…halogen interaction was strong enough to stabilize the ordered molecular self-assemblies. This work verifies the existence of bromine…bromine interactions, and meanwhile provides a kind of effective approach for quickly building ordered molecular nanoarchitectures with large areas and different geometries.
Synthesis and reactivity of carbazole-containing hypervalent iodine(Ⅲ) reagents
Tianlei Lan, Haijuan Qin, Wenting Chen, Wei Liu, Chao Chen
2020, 31(2): 357-360  doi: 10.1016/j.cclet.2019.07.031
[摘要]  (208) [HTML全文] (208) [PDF 920KB] (208)
摘要:
A range of bench-stable carbazole-containing hypervalent iodine(Ⅲ) reagents were synthesized by I-N bond formation in good yields. This kind of benziodoxolone reagents was used for a C-N coupling reaction to introduce a carbazole group to aromatic heterocycle compounds.
In-situ polymerized cross-linked binder for cathode in lithium-sulfur batteries
Heng Ye, Danni Lei, Lu Shen, Bin Ni, Baohua Li, Feiyu Kang, Yan-Bing He
2020, 31(2): 570-574  doi: 10.1016/j.cclet.2019.04.047
[摘要]  (212) [HTML全文] (212) [PDF 980KB] (212)
摘要:
Volume expansion and polysulfide shuttle effect are the main barriers for the commercialization of lithium-sulfur (Li-S) battery. In this work, we in-situ polymerized a cross-linked binder in sulfur cathode to solve the aforementioned problems using a facile method under mild conditions. Polycarbonate diol (PCDL), triethanolamine (TEA) and hexamethylene diisocyanate (HDI) were chosen as precursors to prepare the cross-linked binder. The in-situ polymerized binder (PTH) builds a strong network in sulfur cathode, which could restrain the volume expansion of sulfur. Moreover, by adopting functional groups of oxygen atoms and nitrogen atoms, the binder could effectively facilitate transportation of Li-ion and adsorb polysulfide chemically. The Li-S battery with bare sulfur and carbon/sulfur composite cathodes and cross-linked PTH binder displays much better electrochemical performance than that of the battery with PVDF. The PTH-bare S cathode with a mass loading of 5.97 mg/cm2 could deliver a capacity of 733.3 mAh/g at 0.2 C, and remained 585.5 mAh/g after 100 cycles. This in-situ polymerized binder is proved to be quite effective on restraining the volume expansion and suppressing polysulfide shuttle effect, then improving the electrochemical performance of Li-S battery.
Ba3LaNa(PO4)3F:Tm3+, Dy3+: A tunable blue-white color emitting phosphor via energy transfer for UV white LEDs
Dingdian Xu, Wei Zhou, Shujing Li, Dongsheng Bai
2020, 31(2): 575-578  doi: 10.1016/j.cclet.2019.04.046
[摘要]  (274) [HTML全文] (274) [PDF 1068KB] (274)
摘要:
A series of Tm3+/Dy3+ co-doped Ba3LaNa(PO4)3F (BLNPF) phosphors were synthesized successfully via a high-temperature solid-reaction, and luminescence properties were investigated. Upon near violet excitation, BLNPF:Tm3+, Dy3+ phosphors exhibit Tm3+:1D2-3F4 and Dy3+:4F9/2-6HJ (J = 15/2, 13/2, 11/2) transitions with different luminescence intensity. The emitting color of the obtained products was found to shift from blue to white as a result of efficient energy transfer (ET) from Tm3+ to Dy3+ ions. According to photoluminescence emission intensity, the positive effect of activator on ETefficiency was calculated and the maximum ET efficiency was found around 72.6% with Dy3+ concentration was 0.04. By means of Dexter's theoretical model, furthermore, dipole-dipole interaction was confirmed as the mechanism of energy transfer from Tm3+ to Dy3+ ions. The results suggested that BLNPF:Tm3+, Dy3+ phosphor might be a promising single-phased white-light-emitting phosphor for UV white-light LED.
Water-in-salt electrolyte ion-matched N/O codoped porous carbons for high-performance supercapacitors
Jingjing Yan, Dazhang Zhu, Yaokang Lv, Wei Xiong, Mingxian Liu, Lihua Gan
2020, 31(2): 579-582  doi: 10.1016/j.cclet.2019.05.035
[摘要]  (226) [HTML全文] (226) [PDF 824KB] (226)
摘要:
Pore size and distribution in carbon-based materials are regarded to be a key factor to affect the electrochemical capacitive performances of the resultant electrodes. In this study, nitrogen and oxygen codoped porous carbons (NOPCs) are fabricated based on a simple Schiff-base reaction between m-phenylenediamine and terephthalaldehyde. The NOPCs have tunable morphologies, high surface areas, abundant heteroatom doping. More importantly, the carbons show a dominant micropores of 0.5-0.8 nm, comparable to the ionic sizes of LiTFSI (Li+ 0.069 nm; TFSI-0.79 nm) water-in-salt electrolyte with a high potential window of 2.2 V. Consequently, the fabricated symmetric supercapacitor gives a high energy output of 30.5 Wh/kg at 1 kW/kg, and high stability after successive 10, 000 cycles with ~96.8% retention. This study provides promising potential to develop high-energy supercapacitors.
Nitrogen doped porous carbon as excellent dual anodes for Li-and Na-ion batteries
Zhanheng Yan, Qin-Wen Yang, Qinghong Wang, Jianmin Ma
2020, 31(2): 583-588  doi: 10.1016/j.cclet.2019.11.002
[摘要]  (232) [HTML全文] (232) [PDF 1173KB] (232)
摘要:
Biomass-derived carbon materials have obtained great attention due to their sustainability, easy availability, low cost and environmentally benign. In this work, bamboo leaves derived nitrogen doped hierarchically porous carbon have been efficiently synthesized via an annealing approach, followed by an etching process in HF solution. Electrochemical measurements demonstrate that the unique porous structure, together with the inherent high nitrogen content, endow the as-derived carbon with excellent lithium/sodium storage performance. The porous carbon annealed at 700 ℃ presents outstanding rate capability and remarkable long-term stability as anodes for both lithium-ion batteries and sodium-ion batteries. The optimized carbon delivers a high discharge capacity of 450 mAh/g after 500 cycles at the current density of 0.2 A/g for LIBs, and a discharge capacity of 180 mAh/g after 300 cycles at the current density of 0.1 A/g for SIBs
Communication
Unsymmetrical photochromic bithienylethene-bridge tetraphenylethene molecular switches: Synthesis, aggregation-induced emission and information storage
Liangwei Ma, Chengpeng Li, Qing Yan, Sheng Wang, Wangen Miao, Derong Cao
2020, 31(2): 361-364  doi: 10.1016/j.cclet.2019.07.040
[摘要]  (207) [HTML全文] (207) [PDF 776KB] (207)
摘要:
Aggregation-induced emission (AIE) active photochromic molecules have attracted growing attention for their versatile applications. Here we designed and synthesized five newly unsymmetrical photochromic diarylethene (DAE) dyads (BTE1-5) by connecting tetraphenylethene (TPE) and aromatic substituent via bithienylethene (BTE) bridge. The chemical structures of those compounds were identified by 1H NMR, 13C NMR and HRMS.The absorption and emission of these dyads were investigated by UV-vis and fluorescence spectroscopy, respectively. The results showed that all those compounds exhibited typically AIE or aggregation-induced emission enhancement (AIEE) characteristic. Particularly, when an aggregation caused quenching (ACQ) fluorophore (triphenylamine) was grafted to the molecule, connecting with TPE via BTE-bridge, the ACQ phenomenon was dissipated and converted to an AIE luminophore, and those compounds exhibited photochromism upon irradiation with alternative UV and visible light. The solution or solid of those compounds showed distinctly fluorescence switching "ON" or "OFF" observation upon irradiation with alternative UV and visible light.It is interesting that BTE1 could be applied in recording and rewritable information storage, and the cyclization quantum yields could be affected by substituent significantly.
Simple fabrication of superhydrophobic PLA with honeycomb-like structures for high-efficiency oil-water separation
Xiaolong Wang, Yamin Pan, Huan Yuan, Meng Su, Chunguang Shao, Chuntai Liu, Zhanhu Guo, Changyu Shen, Xianhu Liu
2020, 31(2): 365-368  doi: 10.1016/j.cclet.2019.07.044
[摘要]  (214) [HTML全文] (214) [PDF 925KB] (214)
摘要:
Polylactic acid (PLA) is one of the most suitable candidates for environmental pollution treatment because of its biodegradability which will not cause secondary pollution to the environment after application. However, there is still a lack of a green and facile way to prepare PLA oil-water separation materials. In this work, a water-assisted thermally induced phase separation method for the preparation of superhydrophobic PLA oil-water separation material with honeycomb-like structures is reported. The PLA material shows great ability in application and could adsorb 27.3 times oil to its own weight. In addition, it could also be applicated as a filter with excellent efficiency (50.9 m3 m-2 h-1).
Salt/current-triggered stabilization of β-cyclodextrins encapsulated host-guest low-molecular-weight gels
Huan Xu, Chaoyu Zhou, Chuanjiang Jian, Sunhai Yang, Miaochang Liu, Xiaobo Huang, Wenxia Gao, Huayue Wu
2020, 31(2): 369-372  doi: 10.1016/j.cclet.2019.07.048
[摘要]  (218) [HTML全文] (218) [PDF 1024KB] (218)
摘要:
Host-guest supramolecular gels were developed via the self-assembly of inclusion complexes (ICs) of β-cyclodextrins/phenylboronic acid gelator (PBA). Salts and current were involved in the self-assembly to stabilize the host-guest gels. The stability of the gels was greatly improved after salts were added. The stable time of gels was extended from 2.5 h to 120 h with the addition of NH4NO3 at the concentration of 2.5×10-2 g/mL. The morphology of the gel was affected by the concentrations of NH4NO3. SEM images revealed that the gels were three-dimensional nanofibrous networks, the sizes of fibers decreased with decreasing NH4NO3 concentrations, which affected the stability of gels, further proved by the rheological properties of gels. More stable gels were obtained with current stimulation, the stable time of the gel was increased from 2.5 h to 55 h with current by adding NaBF4. The current also exhibited significant influence on the aggregation as the voltage varied (0-500 mV) with a constant concentration of salts. The result showed the self-assembly process of host-guest gel could be well controlled via the addition of salts and current to desired morphology and stability.
Silver-mediated aminophosphinoylation of propargyl alcohols with aromatic amines and H-phosphine oxides leading to α-aminophosphine oxides
Qiang Huang, Lei Zhu, Dong Yi, Xiaohui Zhao, Wei Wei
2020, 31(2): 373-376  doi: 10.1016/j.cclet.2019.07.049
[摘要]  (194) [HTML全文] (194) [PDF 885KB] (194)
摘要:
A new silver mediated aminophosphinoylation of propargyl alcohols with aromatic amines and Hphosphine oxides for the construction of α-aminophosphine oxides has been developed. The C-N and C-P bond could be efficiently formed in one pot operation via sequential C-C and C-O bond cleavage of propargylic alcohols. This present methodology, which not only provides a simple and alternative strategy for the synthesis of α-aminophosphine oxides, but also opens a new window for the cleavage reactions of propargyl alcohols via dealkynalation coupling.
Remote regioselective organocatalytic asymmetric [3+2] cycloaddition of N-2, 2, 2-trifluoroethyl isatin ketimines with cyclic 2, 4-dienones
Chuncheng Zou, Yuanyuan Han, Chuikun Zeng, Tony Y. Zhang, Jinxing Ye, Gonghua Song
2020, 31(2): 377-380  doi: 10.1016/j.cclet.2019.07.052
[摘要]  (225) [HTML全文] (225) [PDF 935KB] (225)
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An organocatalytic asymmetric [3+2] cycloaddition of trifluoromethyl-containing azomethine ylides with cyclic 2, 4-dienones was developed. The process enables efficient incorporation of CF3 groups into functionalized spiro[pyrrolidin-3, 2'-oxindoles] in high yields with good to excellent enantio-and diastereoselectivities.
Highly efficient enantioselective synthesis of bispiro [benzofuran-oxindole/benzofuran-chromanone]s through organocatalytic inter-/intramolecular Michael cycloaddition
Min Zhang, Jun-Xin Wang, Shun-Qin Chang, Xiong-Li Liu, Xiong Zuo, Ying Zhou
2020, 31(2): 381-385  doi: 10.1016/j.cclet.2019.06.015
[摘要]  (224) [HTML全文] (224) [PDF 2547KB] (224)
摘要:
A quinine-derived thiourea-catalyzed inter-/intramolecular Michael cycloaddition of chromoneoxindole/benzofuranone synthons with 3-substituted methylenebenzofuranones has been established, which constructed enantiomerically pure bispiro[benzofuran-oxindole/benzofuran-chromanone]s bearing five consecutive stereocenters including two spiro quaternary carton centers in good yields (up to 93%) with high diastereoselectivities (up to >20:1 dr) and good enantioselectivities (up to >99% ee). Moreover, this is the first example of bifunctional chromone-benzofuranone synthon directed organocatalytic tandem reaction, and also the first example of the bispiro[benzofuran-oxindole] and bispirobenzofuranone, potentially useful in medicinal chemistry.
A heteropore covalent organic framework for adsorptive removal of Cd(Ⅱ) from aqueous solutions with high efficiency
Na Liu, Liangfeng Shi, Xianghao Han, Qiao-Yan Qi, Zong-Quan Wu, Xin Zhao
2020, 31(2): 386-390  doi: 10.1016/j.cclet.2019.06.050
[摘要]  (340) [HTML全文] (340) [PDF 1046KB] (340)
摘要:
A heteropore covalent organic framework (COF) integrating tetraphenylethene skeleton and catechol segment is designed and synthesized. It exhibits extremely high stability in water under different pH conditions, which makes it an excellent material for adsorptive removal of Cd(Ⅱ) from aqueous solutions with very fast adsorption kinetics, high uptake capacity, and good recyclability.
An efficient Bi/NH4I-mediated addition reaction for the highly diastereoselective synthesis of homoallylic alcohols in aqueous media
Zhen Wu, Xue-Xin Feng, Qing-Dong Wang, Xuan-Yu Liu, Weidong Rao, Jin-Ming Yang, Zhi-Liang Shen
2020, 31(2): 391-395  doi: 10.1016/j.cclet.2019.07.030
[摘要]  (205) [HTML全文] (205) [PDF 1009KB] (205)
摘要:
An efficient water-based bismuth-mediated addition reaction of carbonyl compound with cyclic allylic halide was developed. The reactions proceeded smoothly in aqueous DMF in the presence of ammonium iodide to afford the corresponding syn-homoallylic alcohols in moderate to good yields with excellent diastereoselectivities (>99:1 syn:anti). Reversal of product diastereoselectivity was observed when heteroaryl aldehyde possessing an adjacent chelating nitrogen atom was employed as substrate.
Ring opening [3+2] cyclization of azaoxyallyl cations with benzo[d]isoxazoles: Efficient access to 2-hydroxyaryloxazolines
Yicheng He, Chao Pi, Yangjie Wu, Xiuling Cui
2020, 31(2): 396-400  doi: 10.1016/j.cclet.2019.09.025
[摘要]  (199) [HTML全文] (199) [PDF 884KB] (199)
摘要:
A selective ring-opening [3+2] cyclization reaction of benzo[d]isoxazoles with 2-bromo-propanamides has been developed. The azaoxyallyl cation intermediates are employed as C~O 3-atom synthon to build oxa-heterocycles via the selectivity of suitable cyclization partners. This transformation provides rapid access to highly functionalized 2-hydroxyaryl-oxazolines under mild conditions and excellent regioselectivity.
Seven-step total synthesis of α-cyclopiazonic acid
Shibin Shi, Kuo Yuan, Yanxing Jia
2020, 31(2): 401-403  doi: 10.1016/j.cclet.2019.06.048
[摘要]  (218) [HTML全文] (218) [PDF 797KB] (218)
摘要:
A seven-step total synthesis of α-cyclopiazonic acid is reported from a commercially available 4-bromoindole. Salient feature of the work is the rapid formation of tetracyclic skeleton via a bioinspired [3+2] annulation to form the C/D rings.
Design, synthesis and biological evaluation of novel phthalazinone acridine derivatives as dual PARP and Topo inhibitors for potential anticancer agents
Qiuzi Dai, Jiwei Chen, Chunmei Gao, Sun Qinsheng, Zigao Yuan, Jiang Yuyang
2020, 31(2): 404-408  doi: 10.1016/j.cclet.2019.06.019
[摘要]  (206) [HTML全文] (206) [PDF 963KB] (206)
摘要:
In this study, we designed and synthesized a series of phthalazinone acridine derivatives as dual PARP and Topo inhibitors. MTT assays indicated that most of the compounds significantly inhibited multiple cancer cells proliferation. In addition, all the compounds displayed Topo Ⅱ inhibition activity at 10 mol/L, and also possessed good PARP-1 inhibitory activities. Subsequent mechanistic studies showed that compound 9a induced remarkable apoptosis and caused prominent S cell cycle arrest in HCT116 cells. Our study suggested that 9a inhibiting Topo and PARP concurrently can be a potential lead compound for cancer therapy.
N-(2-Phenoxy)ethyl imidazo[1, 2-a]pyridine-3-carboxamides containing various amine moieties: Design, synthesis and antitubercular activity
Linhu Li, Apeng Wang, Bin Wang, Mingliang Liu, Kai Lv, Zeyu Tao, Chao Ma, Xican Ma, Bing Han, Aoyu Wang, Yu Lu
2020, 31(2): 409-412  doi: 10.1016/j.cclet.2019.07.038
[摘要]  (200) [HTML全文] (200) [PDF 673KB] (200)
摘要:
Seven 2, 6-disubstituted N-(2-phenoxy)ethyl imidazo[1, 2-a]pyridine-3-carboxamide series containing various amine moieties were designed and synthesized as new anti-TB agents. Many of them show excellent in vitro activity against both drug-sensitive MTB strain H37Rv and two MDR-MTB clinical isolates (MIC: < 0.002-0.030 μg/mL). Compounds 2f, 5e and 5g display acceptable safety and pharmacokinetic profiles, opening a new direction for further development.
Discovery of synergistic activity of fluoroquinolones in combination with antimicrobial peptides against clinical polymyxin-resistant Pseudomonas aeruginosa DK2
Xinyu Zheng, Qiao Cao, Qin Cao, Fei Mao, Xiaokang Li, Jin Zhu, Lefu Lan, Jian Li
2020, 31(2): 413-417  doi: 10.1016/j.cclet.2019.07.063
[摘要]  (214) [HTML全文] (214) [PDF 754KB] (214)
摘要:
Polymyxin B (PB), as the last-line of defense against multidrug-resistant Gram-negative bacteria, has caused resistance to P. aeruginosa recently. Fortunately, synergistic treatment could preserve the last class of antibiotics and reduce the emergency of drug resistance. Here, we performed a screen of 970 approved drugs synergized with PB against the P. aeruginosa DK2, which is severely resistant to PB, MIC = 512 μg/mL. Encouragingly, we found fluoroquinolones could synergy with PB and achieved an obvious reduction in MIC of PB below the clinical susceptible breakpoint (2 μg/mL). Especially, gemifloxacin achieved the highest synergistic effect with PB, leading to a 4096-fold MIC reduction (reduced from 512 μg/mL to 0.125 μg/mL). Furthermore, synergistic effect was also observed in the combination of gemifloxacin and colistin. Finally, outer membrane permeabilization assay showed that gemifloxacin could increase the permeability of bacterial cell membranes for P. aeruginosa which partly explained the synergy mechanism. These results indicate that fluoroquinolones represent attractive synergists to address the emerging threat of polymyxin-resistant infections.
Discovery of [1, 2, 4]triazolo[1, 5-a]pyrimidine derivatives as new bromodomain-containing protein 4 (BRD4) inhibitors
Shuai Wang, Dandan Shen, Lijie Zhao, Xiaohan Yuan, Jialing Cheng, Bin Yu, Yichao Zheng, Hongmin Liu
2020, 31(2): 418-422  doi: 10.1016/j.cclet.2019.08.029
[摘要]  (213) [HTML全文] (213) [PDF 1050KB] (213)
摘要:
Targeting bromodomain-containing protein 4 (BRD4) has been proved to be an effective strategy for cancer therapy. To date, numerous BRD4 inhibitors and degraders have been identified, some of which have advanced into clinical trials. In this work, a focused library of new [1, 2, 4]triazolo[1, 5-a]pyrimidine derivatives were discovered to be able to inhibit BRD4. WS-722 inactivated BRD4 (BD1/BD2), BRD2 (BD1/BD2) and BRD3 (BD1/BD2) broadly with the IC50 values less than 5 μmol/L. Besides, WS-722 inhibited growth of THP-1 cells with an IC50 value of 3.86 μmol/L. Like (+)-JQ1, WS-722 inhibited BRD4 in a reversible manner and enhanced protein stability. Docking studies showed that WS-722 occupied the central acetyl-lysine (Kac) binding cavity and formed a hydrogen bond with Asn140. In THP-1 cells, WS-722 showed target engagement to BRD4. Cellular effects of WS-722 on THP-1 cells were also examined, showing that WS-722 could block c-MYC expression, induce G0/G1 phase arrest and p21 up-regulation, and promote differentiation of THP-1 cells. BRD4 inhibition by WS-722 resulted in cell apoptosis and upregulated expression of cleaved caspased-3/7 and PARP in THP-1 cell lines. The [1, 2, 4]triazolo[1, 5-a] pyrimidine is a new template for the development of new BRD4 inhibitors.
New seco-dibenzocyclooctadiene lignans with nitric oxide production inhibitory activity from the roots of Kadsura longipedunculata
Xinzhu Qi, Jiabao Liu, Jiabao Chen, Qi Hou, Shuai Li
2020, 31(2): 423-426  doi: 10.1016/j.cclet.2019.06.006
[摘要]  (205) [HTML全文] (205) [PDF 727KB] (205)
摘要:
Four new seco-dibenzocyclooctadiene lignans, kadlongilignans A-D (1-4), consisting of a rare 6, 7-seco-(1), two 15, 16-seco-(2 and 3) and a 9, 10-seco-dibenzocyclooctadiene (4) lignans, were isolated from the roots of Kadsura longipedunculata. Their structures were elucidated by spectroscopic analysis, including extensive NMR, MS and ECD (electronic circular dichroism) spectra. Compounds 3 and 4 exhibited potent inhibitory activities against NO (nitric oxide) production of LPS (lipopolysaccharide)-induced murine macrophages with the inhibition rates of 36.3% and 26.9%, respectively.
Anti-NLRP3 inflammasome abietane diterpenoids from Callicarpa bodinieri and their structure elucidation
Junbo Gao, Xingjie Zhang, Kun Shang, Weimao Zhong, Ruihan Zhang, Xiaochang Dai, Xiaoli Li, Qi Wang, Yan Zou, Weilie Xiao
2020, 31(2): 427-430  doi: 10.1016/j.cclet.2019.09.020
[摘要]  (210) [HTML全文] (210) [PDF 825KB] (210)
摘要:
Callicarpa bodinieri is a Chinese traditional medicine herbwith anti-inflammatory activity in clinic. Herein, we report two new 9, 10-seco and etherified abietane diterpenoids bodinieric acids J and K(1 and 2)and one known compound (3) isolated from the leaves and twigs of this plant. Their chemical structures were elucidated by detailed spectrometry data analysis and DP4+ NMR calculation methods. Hypothetical biosynthetic pathways of 1-3 were preliminarily speculated. Compound 3 inhibited inflammasome activation and exhibited blockage of NLRP3 inflammasome activation at non-cytotoxic concentrations in vitro.
Euphoractone, a cytotoxic meroterpenoid with an unusual ent-abietane-phloroglucinol skeleton, from Euphorbia fischeriana Steud.
Rihan Xie, Linsheng Li, Xiaona Fan, Jiachen Zi
2020, 31(2): 431-433  doi: 10.1016/j.cclet.2019.07.068
[摘要]  (208) [HTML全文] (208) [PDF 710KB] (208)
摘要:
A novel meroterpenoid, euphoractone (1), was isolated from the extracts of the roots of Euphorbia fischeriana Steud. Its structure was determined by spectroscopic methods and X-ray crystallography. 1 possesses an unusual ent-abietane-phloroglucinol skeleton. The plausible biosynthetic pathway for 1 was proposed.1 showed inhibitory activities against human lung cancer H23 and H460 cells with the IC50 values of 21.07±3.54 and 20.91±4.07 μmol/L.
Synthesis, in vitro antibacterial and antifungal evaluation of novel 1, 3, 4-oxadiazole thioether derivatives bearing the 6-fluoroquinazolinylpiperidinyl moiety
Jun Shi, Na Luo, Muhan Ding, Xiaoping Bao
2020, 31(2): 434-438  doi: 10.1016/j.cclet.2019.06.037
[摘要]  (181) [HTML全文] (181) [PDF 784KB] (181)
摘要:
A series of structurally novel 1, 3, 4-oxadiazole thioether derivatives (6a-6z) containing a 6-fluoroquinazolinylpiperidinyl moiety were designed and synthesized using pharmacophore hybrid approach, and their structures were fully characterized by 1H NMR, 13C NMR and HRMS spectra. Among them, the structure of compound 6d was further corroborated via single-crystal X-ray diffraction analysis. In vitro antibacterial bioassays showed that compounds 6a, 6g, 6u and 6v possessed EC50 values of 30.4, 30.6, 27.5 and 26.0 μg/mL against phytopathogenic bacterium Xanthomonas oryzae pv. oryzae, respectively, which were significantly superior to that of commercially-available bactericide Bismerthiazol (85.1 μg/mL). Moreover, in vitro antifungal bioassays indicated that seven compounds demonstrated broad-spectrum fungicidal acitivties against six types of phytopathogenic fungi at 50 μg/mL. The present work showed the potential of 1, 3, 4-oxadiazole thioether derivatives carrying a 6-fluoroquinazolinylpiperidinyl moiety as effective antimicrobial agents for crop protection, deserving further investigations in the future.
Constructing boronate-bridged core-satellite gold nanoassembly and its application in high sensitive colorimetric detection of benzoyl peroxide residues in food matrices
Ting Li, Jiefang Sun, Jinyuan Liu, Baolei Dong, Huachao Zhao, Xiaoting Qiao, Wencong Shan, Jing Zhang, Bing Shao
2020, 31(2): 439-442  doi: 10.1016/j.cclet.2019.08.051
[摘要]  (200) [HTML全文] (200) [PDF 816KB] (200)
摘要:
Here, a new designed core/satellite gold nanoprobe was developed for detecting trace mount of benzoyl peroxide (BPO) based on its deboronation. This gold nanoassembly (the BE-AuNPs12/65) was constructed via borate ester formation between large 4-mercaptophenylboronic acid (MPBA) modified AuNPs (the MPBA-AuNPs65, as cores)and smalldopamine modifiedAuNPs (theDPA-AuNPs12, assatellites).Particularly, upon addition of BPO, it would trigger the deboronation for the BE-AuNPs12/65 probes accompanying with distinct color changes from blue, purple to wine red, which implied the disassembly of the core/satellite nanostructure after the breakage of carbon to boron chemical bond. By measuring the absorbance ratio at 665 nm and 545 nm, quantification of BPO was achieved in the range of 10.0-100.0 nmol/L, which could also be easilyobserved bynaked eyes. The nanoprobeutilized a boronate deprotection mechanism and the LSPR properties of AuNPs to provide high selectivity for detecting BPO over similar ROS/RNS with the limit of detection as low as 7.2 nmol/L. The practical applicability of this assay was verified through successful determining BPO in flour samples, which demonstrated its great potentials in food safety field.
FRET-based ratiometric fluorescent detection of arginine in mitochondrion with a hybrid nanoprobe
Yueyue Li, Yanan Ban, Ruihui Wang, Zheng Wang, Zhanxian Li, Chenjie Fang, Mingming Yu
2020, 31(2): 443-446  doi: 10.1016/j.cclet.2019.07.047
[摘要]  (199) [HTML全文] (199) [PDF 769KB] (199)
摘要:
A ratiometric fluorescent hybrid nanoprobe CDs-1 for arginine (Arg), exhibiting high sensitivity (the limit of detection, LOD, being 6.5×10-8 mol/L) and excellent selectivity and anti-interference ability, was fabricated through fluorescence resonance energy transfer (FRET) and the electrostatic attraction between positively-charged hemicyanine molecules and negatively-charged carbon dots (CDs). Arg can be quantitatively detected in the concentration range from 6.0×10-5 mol/L to 2.7×10-4 mol/L. Further, due to its ability to target mitochondrion and low cytotoxicity, intracellular Arg was successfully tracked through ratiometric fluorescence imaging.
A bright two-photon fluorescent probe for real-time monitoring autophagy in living cells
Chuankun Jiang, Longchun Li, Jiacheng Jiang, Lilin Hou, Gemin Fang, Haizhu Yu, Xiangming Meng
2020, 31(2): 447-450  doi: 10.1016/j.cclet.2019.07.046
[摘要]  (205) [HTML全文] (205) [PDF 5586KB] (205)
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A novel donor-acceptor (D-A) type of two-photon (TP) fluorescent probe, i.e. Lyso-OSC, based on the lysosome-targeting morpholine group was developed. The polarity sensing coumarin group was functionalized as the acceptor and the 1-vinyl-4-methoxybenzene group was engineered as the donor. The fluorescence intensity and emission maximum wavelength of Lyso-OSC are highly sensitive to the polarity changes of solvent. The two-photon absorption cross-section and tissue penetration depth are up to 254 GM and 150 μm, respectively. The strong fluorescence, high sensitivity to polarity, low cytotoxicity, and accurate lysosome-targeting ability entail Lyso-OSC the excellent performance in detecting the polarity changes of cellular environment. To this end, a bright, real-time imaging autophagy of living cells has been achieved.
Imitation of drug metabolism in cell co-culture microcapsule model using a microfluidic chip platform coupled to mass spectrometry
Yajing Zheng, Zengnan Wu, Jin-Ming Lin, Ling Lin
2020, 31(2): 451-454  doi: 10.1016/j.cclet.2019.07.036
[摘要]  (197) [HTML全文] (197) [PDF 920KB] (197)
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In this work, a multi-functional analysis platform by coupling a microfluidic chip to a mass spectrometry (MS) detector was described. We constructed a three-dimensional tumor-endothelial co-culture model for simulating drug resistance during tumor treatment. On this specially designed integrated platform, the first step was to prepare heterogeneous cell-encapsulated alginate microcapsules for threedimensional co-culture, and the second step was to achieve on-line perfusion culture and continuous drug stimulation on chip. It facilitates cell proliferation analysis and the collection of metabolism medium. After micro solid phase extraction column (SPE) pretreatment, subsequent mass spectrometry could detect drug metabolism. The high activity of two kinds of cells (A549 and HUVEC) shows the biocompatibility of the platform. Paclitaxel was used as a model drug, the distinctions of drug absorption between the mono-culture group and co-culture group were clearly observed by electrospray ionization quadrupole time-of-flight mass spectrometry (ESI-Q-TOF MS). Therefore, the integrated platform has shown promise as a high throughput, low cost for cell metabolism research and drug screening processes.
A fast and colorimetric sensor array for the discrimination of ribonucleotides in human urine samples by gold nanorods
Dan Yuan, Huihong Yan, Jiahui Liu, Jiajun Liu, Chunmei Li, Jian Wang
2020, 31(2): 455-458  doi: 10.1016/j.cclet.2019.07.067
[摘要]  (192) [HTML全文] (192) [PDF 848KB] (192)
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Ribonucleotides are usually functioned as biomarkers to diagnose diseases and monitor the life activities in living organisms, and their discrimination is of great significance but challenging. Taking advantage of the unique characteristics of gold nanorods (AuNRs), herein, a colorimetric sensor array for discrimination of twelve ribonucleotides was developed based on the chemical etching of AuNRs with controllable aspect ratios. During the etching process, AuNRs were preferentially shortened and eventually turned into Au(Ⅲ) state by Fenton's reaction. The morphological change of AuNRs led to the significant color change and blue shift in the corresponding extinction spectrum. However, when Fe2+ bound with ribonucleotides, the Fenton's reaction was prevented and the ability to etch AuNRs was weakened or disappeared. Due to the different structures of nucleotides, the binding ability of them with Fe2+ was distinct, resulting in the discrepancy in the chemical etching of AuNRs, which could be developed for distinguishing ribonucleotides. Moreover, the proposed sensor array was successfully explored to distinguish ribonucleotides in complex human urine samples.
Electrochemical detection of cell concentration based on reaction of DNA with molybdate
Wenzhuo Zhang, Xingxing Jiang, Shuping Liu, Dan Zhao, Minghui Yang
2020, 31(2): 459-462  doi: 10.1016/j.cclet.2019.08.050
[摘要]  (213) [HTML全文] (213) [PDF 804KB] (213)
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This article describes a fast and simple electrochemical assay for detecting cell concentration. After cell death, the membrane of cells will be broken, and DNA molecules contained in the cells will be released, but this does not happen in living cells. Sodium molybdate can react with the phosphate backbone of the released DNA molecules to form phosphomolybdate precipitation and produces a corresponding redox current. The higher the concentration of DNA, the stronger the intensity of the current generated. Sodium molybdate solution and centrifuged cell supernatant were added onto the glassy carbon electrode to determine the cell concentration by measuring the current intensity. The cell viability, which means the ratio of living cells to the total cells, can also be determined by this method. This assay has the advantages of high sensitivity, low detection limit, and wide detection range. In addition, this method was successfully applied to the detection of cell concentration in human serum, which has potential clinical applications.
A FRET biosensor reveals free zinc deficiency in diabetic betacell vesicles
Yi Xian, Mengxuan Zhou, Shangchen Han, Rong Yang, Yi Wang
2020, 31(2): 468-472  doi: 10.1016/j.cclet.2019.08.012
[摘要]  (189) [HTML全文] (189) [PDF 956KB] (189)
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The concentration of free zinc within insulin-storing vesicles is important for vesicle maturity and therefore requires accurate measurement. However, common small-molecule intensity-based probes and most available genetically encoded Förster resonance energy transfer (FRET)-based sensors for zinc are unsuitable for estimating the free zinc concentration in insulin-storing vesicles. Therefore, we have developed a novel FRET-based zinc sensor based on the RING motif of TRIM72, referred to as ZnT72R, which has an approximate Kd that varies from 6.07±0.28 μmol/L to 7.84±0.42 μmol/L in vitro and a cytosol-calibrated Kd of approximately 55.56±4.59 μmol/L in HEK293 T cells. To pinpoint the free zinc concentration of insulin-storing vesicles, we initially targeted ZnT72R to beta-cell vesicles by fusing them to NPY (neuropeptide Y). Following NPY-ZnT72R labeling, the FRET intensity ratios of vesicles were quantified. We found that the free zinc concentration in insulin-storing vesicles of diabetic db/db mice (28.30±1.33 μmol/L) was significantly lower than that of control mice (41.46±3.53 μmol/L).
Rapid ultrasensitive monitoring the single-particle surface-enhanced Raman scattering (SERS) using a dark-field microspectroscopy assisted system
Shaochuang Liu, Yilun Ying, Yitao Long
2020, 31(2): 473-475  doi: 10.1016/j.cclet.2019.07.057
[摘要]  (195) [HTML全文] (195) [PDF 814KB] (195)
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The observation of single-particle surface-enhanced Raman scattering (SERS) has generated considerable interest both in the nanomaterials filed and in the single-particle spectroscopy community. It is a challenge to realize rapid, facile, and high throughput SERS at single nanoparticle level. Here, without the complex experimental device and difficult experimental operations, a general single-particle SERS technique has been achieved by using dark-field-assisted surface-enhanced Raman spectroscopy (DFSERS). This advanced method provides in-situ characterization of the chemical reaction performance at single gold nanorod.
Effect of Dai-Bai-Jie on the proliferation and migration of the A549 cells
Binxin Lin, Xinling Lu, Nan Li, Ning Xu, Jin-Ming Lin
2020, 31(2): 476-478  doi: 10.1016/j.cclet.2019.07.066
[摘要]  (206) [HTML全文] (206) [PDF 855KB] (206)
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Lung cancer is the most malignant tumor disease with the highest diagnosis and mortality rate in China. The development of therapeutic drugs is the current research focus. Dai-Bai-Jie is a traditional medicine of the Dai nationality, which is commonly used in the treatment of decreasing swelling, alleviating pain and detoxification. Most of the current researches focused on the component analysis of Dai-Bai-Jie, but few researches studied on its antitumor and pharmacological effect. In this study, we incubated A549 cells with different concentrations of Dai-Bai-Jie. The cell proliferation experiment showed that the DaiBai-Jie solution inhibited the proliferation of A549 cells and caused cell apoptosis. In this work, we confirmed that Dai-Bai-Jie had an inhibitory effect on the proliferation and migration of non-small cell lung cancer A549, which may be used as a novel candidate of anti-tumor therapy for lung cancer patients.
Revealing the kinetics of ionophore facilitating ion transport across lipid bilayers by surface enhanced infrared absorption spectroscopy
Qianwen Zhang, Yang Liu, Jian Li, Xinghua Xia
2020, 31(2): 479-481  doi: 10.1016/j.cclet.2019.08.009
[摘要]  (205) [HTML全文] (205) [PDF 765KB] (205)
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Ionophore can prominently improve the ion permeability of cell membrane and disrupt cellular ion homeostasis. Most studies regarding ionophore facilitating ion transmembrane transport focus on artificial liquid-liquid interfaces, which have large difference from the actual environment of cell membrane. Here, we construct a supported lipid bilayer on a gold nanoparticles film modified ZnSe prism as an appropriate model of cell membrane to investigate the dynamic of the ion transport facilitated by ionophore using surface enhanced infrared absorption spectroscopy (SEIRAS). We find that the ion transmembrane transport consists of two steps: The ion transmembrane transport starts with the association/disassociation between ion and ionophore at the edge of lipid bilayer; The second step is the transfer of ion-ionophore complex across lipid bilayer. Our results show that the complex transfer across the lipid bilayer is the rate determining step.
Identification and quantification of benzimidazole metabolites of thiophonate-methyl sprayed on celery cabbage using SiO2@NiO solid-phase extraction in combination with HPLC-MS/MS
Qiongwei Yu, Shijie Liu, Feng Zheng, Huaming Xiao, Hongyan Guan, Yuqi Feng
2020, 31(2): 482-486  doi: 10.1016/j.cclet.2019.07.065
[摘要]  (199) [HTML全文] (199) [PDF 798KB] (199)
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Thiophonate-methyl (TPM) is one of fungicides and pesticides widely used in agriculture field. However, the residue of its benzimidazole (BZD) metabolites in related agricultural products poses a potential risk to consumers. In this paper, nickel oxide nanoparticle-deposited silica (SiO2@NiO) composite was used for the selective enrichment and purification of TPM's BZD metabolites in celery cabbage sprayed with TPM. Meanwhile, high-performance liquid chromatography coupled with precursor ion scan-mass spectrometry (HPLC-PIS-MS) and high-resolution MS/MS analysis (HR-MS/MS) was utilized for their qualitative and quantitative analysis. Twenty-one potential TPM's BZD metabolites were found and four of them were identified. One metabolite was discovered for the first time. Besides, a robust and sensitive quantitative method was developed with good linearities (R2 > 0.9972) within a wide range of 10.00-1000 ng/g. The detection limits of three known TPM's metabolites were within the range of 3.20-4.90 ng/g. Relative standard deviations (RSDs) of intra-day and inter-day precisions were less than 18.3%, which showed perfect reproducibility. The method was successfully applied to monitoring TPM's BZD metabolites in celery cabbage sprayed with TPM and the concentration versus time curves of TPM's metabolites in celery cabbage were plotted. This method is expected to be used to monitor BZD residues in various fruits and vegetables.
Synthesis of carbon dots with a tunable photoluminescence and their applications for the detection of acetone and hydrogen peroxide
Shitong Cui, Yanfen Wu, Yao Liu, Qingwen Guan, Yida Zhang, Yilin Zhang, Song Luo, Meng Xu, Juncheng Wang
2020, 31(2): 487-493  doi: 10.1016/j.cclet.2019.04.014
[摘要]  (198) [HTML全文] (198) [PDF 1038KB] (198)
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Carbon dots (CDs) with multi-color emissive properties and a high photoluminescent quantum yield (PLQY) have attracted great attention recently due to their potential applications in chemical, environmental, biological and photo-electronic fields. Solvent-dependent effect in photoluminescence provides a facial and effective approach to tune the emission of CDs. In this study, green emissive nitrogen-doped carbon dots (N-CDs) are synthesized from p-hydroquinone and ethylenediamine through a simple hydrothermal method. The as-prepared N-CDs possess a robust excitation-independent green luminescence and a high PLQYof up to 15.9%. Further spectroscopic characterization indicates that the high PLQY is achieved by the balance of nitrogen doping states and the surface passivation extent in CDs. The N-CDs also exhibit solvent-dependent multi-color emissive property and distinct PLQY in different solvents (the maximum can reach up to 25.3%). Furthermore, the as-prepared N-CDs are applied as fluorescence probes to detect acetone and H2O2 in water. This method has exhibited a low detection limit of acetone (less than 0.1%) and a quick and linear response to the H2O2 with the concentration from 0 to 120 μmol/L. This work broadens the knowledge of applying CDs as probes in the bio and chemical sensing fields.
Core-shell lipid-polymer nanoparticles as a promising ocular drug delivery system to treat glaucoma
Yang Zhou, Aiping Fang, Fazhan Wang, Huili Li, Quansheng Jin, Lingjing Huang, Chunmei Fu, Jun Zeng, Zhaohui Jin, Xiangrong Song
2020, 31(2): 494-500  doi: 10.1016/j.cclet.2019.04.048
[摘要]  (209) [HTML全文] (209) [PDF 1092KB] (209)
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Nowadays, tremendous researches have been focused on the core-shell lipid-polymer nanoparticles (LPNs) due to the advantages of both liposomes and polymer nanoparticles. In this work, LPNs were applied to encapsulate brinzolamide (Brz-LPNs) for achieving sustained drug release, improving drug corneal permeation and enhancing drug topical therapeutic effect. The structure of Brz-LPNs was composed of poly(lactic-co-glycolic) acid (PLGA) nanocore which encapsulated Brz (Brz-NPs) and lipid shell around the core. Brz-LPNs were prepared by a modified thin-film dispersion method. With the parameters optimization of Brz-LPNs, optimal Brz-LPNs showed an average particle size of 151.23±1.64 nm with a high encapsulation efficiency (EE) of 86.7%±2.28%. The core-shell structure of Brz-LPNs were confirmed by transmission electronic microscopy (TEM). Fourier transformed infrared spectra (FTIR) analysis proved that Brz was successfully entrapped into Brz-LPNs. Brz-LPNs exhibited obvious sustained release of Brz, compared with AZOPT® and Brz-LPs. Furthermore, the corneal accumulative permeability of Brz-LPNs significantly increased compared to the commercial available formulation (AZOPT®) in vitro. Moreover, Brz-LPNs (1 mg/mL Brz) showed a more sustained and effective intraocular pressure (IOP) reduction than Brz-LPs (1 mg/mL) and AZOPT® (10 mg/mL Brz) in vivo. In conclusion, Brz-LPNs, as promising ocular drug delivery systems, are well worth developing in the future for glaucoma treatment.
Polymeric nanoparticles of poly(2-oxazoline), tannic acid and doxorubicin for controlled release and cancer treatment
Lin Liu, Liying Yin, Hang Bian, Ning Zhang
2020, 31(2): 501-504  doi: 10.1016/j.cclet.2019.04.041
[摘要]  (203) [HTML全文] (203) [PDF 886KB] (203)
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A straightforward coassembly strategy was developed for the preparation of polymeric nanoparticles driving by the intermolecular hydrogen bond between neutral poly(2-methyl-2-oxaozline) (PMeOx), tannic acid (TA) and doxorubicin hydrochloride (Dox). The occurrence of the hydrogen-bonding amongst the different functionalities within the formed nanoparticles was verified by infrared (IR) spectroscopy. Scanning electron microscopy (SEM), dynamic light scattering (DLS), UV-vis absorption and photoluminescent measurements indicated the rapid formation of uniform and water dispersible/stable nanoparticles. The relative poor stability of PMeOx-TA-Dox in fetal bovine serum (FBS) solution enabled the rapid separation of Dox and PMeOx-TA, facilitating the release of Dox and its entrance into cellular nuclei as revealed by confocal laser scanning microscopy (CLSM). The presented strategy may provide an efficient alternative for the construction of multifunctional nanomedicines.
Tunable morphologies of polymer capsules templated from cuprous oxide particles for control over cell association
Hongyan Pei, Yanyan Bai, Jianman Guo, Zhiliang Gao, Qiong Dai, Qun Yu, Jiwei Cui
2020, 31(2): 505-508  doi: 10.1016/j.cclet.2019.04.049
[摘要]  (186) [HTML全文] (186) [PDF 893KB] (186)
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Over the past two decades, layer-by-layer (LbL) assembly of micro/nanocapsules has been of interest for the investigation of bio-nano interactions to explore bio-applications, such as drug delivery. The choice of an appropriate template that can be easily dissolved under mild conditions is one of the challenges for the assembly of LbL capsules. Herein, we report the engineering of LbL capsules with tunable morphologies using cuprous oxide (Cu2O) particles as templates. Cu2O particles with cubic, tetradecahedral or spherical morphologies were synthesized via hydrothermal processes, which can be dissolved under mild condition (e.g., sodium thiosulfate solution). The influence of capsule morphologies on cell association was investigated, which indicates that LbL capsules with cubic geometry promoted cell association up to 4 and 9-fold than tetradecahedral and spherical capsules, respectively. The reported method provides a new avenue for the assembly of LbL capsules with different morphologies, which has the potential for better understanding of biological interactions of LbL capsules.
Nanoscale mechanical property of marine and continental organic kerogen in shale
Quan Xu, Rui Zhang, Mao Sheng, Shouceng Tian, Wuguang Li, Tianyu Wang, Yilin Zhang
2020, 31(2): 509-512  doi: 10.1016/j.cclet.2019.04.060
[摘要]  (202) [HTML全文] (202) [PDF 892KB] (202)
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Kerogen is known as an important organic part for absorbing and forming shale gas whose absorption function, especially mechanical and tribological properties, has not been fully revealed. Here, we use Fourier transform infrared (FTIR) and X-ray photoelectron spectroscopy (XPS) analysis to reveal the chemical structure of kerogen. We report the first study of the adhesion and friction behavior of kerogen using atomic force microscope (AFM) Nanoman technology. Our finding reveals the friction of kerogen is decreased at higher pressure while is inhibited at increased temperature, and friction decreases logarithmically as the sliding speed increases. The weakened of Al-O linkage at high temperature have great influence on the decrease of friction forces between kerogen and alumina pellet. This finding lays the mechanism for understanding the dynamic adhesion behavior of kerogen in frictions, therefore attracting increasing interests from scientists, researchers, petroleum engineers and investors.
Preparation of carbon nitride nanoparticles by nanoprecipitation method with high yield and enhanced photocatalytic activity
Ziyu Gan, Chaofeng Huang, Yanfei Shen, Qing Zhou, Dan Han, Jin Ma, Songqin Liu, Yuanjian Zhang
2020, 31(2): 513-516  doi: 10.1016/j.cclet.2019.04.065
[摘要]  (211) [HTML全文] (211) [PDF 843KB] (211)
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As an emerging 2D conjugated material, graphitic carbon nitride (CN) has attracted great research attention as important catalytic medium for transforming solar energy. Nanostructure modulation of CN is an effective way to improve catalytic activities and has been extensively investigated, but remains challenging due to complex processes, time consuming or low yield. Here, taking advantage of recent discovered good solvents for CN, a nanoprecipitation approach using poor solvents is proposed for preparation of CN nanoparticles (CN NPs). With simple processes of CN dissolution and precipitation, we can quickly synthesize CN NPs (~40 nm) with a yield of up to 50%, the highest one to the best of our knowledge. As an example of potential applications, the as-prepared CN NPs were applied to photocatalytic degradation of dyes with an evident boosted performance up to 2.5 times. This work would open a new way for batch preparation of nanostructured CN and pave its large-scale industrial applications.
One-dimensional HKUST-1 nanobelts from Cu nanowires
Qin Li, Wei Zhu, Yuebin Lian, Yang Peng, Zhao Deng
2020, 31(2): 517-520  doi: 10.1016/j.cclet.2019.05.005
[摘要]  (190) [HTML全文] (190) [PDF 851KB] (190)
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The controllable synthesis of one-dimensional (1D) structural morphology of metal-organic frameworks (MOFs) is significant for its application in catalysis, sense and gas separation. In this communication, we report a simple and moderate synthetic strategy to obtain uniform HKUST-1 nanobelts (NBs) by using copper nanowires (Cu NWs) as a metal source as well as a template. The control experiments showed that synergy between metal dissolution rate and crystal formation plays a key role in the formation of nanobelts. Our study represents an attractive synthetic strategy of 1D MOFs-based material for applications.
Two-dimensional mesoporous sensing materials
Yu Wen, Facai Wei, Wenqian Zhang, Anyang Cui, Jing Cui, Chengbin Jing, Zhigao Hu, Qingguo He, Jianwei Fu, Shaohua Liu, Jiangong Cheng
2020, 31(2): 521-524  doi: 10.1016/j.cclet.2019.04.071
[摘要]  (205) [HTML全文] (205) [PDF 846KB] (205)
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Two-dimensional mesoporous materials combing ultrathin nanosheet morphology with well-defined mesoporous structures, are now emerging and becoming increasingly important for their promising applications in energy storage, electronic devices, electrocatalysts and so on. Here, we synthesized a kind of polypyrrole-based two-dimensional mesoporous materials with uniform pore size, ultrathin thickness and high surface area. Serving for electrochemical NH3 sensor, they exhibited a fast response and high sensitivity. Therefore, our study would promote much interest in design of new materials for gas sensor applications.
Carbon layer-coated ordered mesoporous silica supported Co-based catalysts for higher alcohol synthesis: The role of carbon source
Siqi Fan, Yue Wang, Zhuoshi Li, Zhuang Zeng, Shaoxia Guo, Shouying Huang, Xinbin Ma
2020, 31(2): 525-529  doi: 10.1016/j.cclet.2019.04.070
[摘要]  (194) [HTML全文] (194) [PDF 874KB] (194)
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Surface chemical properties of supports have an important influence on active sites and their catalytic behavior. Here, we fabricated a series of cobalt-based catalysts supported by carbon layer-coated ordered mesoporous silica (OMS) composites for higher alcohol synthesis (HAS). The carbon layers were derived from different sources and uniformly coated on the porous surface of OMS. Combined with the characterization results of carbonized catalysts, it is demonstrated that the carbon layer-coated supports significantly enhanced the metal dispersion and increased the ratio of Co2+ to Co0 sites, which further increased the CO conversion and alcohols selectivity. Moreover, it is found that the catalytic activity changed in line with the amount of defects and surface oxygenic groups of carbon layers, which resulted from the different carbon sources. The highest space time yield of C2+OH was 27.5 mmol gcat-1 h-1) obtained by the catalyst coated with glucose-derived carbon layer. But the carbon source is not the key factor influencing the distribution of Co-Co2+ dual sites and shows little effect on selectivity in HAS. These results may guide for further design of carbon supported catalysts.
Cobalt sulfides as efficient catalyst towards oxygen reduction reactions
Shuo Yao, Taizhong Huang, Hengyi Fang, Jiemei Yu, Mayilvel Dinesh Meganathan, Zhaoxin Cui, Xianxia Yuan
2020, 31(2): 530-534  doi: 10.1016/j.cclet.2019.04.069
[摘要]  (194) [HTML全文] (194) [PDF 1028KB] (194)
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Developing low-cost and high performance catalysts to replace precious metal based catalysts for oxygen reduction reaction (ORR) is one of the most feasible ways to promote the commercial application of fuel cells. In this work, flower-like CoS and octahedral CoS2 are synthesized by a facile one-pot hydrothermal method without any adjunction of surfactants or follow-up thermolysis, their catalytic performance towards ORR in alkaline electrolyte are comparatively investigated. The results reveal that CoS2 outperforms CoS owing to the higher electron density around S-S bond of S22- in the crystal structure, which promotes the adsorption of oxygen on catalyst surface and facilitates the breakage of O-O bond in oxygen, leading to direct 4-electron transfer ORR. When CoS2 particles are dispersed on the surface of rGO with large surface area, their ORR performance could be further improved.
New ZnCe catalyst encapsulated in SBA-15 in the production of 1, 3-butadiene from ethanol
Yujun Zhao, Sijia Li, Zheng Wang, Shengnian Wang, Shengping Wang, Xinbin Ma
2020, 31(2): 535-538  doi: 10.1016/j.cclet.2019.04.038
[摘要]  (203) [HTML全文] (203) [PDF 797KB] (203)
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ZnO-CeO2/SBA-15 catalysts were prepared by two kinds of solid-state grinding method and used for the production of 1, 3-butadiene (1, 3-BD) from ethanol. A mixture of SBA-15 (with or without organic template) and metal precursors were ground in solid-state. The obtained catalysts were characterized by TG, N2 adsorption-desorption, TEM, XRD, Py-FTIR and NH3-TPD techniques. Superior dispersion of metal oxides and more exposed acid sites were achieved on the catalyst 10Zn1Ce5-AS with the presence of organic template in SBA-15 during the solid-state grinding process. The catalytic performance was evaluated in a fixed-bed reactor and a 1, 3-butadiene selectivity of as high as 45% is achieved. This is attributed to the coupling effect of Zn and Ce species in the mesopores of SBA-15, in which Zn promotes ethanol dehydrogenation and Ce enhances aldol-condensation, respectively. Additionally, solvent-free method inspires new catalyst synthesis strategy for the production of 1, 3-butadiene from ethanol.
A versatile β-cyclodextrin functionalized silver nanoparticle monolayer for capture of methyl orange from complex wastewater
Jun Liu, Cancan Zhang, Shaoxuan Zhang, Huajiang Yu, Wei Xie
2020, 31(2): 539-542  doi: 10.1016/j.cclet.2019.07.037
[摘要]  (200) [HTML全文] (200) [PDF 832KB] (200)
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The toxic organic dye contaminants in wastewater are extremely harmful to the ecosystem. Surface enhanced Raman scattering (SERS) is a technique with high sensitivity and chemical specificity which fulfills the requirements for monitoring dye contaminants in wastewater. However, as one of the common dye contaminants, methyl orange (MO) has very weak affinity to metallic surfaces and is difficult to be detected by SERS at low concentrations. Therefore, a new type of SERS substrate with Ag nanoparticle monolayer functionalized by mono-6-deoxy-6-thio-β-cyclodextrin (β-CD-SH) was prepared to efficiently capture and detect MO in wastewater with a limit of detection of 5×10-7 mol/L. The hydrophobic cavity of β-CD is responsible for the efficient trap and enrichment of MO on the Ag NPs surface, achieving a strong SERS signal of MO at low concentrations and at different pH values. This study provides new insight into designing a well-performed adsorbent for the capture and detection of organic contaminants.
The performance and degradation mechanism of sulfamethazine from wastewater using IFAS-MBR
Huanhuan Hou, Liang Duan, Beihai Zhou, Yuan Tian, Jian Wei, Feng Qian
2020, 31(2): 543-546  doi: 10.1016/j.cclet.2019.08.031
[摘要]  (186) [HTML全文] (186) [PDF 1091KB] (186)
摘要:
Sulfamethazine (SMZ) is an important sulfonamide antibiotic. Although the concentration in the environment is small, it is harmful. The drug residues can be transferred, transformed or accumulated, affecting the growth of animals and plants. In this study, the integrated fixed-film activated sludge membrane bioreactor (IFAS-MBR) were constructed to investigate the performance and degradation mechanism of SMZ. The addition of SMZ had a significant impact on the removal of the chemical oxygen demand (COD) and ammonia nitrogen (NH4+-N). The optimal operating conditions were hydraulic retention time (HRT) at 10 h and solid retention time (SRT) at 80 d, respectively. On this basis, the effects of different SMZ concentrations on nutrient removal, degradation, and sludge characteristics were compared. The removal efficiency of SMZ increased with the increase of SMZ concentration. The maximum removal rate was as high as 87%. The SMZ dosage also had an obvious effect on sludge characteristics. As the SMZ concentration increased, the extracellular polymer substances (EPS) concentration and the membrane resistance both decreased, which were beneficial for the reduction of membrane fouling. Finally, seven kinds of SMZ biodegradation intermediates were identified, and the possible degradation pathways were speculated. The microbial community results showed that the microbial diversity and richness in the reactor decreased after adding SMZ to the influent. The relative abundance of Bacteroidetes, Actinobacteria, Saccharibacteria and Nitrospirae increased at the phylum level. Sphingobacteria and Betaproteobacteria became dominant species at the class level. The relative abundance of norankp-Saccharibacteria and Nitrospirae increased significantly, and norank-p-Saccharibacteria may be the dominant bacteria for SMZ degradation.
All-solid-state BiVO4/ZnIn2S4 Z-scheme composite with efficient charge separations for improved visible light photocatalytic organics degradation
Deling Yuan, Mengting Sun, Shoufeng Tang, Yating Zhang, Zetao Wang, Jinbang Qi, Yandi Rao, Qingrui Zhang
2020, 31(2): 547-550  doi: 10.1016/j.cclet.2019.09.051
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摘要:
Constructing a Z-scheme is a significant approach to improve the separation of photogenerated carriers for effective organic pollutant degradation. Herein, a BiVO4/ZnIn2S4 (BZ) Z-scheme composite was successfully synthesized, and applied to photodegrade methyl orange (MO) irradiated by a LED lamp. Anchoring the BiVO4 on the ZnIn2S4 nanoparticles promoted the separation of photogenerated electronholes and broadened the light response range. The detailed characterizations, including surface morphology, elements valence state, and photocurrent performance, demonstrated that the enhanced separation of photogenerated carriers was the pivotal reason for the enhanced photocatalysis reaction. Benefiting from the excellent photocatalytic characteristics, the 5% mass ratio of BZ composite presented the highest MO degradation rate of 0.00997 min-1, which was 1.9 and 10.3 times greater than the virgin ZnIn2S4 and BiVO4, respectively. Furthermore, the BZ hybrid materials indicated a well photo-stability in the four recycling tests.
In-chain functionalization through the combination of ring opening copolymerization and oxime "Click" reaction towards X-ray opaque polylactide copolymers
Wenhuan Wang, Lin Sang, Weizong Kong, Yiping Zhao, Zhiyong Wei, Yang Li
2020, 31(2): 551-553  doi: 10.1016/j.cclet.2019.04.062
[摘要]  (216) [HTML全文] (216) [PDF 772KB] (216)
摘要:
X-ray imaging functionalization of biodegradable polyesters is a great demand and challenge in biomedical applications. In this work, a strategy of in-chain functionalization through the combination of ring opening copolymerization and oxime "Click" postfunctionalization was developed towards X-ray opaque polylactide copolymers. A functionalized cyclic carbonate was first synthesized and used as comonomer of polylactide copolymers, which were subjected to postfunctionalization of oxime "Click" reaction towards iodinated polylactide copolymers. The chemical structure and physical properties of the target products were traced and confirmed. In vitro cytotoxicity evaluation with 3T3-Swiss albino by Alamar blue demonstrated a low cytotoxicity. The X-ray radiopacity was analyzed by Micro-CT and quantified by Hounsfield Units value, which could be tailorable by the feedstock. It is a promising X-ray visible implantable biomaterial in biomedical applications.
Thermal studies of novel molecular perovskite energetic material (C6H14N2)[NH4(ClO4)3]
Jing Zhou, Li Ding, Fengqi Zhao, Bozhou Wang, Junlin Zhang
2020, 31(2): 554-558  doi: 10.1016/j.cclet.2019.05.008
[摘要]  (219) [HTML全文] (219) [PDF 839KB] (219)
摘要:
(C6H14N2)[NH4(ClO4)3] is a newly developed porous hybrid inorganic-organic framework material with easy access and excellent detonation performances, however, its thermal properties is still unclear and severely hampered further applications. In this study, thermal behaviors and non-isothermal decomposition reaction kinetics of (C6H14N2)[NH4(ClO4)3] were investigated systematically by the combination of differential scanning calorimetry (DSC) and simultaneous thermal analysis methods. In-situ FTIR spectroscopy technology was applied for investigation of the structure changes of (C6H14N2)[NH4(ClO4)3] and some selected referents for better understanding of interactions between different components during the heating process. Experiment results indicated that the novel molecular perovskite structure renders (C6H14N2)[NH4(ClO4)3] better thermal stability than most of currently used energetic materials. Under high temperatures, the stability of the cage skeleton constructed by NH4+ and ClO4- ionsdetermined the decomposition process rather than organic moiety confined in the skeleton. The simple synthetic method, good detonation performances and excellent thermal properties make (C6H14N2)[NH4(ClO4)3] an ideal candidate for the preparation of advanced explosives and propellants.
Synthesis of few-layer N-doped graphene from expandable graphite with melamine and its application in supercapacitors
Yunpeng Wu, Xiaoyang Liu, Dandan Xia, Qiushi Sun, Deyang Yu, Shuanggan Sun, Xilong Liu, Yifei Teng, Weige Zhang, Xudong Zhao
2020, 31(2): 559-564  doi: 10.1016/j.cclet.2019.04.055
[摘要]  (220) [HTML全文] (220) [PDF 916KB] (220)
摘要:
In this paper, we introduced a novel method to prepare the few-layer nitrogen-doped graphene (FNG) from expandable graphite with melamine. The super-capacitive properties of FNG were thoroughly characterized by a three-electrode system, and the results showed the FNG electrode achieved a specific capacitance as high as 83.8 mF/cm2 together with excellent cycling stability. This method could be a novel approach to combine the pseudo-capacitors and electric double layer capacitors.
Reversible chemical switches of functionalized nitrogen-doped graphene field-effect transistors
Rong Rong, Song Liu
2020, 31(2): 565-569  doi: 10.1016/j.cclet.2019.05.014
[摘要]  (207) [HTML全文] (207) [PDF 807KB] (207)
摘要:
Nitrogen doping is a promising way to modulate the electrical properties of graphene to realize graphene-based electronics and promise fascinating properties and applications. Herein, we report a method to noncovalently assembly titanium(Ⅳ) bis(ammoniumlactato) dihydroxide (Ti complex) on nitrogen-doped graphene to create a reliable hybrids which can be used as a reversible chemical induced switching. As the adsorption and desorption of Ti complex in sequential treatments, the conductance of the nitrogen-doped graphene transistors was finely modulated. Control experiments with pristine graphene clearly demonstrated the important effort of the nitrogen in this chemical sensor. Under optimized conditions, nitrogen-doped graphene transistors open up new ways to develop multifunctional devices with high sensitivity.
其它
Enzyme-loaded liposome with biocatalytic precipitation for potentiometric immunoassay of thyroid-stimulating hormone in thyroid carcinoma
Yongjin Cao, Min Zheng, Weihua Cai, Zongcai Wang
2020, 31(2): 463-467  doi: 10.1016/j.cclet.2019.06.024
[摘要]  (185) [HTML全文] (185) [PDF 879KB] (185)
摘要:
A simple and feasible potentiometric immunosensing platform based on enzymatic biocatalytic precipitation technique was designed for the sensitive detection of thyroid-stimulating hormone (TSH; a typical kind of biomarkers for thyroid carcinoma), using horseradish peroxidase (HRP)-loaded liposome for the signal amplification. To construct such an assay system, a sandwich-type immunoreaction was readily carried out on monoclonal anti-TSH capture antibody-coated electrode by using polyclonal antiTSH secondary antibody-conjugated HRP-loaded liposome. Accompanying the formation of sandwichtype immunocomplex, the carried liposome was lysed through the added Triton X-100 to release the entrapped HRP molecules, which catalyzed the oxidation of 4-chloro-1-naphthol to produce an insoluble and uncharged organic precipitation on the electrode surface, thereby causing the change of the local electrical potential. Two labeling protocols with and without the liposome were investigated for detection of target TSH, improved analytical features were achieved with HRP-entrapped liposome. Under optimal conditions, the potentiometric immunosensor had good responses for TSH detection within the linear range of 0.01-30 μIU/mL at a detection limit of 0.0067 μIU/mL. Good reproducibility, high specificity and long-time stability were acquired during the assay procedure. Importantly, a wellmatched accuracy between the potentiometric immunosensor and commercial human TSH ELISA kit was gave for the analysis of human serum samples.