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基于多酯头基的“油-二氧化碳两亲分子”设计及其助混规律
廖培龙, 刘泽宇, 刘卡尔顿, 马骋, ZhuZhiyang, 杨思玉, 吕文峰, 杨永智, 黄建滨
2020, 36(10): 1907034-0  doi: 10.3866/PKU.WHXB201907034
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摘要:
针对目前具有广泛应用的油相-超临界二氧化碳(scCO2)混合体系,我们提出了“油-CO2两亲分子”的概念,实验设计筛选出了一类以多酯头基作为亲CO2基团,长碳链作为亲油基团的油-CO2两亲分子。本工作以白油、煤油等为油相,以自主开发的可视化混相方法作为评价方式,以降低两相最低混相压力的助混效率为指标,系统研究了油-scCO2体系的助混规律。结果表明:(1)越多的酯基将提供越强的“亲CO2性”;(2)碳链长度为16的助混剂拥有最佳的助混效果;(3)与scCO2性质差异越大的油相,两亲分子的助混差异越明显,体现了油相种类带来的区分与拉平效应。本工作不仅将经典的水/油两亲分子概念扩展到油-scCO2两亲体系,对于实际生产中scCO2驱油也具有重要的指导意义。
环糊精与表面活性剂主客体作用诱导的金纳米棒可控自组装
肖军燕, 齐利民
2020, 36(10): 1910001-0  doi: 10.3866/PKU.WHXB201910001
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摘要:
纳米结构基元的可控自组装是自下而上构筑功能材料及纳米器件的有效途径。各向异性的金纳米棒具有独特的等离激元特性,而如何通过简单有效的方法实现其可控自组装仍具有较大的挑战性。本文利用环糊精(CD)与吸附于金纳米棒表面的十六烷基三甲基溴化铵(CTAB)的主客体作用,实现了金纳米棒(GNR)在水溶液中的可控自组装。通过调节α-CD的浓度可以分别实现金纳米棒肩并肩组装或头对头组装,初步揭示α-CD与CTAB的超分子作用是金纳米棒组装的主要诱因。根据实验结果推测α-CD诱导金纳米棒组装的机理如下:在α-CD浓度较低时,GNR表面的CTAB吸附层部分被α-CD/CTAB超分子复合物取代,从而发生缓慢的肩并肩组装;在α-CD浓度较高时,GNR表面的CTAB吸附层大量被α-CD/CTAB复合物取代,并且GNR两端的CTAB几乎完全被取代,因而发生快速的头对头组装。借助于α-淀粉酶对α-CD的水解作用,可以利用该组装体系实现对溶液中微量淀粉酶的检测。这种基于主客体作用的自组装策略为非球形纳米基元的可控自组装提供了新的思路。
基于两亲性喹喔啉的超分子凝胶:手性信号反转以及多重响应手性光学开关
汪含笑, 徐俪菲, 刘鸣华
2020, 36(10): 1910036-0  doi: 10.3866/PKU.WHXB201910036
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摘要:
文设计将具有良好光学性质的喹喔啉衍生物引入L-谷氨酸基两亲分子中,得到包含较大π-共轭头基的手性功能化凝胶因子SQLG。借由多重分子间非共价相互作用的驱动,SQLG可以自组装为由纳米纤维组成的三维网络,胶凝极性从低到高的多种有机溶剂。在自组装的过程中,中心手性通过分子的不对称排列传递到超分子层面,进而在圆二色(CD)和圆偏振发光(CPL)光谱上表现出超分子手性信号。SQLG在极性溶剂和非极性溶剂中组装时采取不同的堆积模式,使两类溶剂体系中形成的组装体表现出相反的手性信号。由于喹喔啉上具有质子接受位点,对超分子凝胶进行酸化后,分子内电荷转移作用(ICT)受到明显强化,并且自组装驱动力发生改变,导致黄色凝胶坍塌为红色分散液,同时堆积模式的改变导致超分子手性信号反转,CPL信号则随着荧光猝灭而关闭,而碱的中和作用可以使体系的一系列性质变化得到恢复。因此,通过向手性两亲分子中引入酸响应性π-共轭体系,我们顺利构筑了一例具有多重外界刺激响应性的超分子手性光学开关。
综述
薄膜基荧光气体传感器中的涂层化学
刘太宏, 苗荣, 彭浩南, 刘静, 丁立平, 房喻
2020, 36(10): 1908025-0  doi: 10.3866/PKU.WHXB201908025
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摘要:
近年来,高性能薄膜基气体传感器的研制备受关注,所涉及的涂层化学已经成为物理化学学科发展的一个热点。传感因分析物与敏感层(涂层)物质相互作用引起薄膜特定静态及动态物理量变化而实现,因此,薄膜传感性能势必受到敏感层物质种类和敏感层微纳结构等因素影响。就薄膜基荧光传感而言,荧光敏感物质的结构和性质对薄膜传感性能起着至关重要的作用。同时,因毛细凝结、色谱效应、尺寸效应、分子间相互作用等因素的存在,敏感层微观结构也极大地影响着薄膜的传感性能。本文结合课题组近期研究工作,简要讨论薄膜基荧光气体传感器研究中的涂层化学基本问题,以及相关薄膜基荧光传感器在隐藏爆炸物、毒品、挥发性有机污染物检测/监测等方面的应用探索。最后,文章展望了薄膜基荧光气体传感器的发展前景和所面临的主要挑战。
肽基超分子胶体
邢蕊蕊, 邹千里, 闫学海
2020, 36(10): 1909048-0  doi: 10.3866/PKU.WHXB201909048
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摘要:
肽基超分子胶体是基于肽分子间超分子作用,自发形成且具有有序分子排布及规整结构,兼具传统胶体及超分子特性的组装体系。利用超分子弱相互作用构筑功能性胶体,不仅是人们对生命组装进程深入理解的有效手段,也是实现优异的超分子材料的重要途径。肽分子具有组成明确、性能可调、生物安全性高及可降解等优势,是超分子化学、胶体与界面化学领域重要的组装基元。基于肽的超分子自组装,能够实现多尺度、多功能的生物胶体的构筑,被广泛应用于医药、催化、能源等领域。如何通过对肽序列的设计及分子间作用力的调控,实现对胶体结构和功能的精确控制,是近年来研究的重要课题之一。从分子尺度研究和揭示超分子胶体的组装过程及物理化学机制,探究胶体结构与功能的关系,是实现超分子结构和功能化的重要内容。本文基于“分子间作用的调控”及“结构与功能的关系”两个基本科学问题,系统地综述了肽基超分子胶体的组装机制、结构与功能,以及研究现状。
Article
Aggregation of Biodegradable Cationic Gemini Surfactants with Amide or Ester Groups
Yingxiong Wang, Manli Deng, Yongqiang Tang, Yuchun Han, Xu Huang, Yanbo Hou, Yilin Wang
2020, 36(10): 1909046-0  doi: 10.3866/PKU.WHXB201909046
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摘要:
In the last thirty years, Gemini surfactants with various structures have been designed, synthesized, and demonstrated to show superior physicochemical properties. However, the utilization of non-degradable surfactants, including these Gemini surfactants, poses a threat to the environment; hence, degradable Gemini surfactants are desirable. Herein, biodegradable cationic Gemini surfactants with amide or ester groups in the hydrophobic chains or the spacer were synthesized. A monomeric surfactant containing an amide group and a Gemini surfactant with amide groups both in the hydrophobic chains and the spacer were synthesized for comparison. The effects of amide group location on the aggregation behavior of Gemini surfactants were studied systematically. The differences between the Gemini surfactants with amide groups and Gemini surfactants with ester groups were evaluated by comparing their aggregation behavior and hydrogen bonding formation. The Gemini surfactants with amide groups (C12A-Cn-AC12) in the chains showed much larger exothermic ΔHmic and more negative ΔGmic values than those of the corresponding monomeric surfactant C12A; besides, their critical micelle concentration (cmc) was more than one order of magnitude lower than that of C12A. The amide groups located in the hydrophobic alkyl chains promoted hydrogen bonding formation and self-assembly of the Gemini surfactants C12A-Cn-AC12. Moreover, 1H NMR spectra revealed that the co-effect of a short spacer and hydrogen bonding leads to slow exchange of the C12A-C2-AC12 molecules between the monomer and the aggregate. For the Gemini surfactant series C12-ACnA-C12, the amide groups notably increased the spacer length, and largest cmc value and smallest exothermic ΔHmic value were observed for C12-AC2A-C12 instead of C12-AC6A-C12. In C12-AC12A-C12, the spacer was long and sufficiently flexible to adopt a "U"-shaped conformation above the cmc, and it acted as the hydrophobic part of the surfactant, as confirmed by 1H NMR spectra. Among the Gemini surfactant with amide groups in both the spacer and the hydrophobic alkyl chains, C12A-AC6A-AC12 had a smaller cmc and I1/I3 ratio as well as more exothermic ΔHmic values than those of C12A-C6-AC12 and C12-AC6A-C12. 1H NMR spectra indicated that an ester-alcohol structural equilibrium exists during aggregation for the Gemini surfactants with ester groups. In addition, the Gemini surfactants with ester groups formed water-mediated hydrogen bonds in the aggregates. This water-mediated hydrogen bonding between ester groups was weaker than the direct hydrogen bonding between amide groups. Therefore, the Gemini surfactants with ester groups, C12E-C6-EC12 and C12-EC6E-C12, exhibited lower surface activity, a larger micelle ionization degree, higher micropolarity, and smaller exothermic ΔHmic and less negative ΔGmic values than their counterparts with amide groups, C12A-C6-AC12 and C12-AC6A-C12.
Wormlike Micelle to Gel Transition Induced by Brij 30 in Ionic Liquid-Type Surfactant Aqueous Solution
Yimin Hu, Jie Han, Rong Guo
2020, 36(10): 1909049-0  doi: 10.3866/PKU.WHXB201909049
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Wormlike micelles and low-molecular-weight hydrogels are composed of three-dimensional networks that endow them with viscoelasticity, but their viscoelastic properties are markedly different. The viscosity of wormlike micelles is attributed to a transient network, while that of gels is due to a stable network. Under certain conditions, wormlike micelles can undergo transition to gels with an increase in the density of the network. In our previous study, we found that the wormlike micelle formed by the ionic liquid-type surfactant 1-hexadecyl-3-octyl imidazolium bromide ([C16imC8]Br) without any additive has high viscoelasticity. The inclusion of a nonionic surfactant polyoxyethylene lauryl ether (Brij 30) is expected to enhance the viscoelasticity of [C16imC8]Br wormlike micelles via electrostatic shielding and strong hydrophobic interactions, which may be the driving factor for the wormlike micelle-to-gel structural transition. The morphology and viscoelasticity of [C16imC8]Br wormlike micelles with Brij 30 were studied as a function of concentration by rheological measurements and freeze-fracture transmission electron microscopy. The thermal stability and gel-sol transition temperature of the Brij 30/[C16imC8]Br gels were studied using rheology. The interaction between Brij 30 and [C16imC8]Br was studied by zeta potential measurements and nuclear magnetic resonance (NMR) spectroscopy. Upon the inclusion of Brij 30 into the [C16imC8]Br wormlike micelles, the viscoelasticity of the Brij 30/[C16imC8]Br samples first increased and then decreased with an increase in the Brij 30 concentration, at different initial concentrations of [C16imC8]Br. At a certain Brij 30 concentration, the Brij 30/[C16imC8]Br samples rheologically behaved as a gel. The maximum viscoelasticity of the [C16imC8]Br (4.06% (w))/Brij 30 gel was observed at a Brij 30/[C16imC8]Br molar ratio of 4.55. The viscoelasticity of the Brij 30/[C16imC8]Br gels was positively correlated with the activation energy of the gels. The gel-sol transition temperature of the Brij 30/[C16imC8]Br gels also increased first and then decreased with an increase in the Brij 30 concentration. The highest gel-sol transition temperature of the Brij 30/[C16imC8]Br (4.06% (w)) gel was observed at a Brij 30/[C16imC8]Br molar ratio of 2.93. The Brij 30 concentration had a notable impact on the viscoelasticity, thermal stability, and gel-sol transition temperature of the Brij 30/[C16imC8]Br gels. The zeta potential and 1H NMR measurements revealed that the neutral Brij 30 molecules are inserted into the palisade layer of the [C16imC8]Br wormlike micelles via hydrophobic interactions. This decreased the electrostatic repulsion between the [C16imC8]Br headgroups, which in turn induced the rapid growth of wormlike micelles and the formation of a stiffer network structure. Finally, the wormlike micelles underwent a structural transition to gels. The obtained results would aid in better understanding the relationship between wormlike micelles and gels, and may be of potential value for industrial and technological applications.
Structure–Property Relationship of Light-Responsive Wormlike Micelles Using Methoxycinnamate Derivatives as Light-Switchable Molecules
Tongqing Liu, Fangfang Xue, Ping Yi, Zhiyu Xia, Jinfeng Dong, Xuefeng Li
2020, 36(10): 1910004-0  doi: 10.3866/PKU.WHXB201910004
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摘要:
In this work, light-responsive viscoelastic wormlike micelles based on cetyltrimethylammonium hydroxide (CTAOH) and cinnamic acid derivatives, including cinnamic acid (CA), 2-methoxycinnamic acid (2-MCA), 3-methoxycinnamic acid (3-MCA), 4-methoxycinnamic acid (4-MCA), 2, 3-dimethoxycinnamic acid (2, 3-DMCA), 2, 4-dimethoxycinnamic acid (2, 4-DMCA), 2, 3, 4-trimethoxycinnamic acid (2, 3, 4-DMCA), and 3, 4, 5-trimethoxycinnamic acid (3, 4, 5-DMCA), were prepared. The effects of the CA derivative structures, especially the position and number of methoxy moieties, on the formation of wormlike micelles were systematically determined. The CA derivatives facilitated the formation of long and entangled wormlike micelles. 1H NMR results showed that the CA derivatives participated in the formation of wormlike micelles via insertion of the aromatic moieties into the aggregates. The number of methoxy moieties had a much stronger effect on the viscosity of the wormlike micelle solution than the position of this moiety. The larger the number of methoxy moiety, the smaller was the aggregate. Substituted methoxy moieties increased the steric hindrance between the surfactants and CA molecules, thus hindering the formation of large aggregates. However, the position of the methoxy moiety had a predominant effect on the UV-light-induced transition of the wormlike micelles. Specifically, the ortho-methoxy moiety in the CA molecules dramatically enhanced the efficiency of UV-light-induced trans-cis isomerization. For example, the 2-MCA/CTAOH, 3-MCA/CTAOH, and 4-MCA/CTAOH binary systems (90 mmol·L-1/100 mmol·L-1) were gel-like with similar viscosities of around 20 Pa·s, but after UV light irradiation, they were transformed into a fluid with lower viscosity because of the formation of smaller aggregates. However, the irradiation time required for the transition varied significantly, as suggested by the results of viscosity measurements and UV-Vis spectroscopy. The 2-MCA/CTAOH system underwent complete phase transition within 3 h, whereas continuous transitions were observed for the 3-MCA/CTAOH and 4-MCA/CTAOH systems upon irradiation for 24 h. 1H NMR results suggested that the change in the configuration of MCA in the micelles before and after irradiation was the major cause of the abovementioned difference in the phase transition pattern. Initially, all the aromatic moieties of the trans-2-MCA molecules were deeply inserted into the hydrophobic cores of the micelles in a vertical manner, and the ionized carboxyl moiety was located in the palisade layer because of the electrostatic interactions between CTAOH and trans-2-MCA. In contrast, cis-2-MCA was inserted into the micelles in a horizontal manner, and some of the protons in the aromatic moiety were also transferred from the micellar core to the polar palisade layer. Accordingly, the CTAOH and cis-2-MCA molecules were packed loosely in the aggregates, thereby resulting in the formation of spherical micelles. Similar UV-light-induced transitions were observed for the 3-MCA/CTAOH and 4-MCA/CTAOH systems.
Solvent-Induced Inversion of Pickering Emulsions for In Situ Recycling of Enzyme Biocatalysts
Houbing Zou, Rammile Ettelaie, Shuai Yan, Nan Xue, Hengquan Yang
2020, 36(10): 1910006-0  doi: 10.3866/PKU.WHXB201910006
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Separation and recycling of catalysts are crucial for realizing the objectives of sustainable and green chemistry but remain a great challenge, especially for enzyme biocatalysts. In this work, we report a new solvent-induced reversible inversion of Pickering emulsions stabilized by Janus mesosilica nanosheets (JMSNs), which is then utilized as a strategy for the in situ separation and recycling of enzymes. The interfacial active solid particle JMSNs is carefully characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), nitrogen sorption experiments, Fourier transform infrared (FT-IR) spectroscopy, and thermogravimetric analysis (TGA).The JMSNs are demonstrated to show order-oriented mesochannels with a large specific surface area, and the hydrophobic octylgroup is selectively modified on one side of the nanosheets. Furthermore, the inversion is found to be a fast process that is strongly dependent on the interfacial activity of the solid emulsifier JMSNs. Such a phase inversion is also a general process that can be realized in various oil/water phasic systems, including ethyl acetate-water, octane-water, and cyclohexane-water systems. By carefully analyzing the capacity of JMSNs with different surface wettabilities for phase inversion, a triphase contact angle (θ) close to 90° and a critical oil-water ratio of 1 : 2 are identified as the key factors to achieve solvent-induced phase inversion via a catastrophic phase inversion mechanism. Importantly, this reversible phase inversion is suitable for the separation and recycling of enzyme biocatalysts that are sensitive to changes in the reaction medium. Specifically, during the reaction, the organic substrates are dissolved in the oil droplets and the water-soluble catalysts are dispersed in the water phase, while a majority of the product is released into the upper oil phase and the enzyme catalyst is confined inside the water droplets in the bottom layer after phase inversion. The perpendicular mesochannels of JMSNs provide a highly accessible reaction interface, and their excellent interfacial activity allows for more than 10 rounds of consecutive phase inversions by simply adjusting the ratio of oil to water in the system. Using the enzymatic hydrolysis kinetic resolution of racemic acetate as an example, our Pickering emulsion system shows not only a 3-fold enhanced activity but also excellent recyclability. Because no sensitive chemical reagents are used in this phase inversion process, the intrinsic activities of the catalysts can be preserved even after seven cycles. The current study provides an alternative strategy for the separation and recycling of enzymes, in addition to revealing a new innovative application for Janus-type nanoparticles.
Review
Probing Molecular Structures of Antifouling Polymer/Liquid Interfaces In Situ
Chengcheng Zhang, Ralph Crisci, Zhan Chen
2020, 36(10): 1910003-0  doi: 10.3866/PKU.WHXB201910003
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摘要:
Marine organisms such as plants, algae or small animals can adhere to surfaces of materials that are submerged in ocean. The accumulation of these organisms on surfaces is a marine biofouling process that has considerable adverse effects. Marine biofouling on ship hulls can cause severe fuel consumption increase. Investigations on antifouling polymers are therefore becoming important research topics for marine vessel operations. Antifouling polymers can be applied as coating layers on the ship hull, protecting it against the settlement and growth of sea organisms. Polyethylene glycol (PEG) is a hydrophilic polymer that can effectively resist the accumulation of marine organisms. PEG-based antifouling coatings have therefore been extensively researched and developed. However, the inferior stability of PEG makes it subject to degradation, rendering it ineffective for long-term services. Zwitterionic polymers have also emerged as promising antifouling materials in recent years. These polymers consist of both positively charged and negatively charged functional groups. Various zwitterionic polymers have been demonstrated to exhibit exceptional antifouling properties. Previously, surface characterizations of zwitterionic polymers have revealed that strong surface hydration is critical for their antifouling properties. In addition to these hydrophilic polymers, amphiphilic materials have also been developed as potential antifouling coatings. Both hydrophobic and hydrophilic functional groups are incorporated into the backbones or sidechains of these polymers. It has been demonstrated that the antifouling performance can be enhanced by precisely controlling the sequence of the hydrophobic-hydrophilic functionalities. Since biofouling generally occurs at the outer surface of the coatings, the antifouling properties of these coatings are closely related to their surface characteristics in water. Therefore, understanding of the surface molecular structures of antifouling materials is imperative for their future developments. In this review, we will summarize our recent advancements of antifouling material surface analysis using sum frequency generation (SFG) vibrational spectroscopy. SFG is a surface-sensitive technique which can provide molecular information of water and polymer structures at interfaces in situ in real time. The antifouling polymers we will review include zwitterionic polymer brushes, mixed charged polymers, and amphiphilic polypeptoids. Interfacial hydration studies of these polymers by SFG will be presented. The salt effect on antifouling polymer surface hydration will also be discussed. In addition, the interactions between antifouling materials and protein molecules as well as algae will be reviewed. The above research clearly established strong correlations between strong surface hydration and good antifouling properties. It also demonstrated that SFG is a powerful technique to provide molecular level understanding of polymer antifouling mechanisms.
Particle-Stabilized Interfaces and Their Interactions at Interfaces
Guanqing Sun, Zonglin Yi, To Ngai
2020, 36(10): 1910005-0  doi: 10.3866/PKU.WHXB201910005
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Particle-stabilized dispersions such as emulsions, foams and bubbles are catching increasing attentions across a number of research areas. The adsorption mechanism and role of these colloidal particles in stabilizing the oil-water or gas-water interfaces and how these particles interact at interfaces are vital to the practical use of these dispersion systems. Although there have been intensive investigations, problems associated with the stabilization mechanisms and particle-particle interactions at interfaces still remain to explore. In this paper, we first systematically review the historical understanding of particle-stabilized emulsions or bubbles and then give an overview of the most important and well-established progress in the understanding of particle-stabilized systems, including emulsions, foams and liquid marbles. The particle-adsorption phenomena have long been realized and been discussed in academic paper for more than one century and a quantitative model was proposed in the early 1980s. The theory can successfully explain the adsorption of solid particles onto interface from energy reduction approaches. The stability of emulsions and foams can be readily correlated to the wettability of the particles towards the two phases. And extensive researches on emulsion stability and various strategies have been developed to prepared dispersion systems with a certain trigger such as pH and temperature. After that, we discuss recent development of the interactions between particles when they are trapped at the interface and highlight open questions in this field. There exists a huge gap between theoretical approaches and experimental results on the interactions of particles adsorbed at interfaces due to demanding experimental devices and skills. In practice, it is customary to use flat surfaces/interfaces as model surfaces to investigate the particle-particle at interfaces although most of the time interfaces are produced with a certain curvature. It is shown that the introduction of particles onto interfaces can generate charges at the interfaces which could possibly account for the long range electrostatic interactions. Finally, we illustrate that particle-stabilized dispersions have been found wide applications in many fields and applications such as microcapsules, food, biomedical carriers, and dry water. One of the most investigated areas is the microencapsulation of actives based on Pickering emulsion templates. The particles adsorbed at the interface can serve as interfacial stabilizers as well as constituting components of shells of colloidal microcapsules. Emulsions stabilized by solid particles derived from natural and bio-related sources are promising platforms to be applied in food related industries. Emulsion systems stabilized by solid particles of the w/w (water-in-water) feature are discussed. This special type of emulsion is attracting increasing attentions due to their all water features. Besides of oil-water interface, particle stabilized air-water interface share similar stabilization mechanism and several applications reported in the literature are subsequently discussed. We hope that this paper can encourage more scientists to engage in the studies of particle-stabilized interfaces and more novel applications can be proposed based on this mechanism
Liquid Marbles: Fabrication, Physical Properties, and Applications
Xinjie Luo, Xi Zhang, Yujun Feng
2020, 36(10): 1910007-0  doi: 10.3866/PKU.WHXB201910007
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摘要:
Liquid marbles (LMs) are liquid droplets coated with a layer of lyophobic particles at the air-liquid interface. Since the pioneering work by Aussillous et al. in 2001, LMs have attracted significant attention owing to their facile fabrication, flexibility in the choice of the constituent particles and liquids, intriguing properties such as non-wetting and non-adhesive nature, satisfactory elasticity and stability, as well as promising applications in microfluidics, sensors, controlled release, and microreactors. The classical strategy for the preparation of LMs involves rolling a small volume of a droplet on a lyophobic powder bed for complete encapsulation of the liquid by the particles. In addition, various innovative methods, including electrostatic and coalescent approaches, have been developed for preparing special LMs with a complicated structure or morphology. Diverse materials such as water, surfactant solutions, liquid metals, reagents, blood, and even viscous adhesives have been employed as the internal liquid for the fabrication of LMs. Theoretically, any particulates such as lycopodium, polytetrafluoroethylene, Fe3O4, SiO2, and graphite grains can be employed as the outer coating, but they are usually required to be lyophobic with sizes of less than hundreds of microns. The unique structure of the particle-covered droplet and the dual solid-liquid characteristics endow LMs with some unique and interesting properties, especially the non-wetting and non-adhesive nature. As the lyophobic coating particles restrain the internal liquid from contacting the substrate, LMs can move easily across either solid or liquid surfaces, neither wetting the substrate nor contaminating the internal liquid. An equally fascinating property of LMs is their satisfactory stability, which is necessary for most of their applications. The high stability of LMs stems from the protection of the coating powders and is embodied in both good mechanical stability (remaining intact after being released from a certain height or under a certain compression) and long lifetime (greatly suppressing the evaporation of the internal liquid). These extraordinary properties make LMs promising candidates for use in multitudinous fields, especially droplet microfluidics and microreactors. The potential application of LMs in microfluidics is ascribed to their non-wetting, non-adhesive nature and other features such as an ability to float on a liquid surface, coalescence, split, a small force of rolling friction, and response to external forces. Notably, LMs hold great promise for applications in microreactions, because they can create a confined reaction microenvironment, minimize reagent usage, facilitate unhindered gas exchange between the internal liquid medium and the surrounding environment, and allow the entry/exit of the reactants/products. We herein review the recent advances in LMs, such as manufacturing techniques, formation mechanisms, physical properties, and emerging applications. In particular, much attention is paid to the factors affecting the stability of LMs and the potential strategies to increase their stability. Moreover, this review discusses the challenges in the future development of LMs, suggests several possible ways of addressing these challenges, and forecasts the future development directions. We believe that this review can help researchers gain a better understanding of LMs and promote their further advances.
亮点
结晶水调控聚集诱导发光
唐本忠
2020, 36(10): 2001037-0  doi: 10.3866/PKU.WHXB202001037
[摘要]  (73) [HTML全文] (73) [PDF 290KB] (4)
摘要:
Gemini和寡聚阳离子表面活性剂的高效抗菌活性
刘鸣华
2020, 36(10): 2003073-0  doi: 10.3866/PKU.WHXB202003073
[摘要]  (80) [HTML全文] (80) [PDF 622KB] (6)
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液-液相分离:超分子聚合物成核-生长的启动子
张希
2020, 36(10): 2004004-0  doi: 10.3866/PKU.WHXB202004004
[摘要]  (82) [HTML全文] (82) [PDF 286KB] (1)
摘要:
软颗粒在液-液界面吸附及界面催化
杨恒权
2020, 36(10): 2004021-0  doi: 10.3866/PKU.WHXB202004021
[摘要]  (73) [HTML全文] (73) [PDF 357KB] (3)
摘要:
手性导电高分子纳米结构的无手性构筑及手性分离应用
刘鸣华
2020, 36(10): 2004031-0  doi: 10.3866/PKU.WHXB202004031
[摘要]  (76) [HTML全文] (76) [PDF 318KB] (3)
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前言
胶体与界面化学
郝京诚
2020, 36(10): 2004078-0  doi: 10.3866/PKU.WHXB202004078
[摘要]  (80) [HTML全文] (80) [PDF 314KB] (2)
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专访
胶体与界面化学研究进展——郝京诚教授及其团队专访
《物理化学学报》编辑部
2020, 36(10): 2005053-0  doi: 10.3866/PKU.WHXB202005053
[摘要]  (81) [HTML全文] (81) [PDF 277KB] (3)
摘要:

论文
空气下光诱导有机金属卤化钙钛矿薄膜的降解机理
葛杨, 牟许霖, 卢岳, 隋曼龄
2020, 36(8): 1905039-0  doi: 10.3866/PKU.WHXB201905039
[摘要]  (123) [HTML全文] (123) [PDF 3280KB] (123)
摘要:
近几年来钙钛矿材料作为新兴光伏材料取得了巨大的发展进步,但有机无机杂化钙钛矿较差的环境稳定性限制了它的大规模应用。因此深入研究钙钛矿材料的降解机制有助于开发更稳定的钙钛矿光伏器件。本文基于透射电子显微学的微观形貌观察、晶体结构及元素成分表征,详细研究了杂化钙钛矿CH3NH3PbI3薄膜在光照以及空气共同作用下的降解机理。研究发现,光诱导下CH3NH3PbI3薄膜会与空气中的氧气发生交互作用,同时生成六方晶态PbI2甚至氧化为非晶态化合物PbI2−2xOx (0.4 < x < 0.6),而其衰减位点主要存在于薄膜与空气接触的表面。降解过程中,由于存在着挥发性分解产物(I2,CH3NH2)的大量丢失,薄膜的表面会产生许多小孔洞,继而形成一种蜂窝状的介孔衰竭通道。而这种衰竭方式主要与光照下钙钛矿中光生电子与氧气结合形成超氧根自由基(O2•−)有关,该基团诱导了CH3NH3PbI3向PbI2和非晶氧化态的转变。本文揭示了空气中光照诱导钙钛矿薄膜的降解机理,这将为未来设计和优化更稳定的钙钛矿太阳能电池提供全面的实验数据与理论支持。
多孔双金属氧化物/碳复合光催化剂对四环素的高效光催化降解
王艺蒙, 张申平, 葛宇, 王臣辉, 胡军, 刘洪来
2020, 36(8): 1905083-0  doi: 10.3866/PKU.WHXB201905083
[摘要]  (115) [HTML全文] (115) [PDF 4342KB] (115)
摘要:
本工作以金属有机框架材料UiO-67为载体,通过原位水解负载TiO2,经焙烧后得到系列ZrxTi/C光催化剂。我们以四环素为典型抗生素在300 W氙灯光源下进行光降解研究,Zr0.3Ti/C复合催化剂表现出优异的光催化效率,对于10 mg·L-1四环素溶液,30 min可以降解98%。光降解速率常数分别是TiO2、纯UiO-67焙烧产物Zr-O-C的16倍和3.7倍。这得益于Zr0.3Ti/C较大的比表面积,对四环素具有优异的吸附性能;同时具有能级匹配的Zr-O-C/TiO2异质结构和高导电性碳材料共掺,有效提高了电子-空穴对的分离与迁移;机理研究表明光照下产生的超氧自由基(O2•-)、羟基自由基(•OH)以及少量的空穴(h+),共同促进了光催化降解四环素。本研究基于吸附和光催化协同作用原理,所提出的高比表面积、双金属活性的复合光催化材料的制备方法,对抗生素等环境污染物光降解治理方面有一定的指导作用。
温度对乙醇电催化氧化的影响
涂昆芳, 李广, 姜艳霞
2020, 36(8): 1906026-0  doi: 10.3866/PKU.WHXB201906026
[摘要]  (107) [HTML全文] (107) [PDF 2526KB] (107)
摘要:
升高温度可以提高反应速率和增加物质的输运,因此通过不同温度下反应机理的研究可以深入理解电催化过程,对催化剂的设计具有指导意义。本工作初步建立了变温原位红外测定方法。采用温控电极,用电势测温法进行温度的校准,实验得出控温仪器加热温度Th与电极表面温度TS的关系为TS = 0.57Th + 7.71 (30 ℃ < Th≤ 50 ℃);TS = 0.62Th + 5.12 (50 ℃ < Th ≤ 80 ℃),误差分析最大温差为1 ℃。利用该方法我们研究了商业Pt/C催化剂在不同温度下乙醇的电氧化过程。从循环伏安图可以明显看到随着温度的升高整体氧化电流增大,起始电位、峰电位均负移,说明热活化使得氧化反应更容易进行;第一个峰电流与第二个峰电流的比值用于定性评估CO2的选择性,对比25 ℃,商业Pt/C催化剂在65 ℃下第一峰提高30%,说明高温有利于C―C键的断裂。对比25 ℃的原位红外谱图,我们发现35 ℃及50 ℃下商业Pt/C催化剂上CO2产物的起始电位负移200 mV,说明高温下,Pt/C催化剂能在更低的电位提供含氧物种;而CH3CHO、CH3COOH起始电位不随温度变化。用CO2与CH3COOH的积分面积比来评估CO2选择性,发现高温低电位其选择性最高,说明高温低电位有利于乙醇完全氧化生成CO2,而高温高电位下表面吸附含氧物种占据了活性位,阻碍C―C键断裂。
单原子分散的Au/Cu(111)表面合金的表面结构与吸附性质
王文元, 张杰夫, 李喆, 邵翔
2020, 36(8): 1911035-0  doi: 10.3866/PKU.WHXB201911035
[摘要]  (117) [HTML全文] (117) [PDF 3321KB] (117)
摘要:
Au-Cu双金属合金纳米颗粒对包括CO氧化和CO2还原等在内的多个反应有较好的催化活性,然而关于其表面性质的研究却相当匮乏。在此工作中,我们通过对低覆盖度的Au/Cu(111)和Cu/Au(111)双金属薄膜退火,制备出了单原子级分散的Au/Cu(111)和Cu/Au(111)合金化表面,并利用高分辨扫描隧道显微镜(STM)和扫描隧道谱(STS)进一步研究了掺杂原子的电子性质及其对CO吸附行为的影响。研究发现,分散在Cu(111)表面的表层和次表层Au单原子在STM上表现出不同衬度。在−0.5 eV附近,前者表现出相较于Cu(111)明显增强的电子态密度,而后者则明显减弱。吸附实验表明表层Au单原子对CO的吸附能力并没有得到增强,甚至会减弱其周围Cu原子的吸附能力。与Au在Cu(111)表面较好的分散相反,Cu原子倾向于钻入Au(111)的次表层,并且形成多原子聚集体。且Cu原子受Au(111)衬底吸电子作用的影响,其对CO的吸附能力明显减弱。这个研究结果揭示了合金表面的微观结构与性质的关联,为进一步阐明Au-Cu双金属催化剂的表面反应机理提供参考。
Article
Catalytic Oxidation of Toluene Over Potassium Modified Mn/Ce0.65Zr0.35O2 Catalyst
Xiaoxiao Lai, Jie Feng, Xiaoying Zhou, Zhongyan Hou, Tao Lin, Yaoqiang Chen
2020, 36(8): 1905047-0  doi: 10.3866/PKU.WHXB201905047
[摘要]  (114) [HTML全文] (114) [PDF 1141KB] (114)
摘要:
Volatile organic compounds (VOCs) are both harmful to human health and the environment; however, catalytic combustion offers a promising method for VOC purification because of its high efficiency without secondary pollution. Although manganese-based catalysts have been well studied for VOC catalytic oxidation, their catalytic activity at low temperature must be improved. Alkali metals as promoters have the potential to modulate the electronic and structural properties of the catalysts, improving their catalytic activity. Herein, a Ce0.65Zr0.35O2 support was prepared by co-precipitation and MnOx/Ce0.65Zr0.35O2 catalysts were obtained through the incipient-wetness impregnation method. The catalytic properties of K-modified MnOx/Ce0.65Zr0.35O2 for toluene oxidation with different molar ratios of K/Mn were investigated. In addition, the catalysts were characterized by XRD, UV/visible Raman, Hydrogen temperature program reduction (H2-TPR), Oxygen temperature programmed desorption (O2-TPD), X-ray photoelectron spectroscopy (XPS) and in situ diffuse reflectance FTIR spectroscopy (DRIFTS) experiments. The results showed that alkali metal doping with K significantly improved the catalytic activity. In particular, when the molar ratio of K/Mn was 0.2, the monolith catalyst Mn/Ce0.65Zr0.35O2-K-0.2 exhibited the best performance with the lowest complete conversion temperature T90 of 242 ℃ at a GHSV of 12000 h−1. The XRD results suggested that MnOx was uniformly distributed on the surface of the catalyst and that Mn4+ partially reduced to Mn3+ on the addition of K. The Raman spectrum demonstrated that with increasing K content, both the β- and α-MnO2 phases coexisted on the Mn/Ce0.65Zr0.35O2-K-0.2 catalyst, increasing the number of surface defect sites. The H2-TPR experiment results confirmed that Mn/Ce0.65Zr0.35O2-K-0.2 exhibited the lowest reduction temperature and good reducibility. From the O2-TPD experiments, it was clear that Mn/Ce0.65Zr0.35O2-K-0.2 contained the most surface adsorbed oxygen species and excellent lattice oxygen mobility, which benefitted the toluene oxidation activity. In addition, the XPS results suggested that the content of surface adsorbed oxygen species of the Mn/Ce0.65Zr0.35O2-K-0.2 catalyst was the highest among all the tested samples. In addition, toluene-TPSR in N2 as measured by in situ DRIFTs analysis demonstrated that available lattice oxygen was present in the Mn/Ce0.65Zr0.35O2-K-0.2 catalyst. Therefore, the Mn/Ce0.65Zr0.35O2-K-0.2 catalyst exhibited the best redox properties and oxygen mobility of the prepared samples and showed excellent activity toward toluene oxidation. Therefore, it was concluded that the addition of an appropriate amount of K improved the redox performance of the catalyst and increased the number of surface defect sites and mobility of the lattice oxygen of the catalyst as well as the concentration of the surface active oxygen species, thereby significantly improving catalytic ability.
Preparation and Characterization of Pt@Au/Al2O3 Core-Shell Nanoparticles for Toluene Oxidation Reaction
Chao Zhang, Sihan Li, Chenliang Wu, Xiaoqing Li, Xinhuan Yan
2020, 36(8): 1907057-0  doi: 10.3866/PKU.WHXB201907057
[摘要]  (110) [HTML全文] (110) [PDF 2461KB] (110)
摘要:
Customizing core-shell nanostructures is considered to be an efficient approach to improve the catalytic activity of metal nanoparticles. Various physiochemical and green methods have been developed for the synthesis of core-shell structures. In this study, a novel liquid-phase hydrogen reduction method was employed to form core-shell Pt@Au nanoparticles with intimate contact between the Pt and Au particles, without the use of any protective or structure-directing agents. The Pt@Au core-shell nanoparticles were prepared by depositing Au metal onto the Pt core; AuCl4− was reduced to Au(0) by H2 in the presence of Pt nanoparticles. The obtained Pt@Au core-shell structured nanoparticles were characterized by transmission electron microscopy (TEM), energy-dispersive X-ray spectroscopy (EDX), high-resolution TEM, fast Fourier transform, powder X-ray diffraction (PXRD), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR), and H2-temperature programmed reduction (H2-TPR) analyses. The EDX mapping results for the nanoparticles, as obtained from their scanning transmission electron microscopy images in the high-angle annular dark-field mode, revealed a Pt core with Au particles grown on its surface. Fourier transform measurements were carried out on the high-resolution structure to characterize the Pt@Au nanoparticles. The lattice plane at the center of the nanoparticles corresponded to Pt, while the edge of the particles corresponded to Au. With an increase in the Au content, the intensity of the peak corresponding to Pt in the FTIR spectrum decreased slowly, indicating that the Pt nanoparticles were surrounded by Au nanoparticles, and thus confirming the core-shell structure of the nanoparticles. The XRD results showed that the peak corresponding to Pt shifted gradually toward the Au peak with an increase in the Au content, indicating that the Au particles grew on the Pt seeds; this trend was consistent with the FTIR results. Hence, it can be stated that the Pt@Au core-shell structure was successfully prepared using the liquid-phase hydrogen reduction method. The catalytic activity of the nanoparticles for the oxidation of toluene was evaluated using a fixed-bed reactor under atmospheric pressure. The XPS and H2-TPR results showed that the Pt1@Au1/Al2O3 catalyst had the best toluene oxidation activity owing to its lowest reduction temperature, lowest Au 4d & 4f and Pt 4d & 4f binding energies, and highest Au0/Auδ+ and Pt0/Pt2+ proportions. The Pt1@Au2Al2O3 catalyst showed high stability under dry and humid conditions. The good catalytic performance and high selectivity of Pt@Au/Al2O3 for toluene oxidation could be attributed to the high concentration of adsorbed oxygen species, good low-temperature reducibility, and strong interaction.
亮点
由二氧化碳合成长链羧酸
刘志敏
2020, 36(8): 1912045-0  doi: 10.3866/PKU.WHXB201912045
[摘要]  (118) [HTML全文] (118) [PDF 279KB] (118)
摘要:
对结冰过程中临界冰核的探测
刘忠范
2020, 36(8): 2001013-0  doi: 10.3866/PKU.WHXB202001013
[摘要]  (104) [HTML全文] (104) [PDF 373KB] (104)
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“一箭双雕”:同时赋予金纳米团簇催化活性和水溶性
刘鸣华
2020, 36(8): 2001014-0  doi: 10.3866/PKU.WHXB202001014
[摘要]  (118) [HTML全文] (118) [PDF 544KB] (118)
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水/固界面的氢键动力学
江颖
2020, 36(8): 2001023-0  doi: 10.3866/PKU.WHXB202001023
[摘要]  (120) [HTML全文] (120) [PDF 770KB] (120)
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非金属元素催化活性的调控机理
杨金龙
2020, 36(8): 2001026-0  doi: 10.3866/PKU.WHXB202001026
[摘要]  (104) [HTML全文] (104) [PDF 0KB] (104)
摘要:
一种利用精确纳米组装结构调控水下产气速率的普适方法
俞书宏
2020, 36(8): 2001028-0  doi: 10.3866/PKU.WHXB202001028
[摘要]  (125) [HTML全文] (125) [PDF 616KB] (125)
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锌阳极原位固态电解质界面
陈立泉
2020, 36(8): 2001035-0  doi: 10.3866/PKU.WHXB202001035
[摘要]  (114) [HTML全文] (114) [PDF 582KB] (114)
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可编程DNA胶束
刘鸣华
2020, 36(8): 2001036-0  doi: 10.3866/PKU.WHXB202001036
[摘要]  (108) [HTML全文] (108) [PDF 873KB] (108)
摘要:
单壁碳纳米管的控制生长与生长动力学
杨金龙
2020, 36(8): 2002014-0  doi: 10.3866/PKU.WHXB202002014
[摘要]  (101) [HTML全文] (101) [PDF 528KB] (101)
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周期性长程有序介孔钯催化剂用于高效甲酸氧化催化
杨金龙
2020, 36(8): 2003010-0  doi: 10.3866/PKU.WHXB202003010
[摘要]  (104) [HTML全文] (104) [PDF 845KB] (104)
摘要:
专访
专访中国理论与计算化学领军人物:2019年新科院士杨金龙
《物理化学学报》编辑部
2020, 36(8): 1912046-0  doi: 10.3866/PKU.WHXB201912046
[摘要]  (121) [HTML全文] (121) [PDF 334KB] (121)
摘要:
特邀述评
建立学术共同体互信的基金评审机制的尝试与思考
戴亚飞, 高飞雪, 王翠霞, 陈拥军
2020, 36(8): 2003034-0  doi: 10.3866/PKU.WHXB202003034
[摘要]  (100) [HTML全文] (100) [PDF 292KB] (100)
摘要:
完善评审机制是国家自然科学基金委新时代基金改革的重要任务之一。为切实落实该项改革任务,建立符合新时代科学基金资助导向的科学、公正、高效的评审机制,基金委化学部努力探索新的学科基金管理模式,尝试了在通信评审阶段由科学家与学科管理人员共同参与项目的分组、指派,共同完成同行评议专家遴选工作的新模式。本文分析了科学家参与同行评议专家遴选工作的利弊,探讨了如何更好的发挥科学家在同行评议专家遴选工作中的作用,建立学术共同体互信的基金评审机制。
科学基金项目会议评审机制刍议
张国俊, 付雪峰, 戴亚飞, 陈拥军
2020, 36(8): 2003051-0  doi: 10.3866/PKU.WHXB202003051
[摘要]  (101) [HTML全文] (101) [PDF 515KB] (101)
摘要:
项目评审是科学基金管理工作的核心。本文梳理分析了目前科学界日益关注的会议评审过程中存在的问题,重新审视会议评审的意义和功能,提出基于“确认-纠偏-择优”原则的会评评审改革建议和措施。
大处着眼,小处入手——基金委化学科学部2019年基金项目会议评审工作的几点尝试和思考
付雪峰, 黄艳, 崔琳, 陈拥军
2020, 36(8): 2004002-0  doi: 10.3866/PKU.WHXB202004002
[摘要]  (138) [HTML全文] (138) [PDF 722KB] (138)
摘要:
国家自然科学基金是我国资助基础研究的主渠道,基金项目的同行评审环节对于自然科学基金资助工作至关重要。本文总结了化学科学部2019年基金项目会议评审工作的一些尝试,以营造良好学术评审环境为着眼点,采用分组会评、规范会评程序、细化会评流程等措施,完善项目会评工作。
浅析基金评审的模糊属性
付雪峰, 戴亚飞, 黄艳, 崔琳, 陈拥军
2020, 36(8): 2004048-0  doi: 10.3866/PKU.WHXB202004048
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编委会

发布时间:


《物理化学学报》第4届编委会

(按拼音排序)

名誉主编

唐有祺

北京大学

顾问编委

包信和

中国科学院大连化学物理研究所

段雪

北京化工大学

付贤智

福州大学

侯建国

中国科学技术大学

黄维

南京工业大学

LIEBER Charles M.

Harvard University

田中群

厦门大学

万立骏

中国科学院化学研究所

吴云东

北京大学

谢晓亮

Harvard University, 北京大学

杨伟涛

 Duke University

姚建年

中国科学院化学研究所

赵新生

北京大学

主编

刘忠范

北京大学

副主编

韩布兴

中国科学院化学研究所

刘鸣华

国家纳米科学中心

申文杰

中国科学院大连化学物理研究所

吴凯

北京大学

杨金龙

中国科学技术大学

庄林

武汉大学

迟力峰

苏州大学

编委

曹勇

复旦大学

陈经广

University of Delaware

陈军

南开大学

崔屹

Stanford University

邓风

中国科学院武汉物理与数学研究所

邓友全

中国科学院兰州化学物理研究所

樊卫斌

中国科学院山西煤炭化学研究所

房喻

陕西师范大学

付红兵

中国科学院化学研究所

傅强

中国科学院大连化学物理研究所

高毅勤

北京大学

郭林

北京航空航天大学

郝京诚

山东大学

侯文华

南京大学

金荣超

Carnegie Mellon University

来鲁华

北京大学

李朝军

McGill University

李隽

清华大学

李象远

四川大学

梁万珍

厦门大学

刘海超

北京大学

刘洪来

华东理工大学

刘述斌

University of North Carolina

刘义

武汉大学

刘志敏

中国科学院化学研究所

罗小民

中国科学院上海药物研究所

马晶

南京大学

孟庆波

中国科学院物理研究所

邵翔

中国科学技术大学

孙俊奇

吉林大学

谭蔚泓

湖南大学

唐智勇

国家纳米科学中心

王键吉

河南师范大学

王鹏

中国科学院长春应用化学研究所

王心晨

福州大学

王永锋

北京大学

魏子栋

重庆大学

翁羽翔

中国科学院物理研究所

吴鹏

华东师范大学

夏永姚

复旦大学

许国勤

National University of Singapore

杨俊林

国家自然科学基金委员会

余家国

武汉理工大学

尉志武

清华大学

占肖卫

北京大学

张东辉

中国科学院大连化学物理研究所

张浩力

兰州大学

张锦

北京大学

章俊良

上海交通大学

周永贵

中国科学院大连化学物理研究所

联系我们

发布时间: 2018-05-02


编辑部工作人员联系方式
 

张小娟
主任
010-62756388
黄路
编辑
010-62751724
欧阳贱华
编辑
010-62751721
於秀芝
编辑
010-62751724
熊英
编辑
010-62751724
周虹
技术编辑
010-62751724

 

通讯地址:北京市北京大学化学学院物理化学学报编辑部

邮政编码:100871

 

发布日期:2009-06-24 浏览: