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综述
水系锌二次电池MnO2正极的晶体结构、反应机理及其改性策略
陈鲜红, 阮鹏超, 吴贤文, 梁叔全, 周江
2022, 38(11): 2111003-0  doi: 10.3866/PKU.WHXB202111003
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摘要:
水系锌二次电池凭借其安全性高、环境友好、成本低廉、能量密度较高等诸多优势,有望应用于下一代大规模储能系统。电池的发展依赖于电极材料,二氧化锰由于其高丰度、低成本、毒性小等优势,在水系锌二次电池领域得到广泛应用。本文将从二氧化锰的晶体结构、反应机理及电化学性能出发,对其在水系锌二次电池中的研究进展进行系统综述。特别地,针对其容量低、循环稳定性差等问题,本文从储能机理(包括嵌入-脱嵌机制和溶解-沉积机制)角度出发,总结相对应的优化策略,为先进水系锌锰二次电池的设计开发提供参考。
纳米SiC基光催化剂研究进展
何科林, 沈荣晨, 郝磊, 李佑稷, 张鹏, 江吉周, 李鑫
2022, 38(11): 2201021-0  doi: 10.3866/PKU.WHXB202201021
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摘要:
工业化无疑促进了经济的发展,提高了生活水平,但也导致了一些问题,包括能源危机、环境污染、全球变暖等, 其中这些所产生问题主要是由燃烧煤炭、石油和天然气等化石燃料引起的。光催化技术具有利用太阳能将二氧化碳转化为碳氢化合物燃料、从水中制氢、降解污染物等优点,从而在解决能源危机的同时避免环境污染,因此被认为是解决这些问题的最有潜力的技术之一。在各种光催化剂中,碳化硅(SiC)由于其优良的电学性能和光电化学性质,在光催化、光电催化、电催化等领域具有广阔的应用前景。本文首先系统地阐述了各种SiC的合成方法,具体包括模板生长法、溶胶凝胶法、有机前驱物热解法、溶剂热合成法、电弧放电法,碳热还原法和静电纺丝等方法。然后详细地总结了提升SiC光催化活性的各种改性策略,如元素掺杂、构建Z型(S型)体系、负载助催化剂、可见光敏化、构建半导体异质结、负载炭材料、构建纳米结构等。最后重点论述了半导体的光催化机理以及SiC复合物在光催化产氢、污染物降解和CO2还原等领域的应用研究进展,并提出了前景展望。
钠离子电池用高性能锑基负极材料的调控策略研究进展
李莹, 来雪琦, 曲津朋, 赖勤志, 伊廷锋
2022, 38(11): 2204049-0  doi: 10.3866/PKU.WHXB202204049
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摘要:
锑(Sb)具有高的理论比容量、较小的电极极化、合适的Na+脱嵌电位、价格低廉以及环境友好的优势,而成为一种具有较大应用前景的钠离子电池负极材料。但是,Sb基负极材料的一个重要挑战是在循环过程中高比容量伴随着大的体积变化,进而导致活性材料粉化,并从集流体上脱落,这大大限制了其在钠离子电池领域的大规模应用。因此,如何解决Sb基负极材料充放电过程中体积膨胀问题对于高性能的钠离子电池设计是至关重要的。本文详细综述和讨论了Sb基材料的结构-性能关系及其在钠离子电池中的应用,详细介绍了钠离子电池Sb基负极材料在氧化还原反应机理、形貌设计、结构-性能关系等方面的最新研究进展。本综述的主要目的是探讨影响Sb基负极材料性能的决定因素,从而提出有前途的改性策略,以提高其可逆容量和循环稳定性。最后,对Sb基钠离子电池负极材料的未来发展、面临的挑战和前景进行了展望。本文可为Sb负极材料的构建和优化提供具体的观点,阐明了Sb基负极材料未来的发展方向,从而促进钠离子电池的快速发展和实际应用。
锂离子电池快充石墨负极研究与应用
丁晓博, 黄倩晖, 熊训辉
2022, 38(11): 2204057-0  doi: 10.3866/PKU.WHXB202204057
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摘要:
相较于传统燃油汽车,电动汽车缓慢的充电速度始终制约了其进一步推广。为电动汽车实现“加油式”快速充电能够缓解充电桩的使用压力,增加电动汽车的应用场景和市场占有率。因此,亟需开发出具有快速充放电能力的高性能锂离子电池。石墨因其低廉的价格和优异的电化学性能已经在锂离子电池负极领域得到了广泛的商业化应用,然而其较低的嵌锂电位导致在快充过程中出现析锂,损害电化学性能的同时会带来安全隐患。因此,必须对石墨进行改良处理,以适应快充技术的需要。本文系统介绍了近年来石墨负极快充化改良领域的研究进展,从成分设计,形貌调控,结构优化,电解液适配等方面进行了评述,并总结了快充石墨面临的挑战,展望了其发展前景,为推动快充技术的商业化应用提供了借鉴。
氟代溶剂在锂金属电池中的应用
何子旭, 陈亚威, 黄凡洋, 揭育林, 李新鹏, 曹瑞国, 焦淑红
2022, 38(11): 2205005-0  doi: 10.3866/PKU.WHXB202205005
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摘要:
近年来,锂金属电池由于具有较高的能量密度而成为储能领域的研究热点。电解液作为锂金属电池的“血液”发挥着至关重要的作用。在传统锂离子电池电解液中,锂金属负极与电解液之间的界面副反应严重并伴随着锂枝晶生长,从而导致安全隐患以及循环寿命缩短等问题。在解决锂金属负极问题上,电解液调控策略具有易操作性和有效性,因而在推动锂金属电池发展方面具有举足轻重的地位。氟代电解液是目前重要的研究方向,氟代电解液在循环过程中能够在电极表面形成富含LiF的固体电解质界面膜(SEI);该界面膜不仅可以有效抑制负极锂枝晶的形成,并且在正极方面能够大幅提高电解液的氧化稳定性,从而提升高电压正极的适配性和锂金属电池的循环稳定性。氟代电解液中氟代溶剂/氟代锂盐的分子结构对电解液的溶剂化结构有重要影响。当氟代溶剂分子中氟原子的位置与数量不同时,氟代溶剂的物理化学性质也会随之发生变化,进而改变了电解液与电极的界面反应性。因此,氟代溶剂能够起到调制SEI膜成分和结构的作用,是决定电池性能的关键因素。本文总结了应用于锂金属电池的主要氟代溶剂,尤其是近几年来发展的新型氟代溶剂;着重介绍了高度氟代的溶剂分子作为局域超浓电解液的稀释剂,以及对溶剂进行精准分子设计得到的部分氟代溶剂等。此外,本文还分析探讨了氟代溶剂分子与电池性能之间的构效关系,展望了构建新型氟代溶剂分子的策略,希望能对电解液溶剂分子的结构设计以及构效关系的评估有一定的启发意义。
Article
Quantum Efficiency and Voltage Losses in P3HT: Non-fullerene Solar Cells
Xiaoyun Xu, Hongbo Wu, Shijie Liang, Zheng Tang, Mengyang Li, Jing Wang, Xiang Wang, Jin Wen, Erjun Zhou, Weiwei Li, Zaifei Ma
2022, 38(11): 2201039-0  doi: 10.3866/PKU.WHXB202201039
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摘要:
From the industrial perspective, poly(3-hexylthiophene) (P3HT) is one of the most attractive donor materials in organic photovoltaics. The large bandgap in P3HT makes it particularly promising for efficient indoor light harvesting, a unique advantage of organic photovoltaic (PV) devices, and this has started to gain considerable attention in the field of PV technology. In addition, the up-scalability and long material stability associated with the simple chemical structure make P3HT one of the most promising materials for the mass production of organic solar cells. However, the solar cells based on P3HT has a low power conversion efficiency (PCE), which is less than 11%, mainly due to significant voltage losses. In this study, we identified the origin of the high quantum efficiency and voltage losses in the P3HT: non-fullerene based solar cells, and we proposed a strategy to reduce the losses. More specifically, we observed that: 1) the non-radiative decay rate of the charge transfer (CT) states formed at the donor–acceptor interfaces was much higher for the P3HT: non-fullerene solar cells than that for the P3HT: fullerene solar cells, which was the main reason for the more severely limited photovoltage; 2) the origin of the high non-radiative decay rate in the P3HT: non-fullerene solar cell could be ascribed to the short packing distance between the P3HT and non-fullerene acceptor molecules at the donor–acceptor interfaces (DA distance), which is a rarely studied interfacial structural property, highly important in determining the decay rate of CT states; 3) the lower voltage loss in the state-of-the-art P3HT solar cell based on the 2, 2'-((12, 13-bis(2-butyldecyl)-3, 9-diundecyl-12, 13-dihydro-[1, 2, 5]-thiadiazolo[3, 4-e]thieno[2'', 3'': 4', 5']thieno[2', 3': 4, 5]p-yrolo[3, 2-g]thieno[2', 3': 4, 5]thieno[3, 2-b]indole-2, 10-diyl)bis(methanelylidene))bis(5, 6-dichloro-1H-indene-1, 3(2H)-dion-e) (ZY-4Cl) acceptor could be associated with the better alignment of the energy levels of the active materials and the longer DA distance, compared to those based on the commonly used acceptors. However, the DA distance was still very short, limiting the device voltage. Thus, improving the performance of the P3HT based solar cells requires a further increase in the DA distance. Our findings are expected to pave the way for breaking the performance bottleneck of the P3HT based solar cells.
Spontaneous Reduction and Adsorption of K3[Fe(CN)6] on Zn Anodes in Alkaline Electrolytes: Enabling a Long-Life Zn-Ni Battery
Yuanhao Shen, Qingyu Wang, Jie Liu, Cheng Zhong, Wenbin Hu
2022, 38(11): 2206020-0  doi: 10.3866/PKU.WHXB202204048
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摘要:
In view of the continuously worsening environmental problems, fossil fuels will not be able to support the development of human life in the future. Hence, it is of great importance to work on the efficient utilization of cleaner energy resources. In this case, cheap, reliable, and eco-friendly grid-scale energy storage systems can play a key role in optimizing our energy usage. When compared with lithium-ion and lead-acid batteries, the excellent safety, environmental benignity, and low toxicity of aqueous Zn-based batteries make them competitive in the context of large-scale energy storage. Among the various Zn-based batteries, due to a high open-circuit voltage and excellent rate performance, Zn-Ni batteries have great potential in practical applications. Nevertheless, the intrinsic obstacles associated with the use of Zn anodes in alkaline electrolytes, such as dendrite, shape change, passivation, and corrosion, limit their commercial application. Hence, we have focused our current efforts on inhibiting the corrosion and dissolution of Zn species. Based on a previous study from our research group, the failure of the Zn-Ni battery was caused by the shape change of the Zn anode, which stemmed from the dissolution of Zn and uneven current distribution on the anode. Therefore, for the current study, we selected K3[Fe(CN)6] as an electrolyte additive that would help minimize the corrosion and dissolution of the Zn anode. In the alkaline electrolyte, [Fe(CN)6]3– was reduced to [Fe(CN)6]4– by the metallic Zn present in the Zn-Ni battery. Owing to its low solubility in the electrolyte, K4[Fe(CN)6] adhered to the active Zn anode, thereby inhibiting the aggregation and corrosion of Zn. Ultimately, the shape change of the anode was effectively eliminated, which improved the cycling life of the Zn-Ni battery by more than three times (i.e., from 124 cycles to more than 423 cycles). As for capacity retention, the Zn-Ni battery with the pristine electrolyte only exhibited 40% capacity retention after 85 cycles, while the Zn-Ni battery with the modified electrolyte (i.e., containing K3[Fe(CN)6]) showed 72% capacity retention. Moreover, unlike conventional organic additives that increase electrode polarization, the addition of K3[Fe(CN)6] not only significantly reduced the charge-transfer resistance in a simplified three-electrode system, but also improved the discharge capacity and rate performance of the Zn-Ni battery. Importantly, considering that this strategy was easy to achieve and minimized additional costs, K3[Fe(CN)6], as an electrolyte additive with almost no negative effect, has tremendous potential in commercial Zn-Ni batteries.
Review
Metal Sulfide-Based Potassium-Ion Battery Anodes: Storage Mechanisms and Synthesis Strategies
Yichen Du, Zhuangzhuang Zhang, Yifan Xu, Jianchun Bao, Xiaosi Zhou
2022, 38(11): 2205017-0  doi: 10.3866/PKU.WHXB202205017
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Rechargeable potassium-ion batteries (PIBs), with their low cost and the abundant K reserves, have been promising candidates for energy storage and conversion. Among all anode materials for PIBs, metal sulfides (MSs) show superiority owing to their high theoretical capacity and variety of material species. Nevertheless, the battery performance of MSs is hindered by many factors such as poor conductivity, low ion diffusivity, sluggish interfacial/surface transfer kinetics, and drastic volume changes. In this review, the electrochemical reaction mechanisms, challenges, and synthesis methods of MSs for PIBs are summarized and discussed. In particular, the most common synthesis methods of MSs for PIBs are highlighted, including template synthesis, hydro/solvothermal synthesis, solid-phase chemical synthesis, electrospinning synthesis, and ion-exchange synthesis. During the potassium storage process, the two-dimensional layered MSs follow the intercalation/extraction mechanism, and the MSs with inactive metal undergo the conversion reaction, whereas the metal-active MSs follow the conversion-alloying reaction mechanism. Given the inherent properties of MSs and the reactions they undergo during cycling, when used as anodes for PIBs, such materials experience a series of problems, including poor ion-/electron-transport kinetics, structural instability, and loss of active material caused by the dissolution of discharged polysulfide products and the occurrence of side reactions. These problems can be solved by optimizing the methods for synthesizing MSs with an ideal composition and structure. The template method can precisely prepare porous or hollow-structured materials, the hydro/solvothermal method can alter the thickness or size of the material by adjusting certain synthesis parameters, and the one-dimensional-structured material obtained via electrospinning often has a large specific surface area, all of which can shorten the transport pathway for potassium ions, thereby improving the performance of the battery. The ion-exchange method affords difficult-to-synthesize MSs via anion- or cation-exchange, in which the product inherits the structure of the starting material. The solid-phase synthesis method makes it possible to combine MSs with other materials. Combinations with materials such as carbon or other MSs helps to provide sufficient buffer space for the volume expansion of MSs during cycling, while promoting electron transport and improving the potassium-storage properties of the anodes. Therefore, this review aims to highlight the current defects of MS anodes and explore the construction of their ideal architecture for high-performance PIBs by optimizing the synthesis methods. Ultimately, we propose the possible future advancement of MSs for PIBs.
Cu-Based Tandem Catalysts for Electrochemical CO2 Reduction
Yongxia Shi, Man Hou, Junjun Li, Li Li, Zhicheng Zhang
2022, 38(11): 2206020-0  doi: 10.3866/PKU.WHXB202206020
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Through the combustion of fossil fuels and other human activities, large amounts of CO2 gas have been emitted into the atmosphere, causing many environmental problems, such as the greenhouse effect and global warming. Thus, developing and utilizing renewable clean energy is crucial to reduce CO2 emission and achieve carbon neutrality. The electrochemical CO2 reduction reaction (CO2RR) has been considered as an effective approach to obtain high value-added chemicals and fuels, which can store intermittent renewable energy and achieve the artificial carbon cycle. In addition, due to its multiple advantages, such as mild reaction conditions, tunable products, and simple implementation, electrochemical CO2RR has attracted extensive attention. Electrochemical CO2RR involves multiple electron–proton transfer steps to obtain multitudinous products, such as C1 products (CO, HCOOH, CH4, etc.) and C2 products (C2H4, C2H5OH, etc.). The intermediates, among which *CO is usually identified as the key intermediate, and reaction pathways of different products intersect, resulting in an extremely complex reaction mechanism. Currently, copper has been widely proven to be the only metal catalyst that can efficiently reduce CO2 to hydrocarbons and oxygenates due to its suitable adsorption energy for *CO. However, the low product selectivity, poor stability, and high overpotential of pure Cu hinder its use for the production of industrial-grade multi-carbon products. Tandem catalysts with multiple types of active sites can sequentially reduce CO2 molecules into desired products. When loaded onto a co-catalyst that can efficiently convert CO2 to *CO (such as Au and Ag), Cu acts as an electron donor owing to its high electrochemical potential. *CO species generated from the substrate can spillover onto the surface of electron-poor Cu due to the stronger adsorption and be further reduced to C2+ products. The use of Cu-based tandem catalysts for electrochemical CO2RR is a promising strategy for improving the performance of CO2RR and thus, has become a research hotspot in recent years. In this review, we first introduce the reaction routes and tandem mechanisms of electrochemical CO2RR. Then, we systematically summarize the recent research progress of Cu-based tandem catalysts for electrochemical CO2RR, including Cu-based metallic materials (alloys, heterojunction, and core-shell structures) as well as Cu-based framework materials, carbon materials, and polymer-modified materials. Importantly, the preparation methods of various Cu-based tandem catalysts and their structure–activity relationship in CO2RR are discussed and analyzed in detail. Finally, the challenges and opportunities of the rational design and controllable synthesis of advanced tandem catalysts for electrochemical CO2RR are proposed.
Tuning the Coordination Structure of Single Atoms and Their Interaction with the Support for Carbon Dioxide Electroreduction
Yuxin Chen, Lijun Wang, Zhibo Yao, Leiduan Hao, Xinyi Tan, Justus Masa, Alex W. Robertson, Zhenyu Sun
2022, 38(11): 2206020-0  doi: 10.3866/PKU.WHXB202207024
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The combustion of fossil fuels increases atmospheric carbon dioxide (CO2) concentrations, leading to adverse impacts on the planetary radiation balance and, consequently, on the climate. Fossil fuel utilization has contributed to a marked rise in global temperatures, now at least 1.2 ℃ above 'pre-industrial' levels. To meet the 2015 Paris Agreement target of 1.5 ℃ above pre-industrial levels, considerable efforts are required to efficiently capture and utilize CO2. Among the different strategies developed for converting CO2, electrochemical CO2 reduction (ECR) to valuable chemicals using renewable energy is expected to revolutionize the manufacture of sustainable "green" chemicals, thereby achieving a closed anthropogenic carbon cycle. However, CO2 is a thermodynamically stable and kinetically inert molecule that requires high electrical energy to bend the linear O=C=O bond by attacking the C atom. To facilitate the ECR with good energy efficiency, it is essential to lower the reaction overpotential as well as maintain a high current density and desirable product selectivity; therefore, the design and development of advanced electrocatalysts are crucial. A plethora of heterogeneous and homogeneous materials has been explored in the ECR. Among these materials, single-atom catalysts (SACs) have been the focus of most extensive research in the context of ECR. A SAC with isolated metal atoms dispersed on a supporting host exhibits a unique electronic structure, well-defined coordination environment, and an extremely high atom utilization maximum; thus, SACs have emerged as promising materials over the last two decades. Single-atom catalysis has covered the periodic table from d-block and ds-block metals to p-block metals. The types of support materials for SACs, ranging from metal oxides to tailored carbon materials, have also expanded. The adsorption strength and catalytic activity of SACs can be effectively tuned by modulating the central metal and local coordination structure of the SACs. In this article, we discuss the progress made to date in the field of single-atom catalysis for promoting ECR. We provide a comprehensive review of state-of-the-art SACs for the ECR in terms of product distribution, selectivity, partial current density, and performance stability. Special attention is paid to the modification of SACs to improve the ECR efficiency. This includes tailoring the coordination of the heteroatom, constructing bimetallic sites, engineering the morphologies and surface defects of supports, and regulating surface functional groups. The correlation of the coordination structure of SACs and metal-support interactions with ECR performance is analyzed. Finally, development opportunities and challenges for the application of SACs in the ECR, especially to form multi-carbon products, are presented.

  

Article
Construction of 1D/2D W18O49/Porous g-C3N4 S-Scheme Heterojunction with Enhanced Photocatalytic H2 Evolution
Yue Huang, Feifei Mei, Jinfeng Zhang, Kai Dai, Graham Dawson
2022, 38(7): 2108028-0  doi: 10.3866/PKU.WHXB202108028
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摘要:
Photocatalytic hydrogen production is an effective strategy for addressing energy shortage and converting solar energy into chemical energy. Exploring effective strategies to improve photocatalytic H2 production is a key challenge in the field of energy conversion. There are numerous oxygen vacancies on the surface of non-stoichiometric W18O49 (WO), which result in suitable light absorption performance, but the hydrogen evolution effect is not ideal because the band potential does not reach the hydrogen evolution potential. A suitable heterojunction is constructed to optimize defects such as high carrier recombination rate and low photocatalytic performance in a semiconductor. Herein, 2D porous carbon nitride (PCN) is synthesized, followed by the in situ growth of 1D WO on the PCN to realize a step-scheme (S-scheme) heterojunction. When WO and PCN are composited, the difference between the Fermi levels of WO and PCN leads to electron migration, which balances the Fermi levels of WO and PCN. Electron transfer leads to the formation of an interfacial electric field and bends the energy bands of WO and PCN, thereby resulting in the recombination of unused electrons and holes while leaving used electrons and holes, which can accelerate the separation and charge transfer at the interface and endow the WO/PCN system with better redox capabilities. In addition, PCN with a porous structure provides more catalytic active sites. The photocatalytic performance of the sample can be investigated using the amount of hydrogen released. Compared to WO and PCN, 20%WO/PCN composite has a higher H2 production rate (1700 μmol·g-1·h-1), which is 56 times greater than that of PCN (30 μmol·g-1·h-1). This study shows the possibility of the application of S-scheme heterojunction in the field of photocatalytic H2 production.
Rationally Designed Mn0.2Cd0.8S@CoAl LDH S-Scheme Heterojunction for Efficient Photocatalytic Hydrogen Production
Shanchi Liu, Kai Wang, Mengxue Yang, Zhiliang Jin
2022, 38(7): 2109023-0  doi: 10.3866/PKU.WHXB202109023
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Constructing an efficient and stable heterojunction photocatalyst system is a promising approach to achieve solar-driven water splitting to produce hydrogen. In this work, a novel Mn0.2Cd0.8S@CoAl LDH (MCCA) S-scheme heterojunction was successfully prepared through the efficient coupling of Mn0.2Cd0.8S nanorods and CoAl LDH nanosheets, employing a physical mixing method. The photoluminescence and photocurrent-time response results demonstrated that the internal electric field of the constructed MCCA S-scheme heterojunction could successfully accelerate charge separation and electron transfer between the Mn0.2Cd0.8S interface and the CoAl LDH. Critically, the introduction of the CoAl LDH effectively inhibited the recombination of photogenerated electrons and holes, thereby improving the photocatalytic hydrogen production activity of Mn0.2Cd0.8S. A maximum H2 production of 1177.9 μmol in 5 h was obtained with MCCA-3. This represents a significant improvement compared to what can be achieved with the pure Mn0.2Cd0.8S nanorods and CoAl LDH nanosheets individually. This work provides a simple and effective approach for the rational design of S-scheme heterojunction photocatalysts for photocatalytic hydrogen production.
P-Doped g-C3N4 Nanosheets with Highly Dispersed Co0.2Ni1.6Fe0.2P Cocatalyst for Efficient Photocatalytic Hydrogen Evolution
Rongchen Shen, Lei Hao, Qing Chen, Qiaoqing Zheng, Peng Zhang, Xin Li
2022, 38(7): 2110014-0  doi: 10.3866/PKU.WHXB202110014
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摘要:
Throughout the twentieth century, temperatures climbed rapidly as the use of fossil fuels proliferated and greenhouse gas levels soared. Thus, the need to develop environmentally friendly energy sources to replace traditional fossil fuels is urgent. Clean and highly efficient, hydrogen is considered the most promising energy source to replace traditional fossil fuels. The production of hydrogen by photocatalytic water splitting is environmentally friendly, and is considered the most promising method for producing hydrogen energy. Enhancing the separation efficiency of photogenerated electron-hole pairs has been identified as a key milestone for constructing high-efficiency photocatalysts. However, the construction of efficient and stable hydrogen-evolution photocatalysts with highly dispersed cocatalysts remains a challenge. Here, we succeeded, for the first time, in fabricating P-doped CNS (PCNS) with a highly dispersed non-noble trimetallic transition metal phosphide Co0.2Ni1.6Fe0.2P cocatalyst (PCNS-CoNiFeP), by a one-step in situ high-temperature phosphating method. Remarkably, the CoNiFeP in PCNS-CoNiFeP demonstrated no aggregation and high dispersibility compared with CoNiFeP prepared by the traditional hydroxide-precursor phosphating method (PCNS-CoNiFeP-OH). X-ray diffraction, X-ray photoelectron spectroscopy, element mapping images, and high-resolution transmission electron microscopy results demonstrate that PCNS-CoNiFeP was successfully synthesized. The UV-Vis absorption results indicate a slight increase in absorbance for PCNS-CoNiFeP in the 200–800 nm wavelength region compared with that of PCNS. Photoluminescence spectroscopy, electrochemical impedance spectroscopy, and photocurrent results demonstrated that CoNiFeP cocatalysts could effectively promote the separation of photogenerated electron-hole pairs and accelerate the migration of carriers. The linear sweep voltammetry results also demonstrate that the CoNiFeP cocatalyst loading could significantly decrease the overpotential of CNS. Therefore, the maximum hydrogen evolution rate of PCNS-CoNiFeP was 1200 μmol·h-1·g-1, which was approximately four times higher than that of pure CNS-Pt (320 μmol·h-1·g-1) when using TEOA solution as a sacrificial agent. The apparent quantum efficiency of PCNS-CoNiFeP was 1.4% at 420 nm. The PCNS-CoNiFeP also exhibited good stability during the photocatalytic reaction. In addition, the TEM results indicate that CoNiFeP with a size of 6–8 nm are highly dispersed on the PCNS surface. The highly dispersed CoNiFeP demonstrated better charge-separation capacity and higher intrinsic electrocatalytic hydrogen-evolution activity than the aggregated CoNiFeP. Thus, the hydrogen evolution rate of aggregated CoNiFeP-PCNs (300 μmol·h-1·g-1) was much lower than that of PCNS-CoNiFeP. Furthermore, P doping of CNS could improve electric conductivity and charge transport. It is expected that loading highly dispersed CoNiFeP and P doping could be extended to promote photocatalytic hydrogen production using various photocatalysts.
Enhancement of Photocatalytic H2-Evolution Kinetics through the Dual Cocatalyst Activity of Ni2P-NiS-Decorated g-C3N4 Heterojunctions
Zhuonan Lei, Xinyi Ma, Xiaoyun Hu, Jun Fan, Enzhou Liu
2022, 38(7): 2110049-0  doi: 10.3866/PKU.WHXB202110049
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摘要:
With rapid industrialization, issues pertaining to the environment and energy have become an alarming concern. Photocatalytic water splitting is considered one of the most promising green technologies capable of resolving these issues, as it can convert solar energy into chemical energy and have a positive impact on the realization of "carbon neutrality". Current research focuses on the development of highly efficient catalysts to improve the photocatalytic H2-production activity. Transition metal phosphides and sulfides are often used as photocatalysts owing to their low H2-evolution overpotential and excellent electrical conductivity. Among them, Ni2P and NiS have generally been used independently during photocatalytic H2 production; however, it is necessary to study the synergistic effect when they are combined as a dual cocatalyst. In this work, we successfully prepared a Ni2P-NiS dual cocatalyst for the first time via a simple hydrothermal method using red phosphorus (RP) and thioacetamide (C2H5NS) as the sources of P and S. Ni2P-NiS was then introduced to the surface of g-C3N4 nanosheets through solvent evaporation to create a Ni2P-NiS/g-C3N4 heterojunction. Furthermore, X-ray diffraction (XRD), scanning electron microscope (SEM), transmission electron microscope (TEM), ultraviolet-visible spectrophotometry (UV-Vis), X-ray photoelectron spectroscopy (XPS), photoluminescence (PL), linear sweep voltammetry (LSV), Mott-Schottky (M-S), and electrochemical impedance spectroscopy (EIS) were used to reveal the crystal structures, morphologies, element compositions, and photoelectric characteristics of the samples; thus, it was demonstrated that Ni2P-NiS was successfully deposited on the surface of g-C3N4 and that together they exhibited better activity than their monomers. Moreover, the optimized 15% Ni2P-NiS/g-C3N4 composite exhibits a H2 generation rate of 6892.7 μmol·g-1·h-1, which is about 46.1, 7.5 and 4.4 times higher than that of g-C3N4 (150 μmol·g-1·h-1), 15% NiS/g-C3N4 (914.5 μmol·g-1·h-1), and 15% Ni2P/g-C3N4 (1565.9 μmol·g-1·h-1), respectively. In addition, photoelectric performance tests show that Ni2P-NiS/g-C3N4 has a stronger photocurrent intensity, smaller charge-transfer resistance, more positive H2-evolution overpotential, and better charge-separation ability than the individual components (i.e., Ni2P and NiS), suggesting that the coexistence of Ni2P and NiS can further boost the activity of g-C3N4 during H2 evolution compared with their monomers. This is mainly due to the Schottky barrier effect between Ni2P-NiS nanoparticles and g-C3N4 nanosheets, which can greatly promote charge separation and charge transfer at their interface. Additionally, Ni2P-NiS can reduce the H2-evolution overpotential, leading to the increased surface kinetics of H2 evolution. This work offers a promising approach to obtaining a highly active and stable noble-metal-free dual cocatalyst for photocatalytic H2 production.
Enhanced Photocatalytic CO2 Reduction over 2D/1D BiOBr0.5Cl0.5/WO3 S-Scheme Heterostructure
Bichen Zhu, Xiaoyang Hong, Liyong Tang, Qinqin Liu, Hua Tang
2022, 38(7): 2111008-0  doi: 10.3866/PKU.WHXB202111008
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摘要:
Catalytic reduction of CO2 to CO has been considered promising for converting the greenhouse gas into chemical intermediates. Compared to other catalytic methods, photocatalytic CO2 reduction, which uses solar energy as the energy input, has attracted significant attention because it is a clean and inexhaustible resource. Therefore, using high-performance photocatalysts for effective CO2 reduction under mild reaction conditions is an active research hotspot. However, several current photocatalysts suffer from low solar energy conversion efficiency due to the extensive charge recombination and few active sites, leading to low CO2 reduction efficiency. Generally, constructing an S-scheme heterojunction can not only promote charge separation but also help maintain strong redox ability. Therefore, the S-scheme heterojunction is expected to help in achieving high conversion activity and CO2 reduction efficiency. Here, 2D tetragonal BiOBr0.5Cl0.5 nanosheets and hexagonal WO3 nanorods were prepared using a simple hydrothermal synthesis method, and the 2D/1D BiOBr0.5Cl0.5 nanosheets/WO3 nanorods (BiOBr0.5Cl0.5/WO3) S-scheme heterojunction with near infrared (NIR) light (> 780 nm) response were prepared via the electrostatic self-assembly method for the photocatalytic CO2 reduction. Following characterization and analysis, including diffuse reflectance spectra (DRS), Mott-Schottky plots, transient photocurrent response, time-resolution photoluminescence spectrum (TRPL), electrochemical impedance spectroscopy (EIS), linear sweep voltammetry (LSV), and electron spin resonance (ESR) measurements, it can be demonstrated that an S-scheme carrier transfer route was formed between the 2D BiOBr0.5Cl0.5 nanosheets and 1D WO3 nanorods. Driven by the internal electric field, which was formed between the two semiconductors, electron migration was boosted, thus inhibiting the recombination of photogenerated carriers, while the stronger redox ability was maintained, thus providing good reduction efficiency over BiOBr0.5Cl0.5/WO3 composite in CO2 reduction. In addition, the 2D/1D nanosheet/nanorod structure allowed for enhanced interface contact with abundant active sites, which favored charge separation and increased photocatalytic activity. Furthermore, the amount of WO3 nanorods added during the preparation of the composites was altered, which led to the optimal amount of 5% (w, mass fraction) for the photocatalytic CO2 reduction. As a result, the BiOBr0.5Cl0.5/WO3 composite exhibited superior photocatalytic reduction performance with a CO yield of 16.68 μmol·g-1·h-1 in the presence of any precious metal cocatalyst or sacrificial agent, which was 1.7 and 9.8 times that of pure BiOBr0.5Cl0.5 and WO3, respectively. In addition, the BiOBr0.5Cl0.5/WO3 composite provided continuously increased CO yields with excellent selectivity under full-spectrum light irradiation, suggesting good photocatalytic stability. This work describes a novel idea for the construction of 2D/1D S-scheme heterojunction photocatalysts for efficient CO2 reduction.
Hollow NiCo2S4 Nanospheres as a Cocatalyst to Support ZnIn2S4 Nanosheets for Visible-Light-Driven Hydrogen Production
Zhuang Xiong, Yidong Hou, Rusheng Yuan, Zhengxin Ding, Wee-Jun Ong, Sibo Wang
2022, 38(7): 2111021-0  doi: 10.3866/PKU.WHXB202111021
[摘要]  (314) [HTML全文] (314) [PDF 2138KB] (314)
摘要:
The rational interface tailoring of nanosheets on hollow spheres is a promising strategy to develop efficient photocatalysts for hydrogen production with solar energy. Among the various photocatalyst materials, metal sulfides have been extensively researched because of their relatively narrow band gap and superior visible-light response. ZnIn2S4 is a layered ternary chalcogenide semiconductor photocatalyst with a tunable band gap energy (approximately 2.4 eV). Among various metal sulfide photocatalysts, ZnIn2S4 has gained considerable attention. However, intrinsic ZnIn2S4 only exhibits a relatively moderate photocatalytic activity, which is mainly owing to the high recombination and low migration rate of photocarriers. Loading cocatalysts onto semiconductor photocatalysts is an effective way to improve the performance of photocatalysts, because it can not only facilitate the separation of electron-hole pairs, but also reduce the activation energy for proton reduction. As a ternary transition metal sulfide, NiCo2S4 features a high electrical conductivity, low electronegativity, excellent redox properties, and outstanding electrocatalytic activity. Such favorable characteristics suggest that NiCo2S4 can expedite charge separation and transfer, thereby promoting photocatalytic H2 production by serving as a cocatalyst. Moreover, both NiCo2S4 and ZnIn2S4 possess the ternary spinel crystal structure, which may facilitate the construction of NiCo2S4/ZnIn2S4 hybrids with tight interfacial contact for an enhanced photocatalytic performance. Herein, ultrathin ZnIn2S4 nanosheets were grown in situ on a non-noble-metal cocatalyst, namely NiCo2S4 hollow spheres, to form hierarchical NiCo2S4@ZnIn2S4 hollow heterostructured photocatalysts with an intimately coupled interface and strong visible light absorption extending to ca. 583 nm. The optimized NiCo2S4@ZnIn2S4 hybrid with a NiCo2S4 content of ca. 3.1% exhibited a high hydrogen evolution rate of 78 μmol·h-1, which was approximately 9 times higher than that of bare ZnIn2S4 and 3 times higher than that of 1% (w, mass fraction) Pt/ZnIn2S4. Additionally, the hybrid photocatalysts displayed good stability in the reaction. Photoluminescence and electrochemical analysis results indicated that NiCo2S4 hollow spheres served as an efficient cocatalyst for facilitating the separation and transport of light-induced charge carriers as well as reducing the hydrogen evolution reaction barrier. Finally, a possible reaction mechanism for the photocatalytic hydrogen evolution was proposed. In the NiCo2S4@ZnIn2S4 composite photocatalyst, the NiCo2S4 cocatalyst with high electrical conductivity favorably accepts the photoinduced electrons transferred from ZnIn2S4 and then employs the electrons to reduce protons for H2 production on the reactive sites. Concurrently, the photogenerated holes are trapped by TEOA that acts as a hole scavenger to accomplish the photoredox cycle. This study provides guidance for the fabrication of hierarchical hollow heterostructures based on nanosheet semiconductor subunits as remarkable photocatalysts for hydrogen production.
A 0D/2D Bi4V2O11/g-C3N4 S-Scheme Heterojunction with Rapid Interfacial Charges Migration for Photocatalytic Antibiotic Degradation
Liang Zhou, Yunfeng Li, Yongkang Zhang, Liewei Qiu, Yan Xing
2022, 38(7): 2112027-0  doi: 10.3866/PKU.WHXB202112027
[摘要]  (268) [HTML全文] (268) [PDF 2344KB] (268)
摘要:
With the rapid development of industrial technology, a large number of organic pollutants are routinely released into the environment, which has caused serious problems. Semiconductor photocatalysis is an environmentally-friendly and effective method to degrade and remove typical pollutants, and photocatalysts play a key role in the application of this technology. Therefore, various semiconductor materials have been tried and used in the field of pollutant removal. Graphite carbon nitride (g-C3N4) has attracted great interest because of its two-dimensional layered structure and good visible light response range. Owing to a narrow bandgap, adjustable band structure, and high physicochemical stability, g-C3N4 absorbs wavelengths up to 450 nm in the visible spectrum, leading to an opportunity for visible-light photocatalytic performance. Nevertheless, there are still some drawbacks that limit the photocatalytic efficiency of g-C3N4 in the removal of antibiotics and dyes under visible light, such as the rapid recombination of photoinduced charges and the weak oxidation capacity of holes. To advance this promising photocatalytic material, multiple methods have been tried to optimize the electronic band structure of g-C3N4, such as doping with various elements, morphology control, and functional group modification. Recently, a novel type of Step-scheme (S-scheme) heterojunction composed of two n-type semiconductor photocatalysts has been proposed, which can utilize a more positive valance band and a more negative conduction band. It was demonstrated that the formation of S-scheme heterojunctions is a valid way to increase photocatalytic activity of g-C3N4. Herein, novel 0D/2D Bi4V2O11/g-C3N4 S-scheme heterojunctions were prepared by a simple in situ solvothermal growth method. The Bi4V2O11/g-C3N4 composites displayed a high photocatalytic activity through the removal of oxytetracycline (OTC) and Reactive Red 2. In particular, the BVCN-50 composite showed the highest degradation efficiency for OTC of 74.1% and for Reactive Red 2 of 84.2% with ·O2- as the primary active species. This highly improved photocatalytic performance can be ascribed to the generation of S-scheme heterojunctions, which provides for a high redox capacity of the heterojunction system (strong oxidative ability of Bi4V2O11 and strong reductive capacity of g-C3N4) and facilitates the space separation of photo-generated charges. Moreover, the surface plasmon resonance effect of metallic Bi0 broadens the light utilization range of the heterojunction system. In addition, the possible degradation pathway and intermediates throughout the degradation process of OTC based on liquid chromatograph mass spectrometer (LC-MS) analysis were also studied. This work provides a novel tactic for the design and fabrication of g-C3N4-based S-scheme heterojunctions with enhanced photocatalytic performance.
Enhanced Photocatalytic H2O2 Production over Inverse Opal ZnO@Polydopamine S-Scheme Heterojunctions
Gaowei Han, Feiyan Xu, Bei Cheng, Youji Li, Jiaguo Yu, Liuyang Zhang
2022, 38(7): 2112037-0  doi: 10.3866/PKU.WHXB202112037
[摘要]  (319) [HTML全文] (319) [PDF 2559KB] (319)
摘要:
Photocatalytic H2O2 production is a sustainable and inexpensive process that requires water and gaseous O2 as raw materials and sunlight as the energy source. However, the slow kinetics of current photocatalysts limits its practical application. ZnO is commonly used as a photocatalytic material in the solar-to-chemical conversion, owing to its high electron mobility, nontoxicity, and relatively low cost. The adsorption capacity of H2O2 on the ZnO surface is low, which leads to the continuous production of H2O2. However, its photoresponse is limited to the ultraviolet (UV) region due to its wide bandgap (3.2 eV). Polydopamine (PDA) has emerged as an effective surface functionalization material in the field of photocatalysis due to its abundant functional groups. PDA can be strongly anchored onto the surface of a semiconducting photocatalyst through covalent and noncovalent bonds. The superior properties of PDA served as a motivation for this study. Herein, we prepare an inverse opal-structured porous PDA-modified ZnO (ZnO@PDA) photocatalyst by in situ self-polymerization of dopamine hydrochloride. The crystal structure, morphology, valency, stability, and energy band structure of photocatalysts are characterized by X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), transmission electron microscopy (TEM), field-emission scanning electron microscopy (FE-SEM), X-ray photoelectron spectroscopy (XPS), UV-visible diffuse reflectance spectroscopy (UV-Vis DRS), electrochemical impedance spectroscopy (EIS), Mott-Schottky curve (MS), and electron paramagnetic resonance (EPR). The experimental results showed that electrons in PDA are transferred to ZnO upon contact, which results in an electric field at their interface in the direction from PDA to ZnO. The photoexcited electrons in the ZnO conduction bands flow into PDA, driven by the electric field and bent bands, and are recombined with the holes of the highest occupied molecular orbital of PDA, thereby exhibiting an S-scheme charge transfer. This unique S-scheme mechanism ensures effective electron/hole separation and preserves the strong redox ability of used photocarriers. In addition, the inverse opal structure of ZnO@PDA promotes light-harvesting due to the supposed "slow photon" effect, as well as Bragg diffraction and scattering. Moreover, the enhanced surface area provides a high adsorption capacity and increased active sites for photocatalytic reactions. Therefore, the resulting ZnO@PDA (0.03% (atomic fraction) PDA) exhibits the optimal H2O2 production performance (1011.4 μmol·L-1·h-1), which is 4.4 and 8.9 times higher than pristine ZnO and PDA, respectively. The enhanced performance is ascribed to the improved light absorption, efficient charge separation, and strong redox capability of photocarriers in the S-scheme heterojunction. Therefore, this study provides a novel strategy for the design of inorganic/organic S-scheme heterojunctions for efficient photocatalytic H2O2 production.
Efficient Degradation of Tetracycline via Coupling of Photocatalysis and Photo-Fenton Processes over a 2D/2D α-Fe2O3/g-C3N4 S-Scheme Heterojunction Catalyst
Wenliang Wang, Haochun Zhang, Yigang Chen, Haifeng Shi
2022, 38(7): 2201008-0  doi: 10.3866/PKU.WHXB202201008
[摘要]  (269) [HTML全文] (269) [PDF 1625KB] (269)
摘要:
Graphitic carbon nitride (g-C3N4) has been widely used as a potential photocatalytic material for the removal of tetracycline from water. However, the poor visible light absorption ability and high recombination rate of the photogenerated charge significantly inhibit the catalytic activity of g-C3N4. Therefore, facile methods to improve the photocatalytic efficiency of g-C3N4 need to be developed. Hematite (α-Fe2O3), which has a good visible light absorption and corrosion resistance, is often used for photocatalysis and photo-Fenton reactions. Therefore, a two-dimension/two-dimension (2D/2D) S-scheme heterojunction constructed of g-C3N4 and α-Fe2O3 nanosheets could be expected to improve the degradation efficiency of tetracycline. In this study, 2D/2D S-scheme α-Fe2O3/g-C3N4 photo-Fenton catalysts were prepared using a hydrothermal strategy. The photo-Fenton catalytic activity of α-Fe2O3/g-C3N4 (α-Fe2O3 50% (w)) was significantly improved by the addition of a small amount of H2O2, removing 78% of tetracycline within 20 min, which was approximately 3.5 and 5.8 times the removal achieved using α-Fe2O3 and g-C3N4, respectively. The high catalytic activity was attributed to the synergy between the photocatalysis and Fenton reaction promoted by the continuous Fe3+/Fe2+ conversion over the 2D/2D S-scheme heterojunction. The 2D/2D S-scheme heterojunction was crucial in the fabrication of the α-Fe2O3/g-C3N4 photocatalyst with a large surface area, adequate active sites, and strong oxidation-reduction capability. Furthermore, the photo-Fenton reaction provided additional hydroxyl radicals for the degradation of tetracycline with the aid of H2O2. The excess reaction product (Fe3+) was reduced to Fe2+ by the photogenerated electrons from the conduction band of α-Fe2O3. The resulting Fe2+ could participate in the photo-Fenton reaction. The morphological structures of α-Fe2O3/g-C3N4 were analyzed using transmission electron microscopy to demonstrate the formation of a 2D/2D structure with face-to-face contact, and the optical properties of the composites were measured using ultraviolet-visible diffuse reflectance spectroscopy. α-Fe2O3/g-C3N4 possessed a significantly improved visible light absorption compared to g-C3N4. Five sequential cyclic degradation tests and X-ray diffraction (XRD) patterns obtained before and after the reaction showed that the α-Fe2O3/g-C3N4 composites possessed stable photo-Fenton catalytic activity and crystal structures. Transient photocurrent responses of α-Fe2O3/g-C3N4 demonstrated that the prepared composites exhibited a higher charge transfer efficiency compared to that of single α-Fe2O3 and g-C3N4. In addition, according to the photoluminescence analysis and active species trapping experiments, a possible S-scheme heterojunction charge transfer process in the photo-Fenton catalytic reaction was proposed. This study provided a promising method for the construction of a high-performance photo-Fenton catalytic system to remove antibiotics from wastewater.
Highlight
Insights into Mechanism of CsPbBr3 Nanocrystal Interfacial Modifier in Perovskite Solar Cells
S. Wageh, Ahmed A. Al-Ghamdi, Li Zhao
2022, 38(7): 2111009-0  doi: 10.3866/PKU.WHXB202111009
[摘要]  (238) [HTML全文] (238) [PDF 582KB] (238)
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Core-Shell Au@NiS1+x Cocatalyst for Excellent TiO2 Photocatalytic H2 Production
S. Wageh, Ahmed A. Al-Ghamdi, Quanlong Xu
2022, 38(7): 2202001-0  doi: 10.3866/PKU.WHXB202202001
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摘要:

编委会

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《物理化学学报》第4届编委会

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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

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发布时间: 2018-05-02


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发布日期:2009-06-24 浏览: