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石墨炔涂层稳定MOF衍生物Co_(3)S_(4)纳米材料用于高效电催化析氧反应

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Science China Materials 2024年第6期67卷 1882-1890页

作者：陆梦玉赵欣张士福蹇恒欣王梅鲁统部 School of Materials Science and Engineering Tianjin University of TechnologyTianjin 300384China

制备高效的OER电催化剂对水裂解制氢至关重要.具有丰富配位构型的MOFs可以衍生出各种优良的电催化材料.由于石墨炔(GDY)具有独特的可控合成特性,我们将其原位复合在MOF衍生的Co_(3)S_(4)/NF材料上,获得了自支撑电极GDY/Co_(3)S_(4)/NF,... 详细信息

制备高效的OER电催化剂对水裂解制氢至关重要.具有丰富配位构型的MOFs可以衍生出各种优良的电催化材料.由于石墨炔(GDY)具有独特的可控合成特性,我们将其原位复合在MOF衍生的Co_(3)S_(4)/NF材料上,获得了自支撑电极GDY/Co_(3)S_(4)/NF,大大提高了其OER催化性能.研究表明,GDY/Co_(3)S_(4)/NF在10 mA cm^(-2)电流密度下表现出223 mV的低过电位,在100 mA cm^(-2)的大电流密度下,能够稳定电解45小时左右,该材料显示出了巨大的实际应用潜力.结果表明,由于GDY独特的炔键和大孔结构,它可以通过强电子相互作用与Co_(3)S_(4)相互作用,从而调节电子结构并提供有效的电荷转移通道,从而大大提高了其电催化OER的性能.

关键词： GDY cobalt-based sulfides MOF-derived Co_(3)S_(4) electrocatalysis OER

Rare earth alloy nanomaterials in electrocatalysis

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能源化学:英文版 2023年第8期83卷 574-594,I0014页

作者： Yifei Li Xilin Yuan Ping Wang Lulin Tang Miao He Pangen Li Jiang Li Zhenxing Li State Key Laboratory of Heavy Oil Processing College of New Energy and MaterialsChina University of Petroleum(Beijing)Beijing 102249China

With the rapid development of society and economy, the excessive consumption of fossil energy has led to the global energy and environment crisis. In order to explore the sustainable development of new energy, research based on electrocatalysis has attracted extensive attention in the academic circle. The main challenge in this field is to develop nano-catalysts with excellent electrocatalytic activity and selectivity for target products. The state of the active site in catalyst plays a decisive role in the activity and selectivity of the reaction. In order to design efficient and excellent catalysts, it is an effective means to adjust the electronic structure of catalysts. Electronic effects are also called ligand effects. By alloying with rare earth(RE) elements, electrons can be redistributed between RE elements and transition metal elements, achieving accurate design of the electronic structure of the active site in the alloy. Because of the unique electronic structure of RE, it has been paid attention in the field of catalysis. The outermost shell structure of RE elements is basically the same as that of the lower shell, except that the number of electrons in the 4f orbital is different, but the energy level is similar, so their properties are very similar. When RE elements form compounds, both the f electrons in the outermost shell and the d electrons in the lower outer shell can participate in bonding. In addition, part of the 4f electrons in the third outer shell can also participate in bonding.In order to improve the performance of metal catalysts, alloying provides an effective method to design advanced functional materials. RE alloys can integrate the unique electronic structure and catalytic behavior of RE elements into metal materials, which not only provides an opportunity to adjust the electronic structure and catalytic activity of the active component, but also enhances the structural stability of the alloy and is expected to significantly improve the catalytic performance of the catalyst. From th

关键词： Rare earth Alloy nanomaterials electrocatalysis Preparation methods Hydrogen evolution reaction Oxygen reduction reaction Methanol oxidation reaction Ethanol oxidation reaction

Phase engineering activation of low-cost iron-containing sulfide minerals for advanced electrocatalysis

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Journal of Materials Science & Technology 2022年第16期111卷 181-188页

作者： Jun Mei Qian Zhang Hong Peng Ting Liao Ziqi Sun Centre for Materials Science Queensland University of Technology2 George StreetBrisbaneQLD 4000Australia School of Chemistry and Physics Queensland University of Technology2 George StreetBrisbaneQLD 4000Australia College of Materials Science and Engineering Taiyuan University of TechnologyTaiyuan 030024China School of Chemical Engineering The University of QueenslandBrisbaneQLD 4072Australia School of Mechanical Medical and Process Engineering Queensland University of Technology2 George StreetBrisbaneQLD 4000Australia

Sustainable energy conversion and storage provide feasible approaches towards green energy solutions and carbon neutralization.The high cost and complex fabrication process of advanced energy nanomaterials,however,has impeded the practical application of emerging sustainable technologies.The direct use of earth-abundant natural minerals which contain active elements for effective catalysis and energy storage should be a promising approach to achieve affordable sustainable energy supply and green fuel generations.Herein,as typical examples of activating natural minerals for electrocatalysis,two common minerals,pyrite and chalcopyrite,are activated via a one-step phase transformation strategy.Through a facile thermal reduction process,the minerals are completely transformed into active pyrrhotite(FeS)and haycockite(Cu_(4)Fe_(5)S_(8))phases.The thermal reduction resulting phase transformation can lead to significant surface disordering and can contribute to the catalytic activity by offering favourable electronic structure for intermediates adsorption,abundant surficial active centres,and substantial surface redox pairs.The activated minerals are examined for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)catalysis.The obtained haycockite phase delivers the best performance towards acidic HER and alkaline OER.Further phase optimization is performed via loading a low percentage of iridium nanoclusters on the haycockite phase deposited onto a carbon cloth substrate,through which an overpotential as low as 310 mV for achieving 10 mA cmand a small Tafel slope of 55.6 m V dec-1are recorded for alkaline OER.This work demonstrates the feasibility of the direct use of cost-effective natural resources for addressing the current energy-related issues and paves a way to reach affordable practical emerging sustainable technologies.

关键词： Minerals Phase transformation Sulfides Oxygen evolution electrocatalysis

Recent advances of amorphous-phase-engineered metal-based catalysts for boosted electrocatalysis

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Journal of Materials Science & Technology 2022年第32期127卷 1-18页

作者： Jiakang Tian Yongqing Shen Peizhi Liu Haixia Zhang Bingshe Xu Yanhui Song Jianguo Liang Junjie Guo Key Laboratory of Interface Science and Engineering in Advanced Materials Ministry of EducationTaiyuan University of TechnologyTaiyuan 030024China Materials Institute of Atomic and Molecular Science Shaanxi University of Science and TechnologyXi’an 710021China College of Mechanical and Vehicle Engineering Taiyuan University of TechnologyTaiyuan 030024China

Amorphous metal-based catalysts(AMCs)have sparked intense research interests in the field of electrocatalysis elicited by their hallmark features such as unlimited volume and morphology,manipulated electronic structures,enriched defects,and unsaturated surface atom coordination.Nevertheless,the manipulation of the amorphous phase in metal-based catalysts is so far impractical,and thus their electrocatalytic mechanism yet remains ambiguous.In this review,the latest advances in AMCs are systematically reviewed,covering amorphous-phase engineering strategy,structure manipulation,and amorphization of various material categories for electrocatalysis.Specifically,a series of applications of AMCs in electrocatalysis for the oxygen reduction reaction(ORR),hydrogen evolution reaction(HER),and oxygen evolution reaction(OER)are summarized based on the classification criteria of substances.Finally,we put forward current challenges that have not yet been clarified in the field of AMCs,and propose possible solutions,particularly from the perspective of the evolution of electron microscopy.It is expected to promote the understanding of the amorphization-catalysis relationship and provide a guideline for designing high-performance electrocatalysts.

关键词： Amorphous metal-based catalysts electrocatalysis Electron microscopy Interface engineering Surface engineering Defect engineering Strain engineering

Standard-state entropies and their impact on the potential-dependent apparent activation energy in electrocatalysis

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能源化学:英文版 2023年第8期83卷 247-254,I0008页

作者： Kai S.Exner Universty Duisburg-Essen Faculty of ChemstryTheretical Inorganic ChemtryUniversitatsstrae 545141 EssenGemay Cluster of Excellence RESOLV 44801 BochumGermany Center for Nanointegration(CENIDE)Duisburg-Essen 47057 DuisburgGermany

The apparent activation energy,Eapp,is a common measure in thermal catalysis to discuss the activity and limiting steps of catalytic processes on solid-state materials.Recently,the electrocatalysis community adopted the concept of Eappand combined it with the Butler-Volmer theory.Certain observations though,such as potential-dependent fluctuations of Eapp,are yet surprising because they conflict with the proposed linear decrease in Eappwith increasing overpotential.The most common explanation for this finding refers to coverage changes upon alterations in the temperature or the applied electrode potential.In the present contribution,it is demonstrated that the modulation of surface coverages cannot entirely explain potential-dependent oscillations of Eapp,and rather the impact of entropic contributions of the transition states has been overlooked so far.In the case of a nearly constant surface coverage,these entropic contributions can be extracted by a dedicated combination of Tafel plots and temperature-dependent experiments.

关键词： electrocatalysis Standard-state entropy Microkinetic modeling Apparent activation energy Degree of rate control

2D/2D Heterostructures:Rational Design for Advanced Batteries and electrocatalysis

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Energy & Environmental Materials 2022年第1期5卷 115-132页

作者： Jun Mei Ting Liao Ziqi Sun School of Chemistry and Physics Queensland University of Technology2 George StreetBrisbane Qld 4000Australia School of Mechanical Medical and Process Engineering Queensland University of Technology2 George StreetBrisbane Qld 4000Australia Centre for Materials Science Queensland University of Technology2 George StreetBrisbane Qld 4000Australia

Two-dimensional/two-dimensional(2D/2D)heterostructures consisting of two or more 2D building blocks possess intriguing electronic features at the nanosized interfacial regions,endowing the possibility for effectively modulating the confinement,and transport of charge carriers,excitons,photons,phonons,etc.to bring about a wide range of extraordinary physical,chemical,thermal,and/or mechanical properties.By rational design and synthesis of 2D/2D heterostructures,electrochemical properties for advanced batteries and electrocatalysis can be well regulated to meet some practical requirements.In this review,a summary on the commonly employed synthetic strategies for 2D/2D heterostructures is first given,followed by a comprehensive review on recent progress for their applications in batteries and various electrocatalysis reactions.Finally,a critical outlook on the current challenges and promising solutions is presented,which is expected to offer some insightful ideas on the design principles of advanced 2D-based nanomaterials to address the current challenges in sustainable energy storages and green fuel generations.

关键词： 2D heterostructures 2D nanomaterials battery electrocatalysis energy storage

Density Functional Theory for electrocatalysis

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Energy & Environmental Materials 2022年第1期5卷 157-185页

作者： Xiaobin Liao Ruihu Lu Lixue Xia Qian Liu Huan Wang Kristin Zhao Zhaoyang Wang Yan Zhao State Key Laboratory of Silicate Materials for Architectures International School of Materials Science and EngineeringWuhan University of TechnologyWuhan 430070China Zhejiang University Hangzhou 310058China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Center of Smart Materials and DevicesSchool of Materials Science and EngineeringWuhan University of TechnologyWuhan 430070China Lynbrook High School San Jose CA 95129USA The Institute of Technological Sciences Wuhan UniversityWuhan 430072China

It is a considerably promising strategy to produce fuels and high-value chemicals through an electrochemical conversion process in the green and sustainable energy systems.Catalysts for electrocatalytic reactions,including hydrogen evolution reaction(HER),oxygen evolution reaction(OER),oxygen reduction reaction(ORR),nitrogen reduction reaction(NRR),carbon dioxide reduction reaction(CO_(2)RR),play a significant role in the advanced energy conversion technologies,such as water splitting devices,fuel cells,and rechargeable metal-air batteries.Developing low-cost and highly efficient electrocatalysts is closely related to establishing the composition-structure-activity relationships and fundamental understanding of catalytic mechanisms.Density functional theory(DFT)is emerging as an important computational tool that can provide insights into the relationship between the electrochemical performances and physical/chemical properties of catalysts.This article presents a review on the progress of the DFT,and the computational simulations,within the framework of DFT,for the electrocatalytic processes,as well as the computational designs and virtual screenings of new electrocatalysts.Some useful descriptors and analysis tools for evaluating the electrocatalytic performances are highlighted,including formation energies,d-band model,scaling relation,egorbital occupation,and free energies of adsorption.Furthermore,the remaining questions and perspectives for the development of DFT for electrocatalysis are also proposed.

关键词： analysis tools density functional theory descriptors electrocatalysis

Ni单原子负载氮掺杂多孔碳促进锂硫电池中的多硫化物转化

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Science China Materials 2024年第6期67卷 1938-1946页

作者：陈乐园孙焱焱常智柴思敏何琼潘安强 School of Materials Science and Engineering Central South UniversityChangsha 410083China School of Materials Science and Engineering Xinjiang UniversityUrumqi 830046China

由分散在氮掺杂碳载体上的原子级金属位点组成的单原子催化剂(M SAC@NC)因其具有最大的原子利用率、独特的物理化学性质和优异的催化活性,已成为Li-S电池中的高性能电催化材料.本文采用物理吸附和热解相结合的方法,成功制备了一系列具... 详细信息

由分散在氮掺杂碳载体上的原子级金属位点组成的单原子催化剂(M SAC@NC)因其具有最大的原子利用率、独特的物理化学性质和优异的催化活性,已成为Li-S电池中的高性能电催化材料.本文采用物理吸附和热解相结合的方法,成功制备了一系列具有相似结构和理化性质的M SAC@NC(M=Ni,Co,Fe).双球差校正高角环形暗场扫描透射电子显微镜和X射线吸收光谱表明成功形成了单原子金属位点.此外,对硫氧化还原反应的催化活性趋势为Ni SAC@NC>Co SAC@NC>Fe SAC@NC,其中Ni SAC@NC在0.5C下表现出1280.6mAh g^(-1)的最高容量,循环800次后,平均每圈容量衰减率仅为0.07%,具有优异的电池性能.

关键词： single-atomic catalyst electrocatalysis Li-S battery

Noble-metal-based high-entropy-alloy nanoparticles for electrocatalysis

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Journal of Energy Chemistry 2022年第5期31卷 721-751页

作者： Xianfeng Huang Guangxing Yang Shuang Li Hongjuan Wang Yonghai Cao Feng Peng Hao Yu School of Biology and Biological Engineering South China University of TechnologyGuangzhou 510006GuangdongChina School of Chemistry and Chemical Engineering South China University of TechnologyGuangzhou 510641GuangdongChina School of Chemistry and Chemical Engineering Guangzhou UniversityGuangzhou 510006GuangdongChina

Since the two seminal papers were published independently in 2004, high-entropy-alloys(HEAs) have been applied to structural and functional materials due to the enhanced mechanical properties, thermal stability, and electrical conductivity. In recent years, HEA nanoparticles(HEA-NPs) were paid much attention to in the field of catalysis for the promoted catalytic activity. Furthermore, the various ratios among the metal components and tunable bulk and surface structures enable HEAs have big room to enhance the catalytic performance. Especially, noble-metal-based HEAs displayed significantly improved performance in electrocatalysis, where the ‘core effects’ were employed to explain the superior catalytic activity. However, it is insufficient to understand the essential mechanism or further guide the design of electrocatalysts. Structure–property relationship should be disclosed for the catalysis on HEA-NPs to accelerate the process of seeking high effective and efficient electrocatalysts. Therefore, we summarized the recent advances of noble-metal-based HEA-NPs applied to electrocatalysis, such as hydrogen evolution reaction, oxygen evolution reaction, oxygen reduction reaction, methanol oxidation reaction, ethanol oxidation reaction, formic acid oxidation reaction, hydrogen oxidation reaction, carbon dioxide reduction reaction and nitrogen reduction reaction. For each electrocatalytic reaction, the reaction mechanism and catalyst structure were presented, and then the structure–property relationship was elaborated. The review begins with the development, concept, four ‘core effect’ and synthesis methods of HEAs. Next,the electrocatalytic reactions on noble-metal-based HEA-NPs are summarized and discussed independently. Lastly, the main views and difficulties pertaining to structure–property relationship for HEAs are discussed.

关键词： Noble-metal-based High-entropy-alloy Nanoparticles ‘Core effects’ Structure–property relationship electrocatalysis