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Chinese Chemical Letters 2024年第10期35卷 152-164页

作者： Qiyan Wu Ruixin Zhou Zhangyi Yao tanyuan wang Qing Li State Key Laboratory of Materials Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology

Water splitting with proton exchange membrane water electrolyzers(PEMWE) is regarded as a promising pathway for sustainable hydrogen conversion. Additionally, oxygen evolution reaction(OER) is considered as the dominant factor during the whole process due to the sluggish kinetics. Among the catalysts, Rubased catalysts draw special attention because of their excellent activity and relatively low price. However, the limited stability impedes their further commercialization and tremendous efforts have been devoted to overcome this challenge. This review firstly introduces the basic mechanisms of OER. Then the evaluation protocols and techniques to investigate the stability of Ru-based catalysts are summarized.A detailed elucidation of the possible degradation mechanisms is also critically analyzed. Furthermore,effective strategies to design durable Ru-based catalysts for acidic OER are discussed. Such as heteroatom doping, phase and facet engineering, heterostructure building and support optimization. Finally, promises,perspectives and challenges in developing highly durable Ru-based catalysts for acidic OER are outlined.

关键词： Acidic oxygen evolution Degradation mechanisms Optimization strategies Ru-based catalysts Stability

Recent progress in C-N coupling for electrochemical CO_(2) reduction with inorganic nitrogenous species in aqueous solution

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Materials Reports(Energy) 2023年第1期3卷 65-77,I0003页

作者： Shuxia Liu tanyuan wang.lior elbaz Qing Li State Key Laboratory of Material Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhanHubei430074China Department of Chemistry and the Institute of Nanotechnology and Advanced Materials Bar-Ilan UniversityRamat-Gan5290002Israel

The electrocatalytic CO_(2) reduction in aqueous solution mainly involves bond cleavage and formation between C,H and O,and it is highly desirable to expand the bond formation reaction of C with other atoms to obtain novel and valuable *** electrochemical synthesis of N-containing organic chemicals in electrocatalytic CO_(2) reduction via introducing N sources is an effective strategy to expand the product scope,since chemicals con-taining C–N bonds(*** and amines)are important reactants/products for medicine,agriculture and *** article focuses on the research progress of C–N coupling from CO_(2) and inorganic nitrogenous species in aqueous ***,the reaction pathways related to the reaction intermediates for urea,formamide,acetamide,methylamine and ethylamine are ***,the electrocatalytic performance of different catalysts for these several N-containing products are summarized and ***,the challenges and op-portunities are analyzed,aiming to provide general insights into future research directions for electrocatalytic C–N coupling.

关键词： CO_(2) reduction C-N coupling Heterogeneous electrocatalysis Amide Amine

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非金属掺杂提升铂族金属电催化剂性能

Chinese Journal of Catalysis 2024年第1期56卷 51-73页

作者：李伊萍王谭源姚璋懿陈麒安李箐华中科技大学材料科学与工程学院材料成形与模具技术国家重点实验室湖北武汉430074

铂族金属(PGM)催化剂被认为是用于能量转换和存储设备(如燃料电池和水电解器)的最佳催化剂之一,但活性和稳定性不足极大地限制了其商业化应用.近年来,非金属原子(氢、硼、碳、氮、磷和硫等)掺杂策略引起了广泛关注,该方法可以对铂族金... 详细信息

铂族金属(PGM)催化剂被认为是用于能量转换和存储设备(如燃料电池和水电解器)的最佳催化剂之一,但活性和稳定性不足极大地限制了其商业化应用.近年来,非金属原子(氢、硼、碳、氮、磷和硫等)掺杂策略引起了广泛关注,该方法可以对铂族金属的精细电子和配位结构进行调控,从而优化铂族金属的电催化活性和稳定性.非金属掺杂具有独特的优势:首先,非金属的原子半径较小,可以进入铂族金属的间隙位点,为调节铂族金属的电子结构提供了更多的可能性;其次,掺杂的非金属会诱导强电荷转移,并与主体金属产生s,p-d杂化,这与金属-金属合金中的d-d轨道耦合不同;第三,非金属掺杂的铂族金属基催化剂由于具有较强的非金属-金属键,从而表现出较好的耐久性.本文详细探讨了非金属掺杂铂族金属催化剂的合成和应用,并揭示了非金属掺杂的催化机理和构效关系.本文总结了非金属掺杂铂族金属基催化剂在电催化领域的一些代表性进展,讨论了影响催化剂活性和稳定性的关键因素,并介绍了非金属掺杂改善铂族金属基催化剂性能的基本原理.探讨了非金属掺杂铂族金属基催化剂的表征技术和理论方法,其中包括可直接观测到非金属原子的先进成像技术以及原位表征方法,辅助以密度泛函理论以及分子动力学模拟等理论计算方法,以进一步揭示催化剂性能增强机制.详细列举了非金属掺杂铂族电催化剂的合成方法,从气相沉积、高温热解、湿化学合成到电化学原位合成,提供了详尽的合成方案,并提出了针对贵金属活性中心的非金属修饰策略,旨在为未来材料设计提供启示.概述了非金属掺杂铂族金属基催化剂在电催化中的应用,重点揭示了非金属掺杂带来的结构-性能构效关系.在活性方面,非金属掺杂可以从配体效应、应力效应、微应变等方面影响铂族金属的d带重心,从而影响活性位点与反应中间体的吸附,而这种影响作用也因每种非金属的电负性、原子半径、掺杂方式等不同而不同,可通过调控掺杂种类/方式实现精细调控;同时,非贵金属的协同效应可以增强对OH的吸附,抑制活性位点的毒化.在稳定性方面,非金属可以通过与金属形成稳定的金属-非金属键抑制金属的溶解,或者减弱金属与氧的相互作用,防止其被氧化;同时,非金属的掺入可以提高金属的功函数,提高其溶解电位,从而提升催化剂稳定性.最后,本文提出了该类电催化材料面临的机遇和挑战,其中包括:(1)开发更加可控的非金属掺杂策略;(2)更加深入地研究非金属掺杂带来的构效关系;(3)探索新的非金属掺杂催化剂,并进一步拓展到其他催化领域;(4)发展抑制非金属组分溶解的通用策略;(5)重视催化剂在器件层面的性能评估.综上,本文不仅为非金属掺杂贵金属基催化剂进一步的研究提供启示,还为深入理解催化、纳米材料的合成提供参考.

关键词：电催化非金属掺杂铂族金属基催化剂氧还原氢析出

Tuning metal-support interaction of Pt-based electrocatalysts for hydrogen energy conversion

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Science China Chemistry 2023年第12期66卷 3398-3414页

作者： Shenzhou Li tanyuan wang Qing Li State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China Shenzhen Huazhong University of Science and Technology Research Institute Shenzhen 518000China

Pt-based electrocatalysts hold great promise for key electrocatalytic reactions in hydrogen-related energy conversion ***,the catalytic performance is significantly influenced by metal-support interactions(MSI)in the catalysts,making the tuning of MSI in Pt-based catalysts a highly intriguing research *** this review,the catalytic mechanism of Pt-based electrocatalysts is firstly ***,the effects of MSI on supported Pt electrocatalysts are summarized into four types:geometric effects,electronic effects,synergistic effects,and structural ***,the prospect of optimizing the performance of Pt-based electrocatalysts by engineering MSI is exhibited,with the aim of inspiring innovation and advancement of supported Pt catalysts,thereby facilitating the development and utilization of hydrogen energy.

关键词： metal-support interaction Pt-based catalysts electrocatalysis hydrogen evolution reaction oxygen reduction reaction

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Design of advanced aerogel structures for oxygen reduction reaction electrocatalysis

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SusMat 2023年第1期3卷 44-57页

作者： Leigh Peles-Strahl Yeela Persky lior elbaz Department of Chemistry Bar-Ilan UniversityRamat-GanIsrael Soreq NRC YavneIsrael

Oxygen reduction reaction(ORR)is considered the bottleneck reaction in fuel *** sluggish kinetics requires the use of scarce and expensive platinum group metal(PGM)*** efforts have been invested in trying to find a PGM-free catalyst to replace Pt for this reaction or reduce its *** interesting family of materials that has shown great promise in doing so is aerogels,which are based on covalent *** aerogels’high surface area and porosity enable good mass transport and high catalyst utilization that is expected to lower PGM loadings or replacing them *** review summarizes recent research in this field,introducing methods of using aerogels as cathodes for ORR,from carbon to metal *** catalytic sites vary from nanoparticles to atomically dispersed metal ions embedded in carbon aerogels that form all-in-one platform which can serve as both the support and the catalyst.

关键词： aerogels catalyst supports electrocatalysis fuel cells oxygen reduction reaction

Energy storage materials derived from Prussian blue analogues

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Science Bulletin 2017年第5期62卷 358-368页

作者： Feng Ma Qing Li tanyuan wang Hanguang Zhang Gang Wu State Key Laboratory of Material Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan 430074 China Department of Chemical and Biological Engineering University at Buffalo The State University of New York Buffalo NY 14260 USA

Prussian blue analogues(PBAs) with open frameworks have drawn much attention in energy storage fields due to their tridimensional ionic diffusion path, easy preparation, and low cost. This review summarizes the recent progress of using PBAs and their derivatives as energy storage materials in alkali ions,multi-valent ions, and metal-air batteries. The key factors to improve the electrochemical performance of PBAs as cathode materials in rechargeable batteries were firstly discussed. Several approaches for performance enhancement such as controlling the amounts of vacancies and coordinated water, optimizing morphologies, and depositing carbon coating are described in details. Then, we highlighted the significance of their diverse architectures and morphologies in anode materials for lithium/sodium ion batteries. Finally, the applications of Prussian blue derivatives as catalysts in metal-air batteries are also reviewed, providing insights into the origin of favorable morphologies and structures of catalyst for the optimal performance.

关键词： Prussian blue analogues Energy storage Rechargeable battery Open frameworks Cathode materials Anode materials Catalysts

Molybdenum disulfide as hydrogen evolution catalyst:From atomistic to materials structure and electrocatalytic performance

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Journal of Energy Chemistry 2023年第12期87卷 256-285,I0007页

作者： Mohsin Muhyuddin Giorgio Tseberlidis Maurizio Filippo Acciarri Oran Lori Massimiliano D'Arienzo Massimiliano Cavallini Plamen Atanassov lior elbaz Alessandro Lavacchi Carlo Santoro Department of Materials Science University of Milano-BicoccaVia Roberto Cozzi 55Building U520125 MilanItaly Istituto per lo Studio dei Materiali Nanostrutturati (ISMN)Consiglio Nazionale delle Ricerche(CNR)Via P.Gobetti 101BolognaItaly Department of Chemical and Biomolecular Engineering University of CaliforniaIrvineCA 92697United States Department of Chemistry and the Institute of Nanotechnology and Advanced Materials Bar-Ilan UniversityRamat-Gan 5290002Israel Institute of Chemistry of the Organometallic Compounds-National Research Council(ICCOM-CNR) Via Madonna del Piano1050019 Sesto Fiorentino(FI)Italy

Hydrogen production via water electrolysis defines the novel energy vector for achieving a sustainable ***,the true progress of the given technology is hindered by the sluggish and complex hydrogen evolution reaction(HER)occurring at the cathodic side of the system where overpriced and scarce Pt-based electrocatalysts are usually ***,efficient platinum group metals(PGMs)-free electrocatalysts to carry out HER with accelerated kinetics are urgently *** this scenario,molybdenum disulfide(MoS_(2))owing to efficacious structural attributes and optimum hydrogen-binding free energy(ΔG_(H*))is emerging as a reliable alternative to ***,the performance of MoS_(2)-based electrocatalysts is still far away from the benchmark *** HER activity of MoS_(2)can be improved by engineering the structural parameters i.e.,doping,defects inducement,modulating the electronic structure,stabilizing the 1 T phase,creating nanocomposites,and altering the morphologies using appropriate fabrication ***,we have comprehensively reviewed the majority of the scientific endeavors published in recent years to uplift the HER activity of MoS_(2)-based electrocatalysts using different *** in the major fabrication strategies including hydrothermal synthesis methods,chemical vapor deposition,exfoliation techniques,plasma treatments,chemical methodologies,*** tune the structural parameters and hence their ultimate influence on the electrocatalytic activity in acidic and/or alkaline media have been thoroughly *** study can provide encyclopedic insights about the fabrication routes that have been pursued to improve the HER performance of MoS_(2)-based electrocatalysts.

关键词： Hydrogen evolution reaction Molybdenum disulphide Electrocatalysts Synthesis techniques Sustainable energy production Water electrolysis

Tuning the oxygen evolution electrocatalysis on NiFe-layered double hydroxides via sulfur doping

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Chinese Journal of Catalysis 2020年第5期41卷 847-852页

作者： Shenzhou Li Jianyun Liu Shuo Duan tanyuan wang Qing Li State Key Laboratory of Material Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina

We report a facile way to prepare sulfur(S) doped Ni4/5 Fe1/5-layered double hydroxide(LDH) electrocatalysts for oxygen evolution reaction(OER). The influence of S doping amount on the OER activity of the resulted Ni Fe-LDHs was studied and the optimal surface S content was ca. 0.43 at%. The developed S-doped Ni Fe-LDH exhibits excellent OER catalyst activity in 1.0 M KOH with overpotential of only 257 m V at the current density of 10 m A cm^-2. Moreover, the catalyst could maintain high activity after 30 h stability test. The high activity of the S-doped Ni Fe-LDH catalysts may originate from the synergistic effect between S and the Fe sites. This work provides a simple but efficient way to improve the OER performance of transition metal oxides/(oxy)hydroxides.

关键词： Oxygen evolution Electrocatalysis Layered double hydroxides Sulfur doping Water splitting

Molybdenum-doped ordered L1_(0)-PdZn nanosheets for enhanced oxygen reduction electrocatalysis

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SusMat 2022年第3期2卷 347-356页

作者： Jiashun Liang Yu Xia Xuan Liu Fanyang Huang Jinjia Liu Shenzhou Li tanyuan wang Shuhong Jiao Ruiguo Cao Jiantao Han Hsing-Lin wang Qing Li State Key Laboratory of Material Processing and Die and Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhanChina Department of Materials Science and Engineering Southern University of Science and TechnologyShenzhenChina School of Physics and Astronomy University of BirminghamBirminghamUK Key Laboratory of Materials for Energy Conversion Chinese Academy of Science(CAS) Department of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefeiChina Institute of Coal Chemistry Chinese Academy of SciencesTaiyuanChina National Energy Center for Coal to Clean Fuels Synfuels China Co.LtdBeijingChina

Ultrathin Pd-based two-dimensional(2D)nanosheets(NSs)with tunable physicochemical properties have emerged as promising candidate for oxygen reduction reaction(ORR).Unfortunately,structurally ordered Pd-based NSs can be hardly prepared as high temperature annealing(>600℃)is necessary for disorder to order phase transition,making it a considerable challenge for morphology ***,a new class of ultrathin structurally ordered Mo-doped L1_(0)-PdZn NSs with curved geometry and abundant defects/lattice distortions is reported as an efficient oxygen reduction electrocatalyst in alkaline *** is found that Mo(CO)_(6) serves as reducing agent and Mo source to generate the unique ordered 2D morphology,which leads to the significantly modified electronic *** developed L1_(0)-Mo-PdZn NSs exhibit excellent ORR mass activity of 2.6 A mg_(Pd)^(−1) at 0.9 V versus reversible hydrogen electrode,31.5 and 17.6 times higher than those of Pd/C and Pt/C,respectively,outperforming most of the reported Pdbased ORR ***,L1_(0)-Mo-PdZn NSs is extremely stable for ORR,with only 2.3% activity loss after 10000 potential *** functional theory study suggests that ordered L1_(0) structure and Mo doping can raise the vacancy formation energy of Pd atom and thus promote the ORR stability.

关键词： electrocatalysis fuel cell nanosheeets oxygen reduction Pd-based intermetallics

Atomically dispersed Zn-Co-N-C catalyst boosting efficient and robust oxygen reduction catalysis in acid via stabilizing Co-N bonds

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Fundamental Research 2023年第6期3卷 909-917页

作者： Feng Ma Xuan Liu Xiaoming wang Jiashun Liang Jianyu Huang Cameron Priest Jinjia Liu Shuhong Jiao tanyuan wang Gang Wu Yunhui Huang Qing Li State Key Laboratory of Material Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhanHubei 430074China State Key Laboratory of Refractories and Metallurgy Institute of Advanced Materials and NanotechnologyKey Laboratory of Hubei Province for Coal Conversion and New Carbon MaterialsSchool of Chemistry and Chemical EngineeringWuhan University of Science and TechnologyWuhan 430081China Clean Nano Energy Center State Key Laboratory of Metastable Materials Science and TechnologyYanshan UniversityQinhuangdao 066004China Department of Chemical and Biological Engineering University at BuffaloThe State University of New YorkBuffaloNY 14260United States State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China National Energy Center for Coal to Clean Fuels Synfuels China Co.LtdHuairou DistrictBeijing 101400China Department of Materials Science and Engineering Key Laboratory of Materials for Energy Conversion Chinese Academy of Science(CAS)University of Science and Technology of ChinaHefei 230026China Department of Chemistry and Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province Shantou UniversityShantou 515063China

Transition metal supported N-doped carbon(M-N-C)catalysts for oxygen reduction reaction(ORR)are viewed as the promising candidate to replace Pt-group metal(PGM)for proton exchange membrane fuel cells(PEMFCs).However,the stability of M-N-C is extremely challenging due to the demetalation,H_(2)O_(2)attack,*** the strongly oxidative conditions of *** this study,we demonstrate the universal effect of Zn on promoting the stability of atomically dispersed M-Nx/C(M=Co,Fe,Mn)catalysts and the enhancement mechanism is unveiled for the first *** best-performing dual-metal-site Zn-Co-N-C catalyst exhibits a high half-wave potential(E1/2)value of 0.81 V *** hydrogen electrode(RHE)in acid and outstanding durability with no activity decay after 15,000 accelerated degradation test(ADT)cycles at 60℃,surpassing most reported Co-based PGM-free catalysts in acid *** comparison,the Co-N-C in the absence of Zn suffers from a rapid degradation after ADT due to the demetalation and higher H_(2)O_(2)yield.X-ray adsorption spectroscopy(XAS)and density functional theory(DFT)calculations suggest the more negative formation energy(by 1.2 eV)and increased charge transfer of Zn-Co dual-site structure compared to Co-N-C could strength the Co-N bonds against the demetalation and the optimized d-band center accounts for the improved ORR kinetics.

关键词： Electrocatalysis Oxygen reduction reaction Non-noble metal catalysts Metal-nitrogen carbon catalysts Demetalation Structural stability