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Nanoscale visualization of hot carrier generation and transfer at non-noble metal and oxide interface

Journal of Materials Science & Technology 2022年第3期98卷 151-159页

作者： Ranveer Singh Qadeer Akbar Sial Seung-ik Han Sanghee Nah Ji-Yong Park Hyungtak Seo Department of Materials Science and Engineering Ajou UniversitySuwon16499Republic of Korea Department of Energy Systems Research Ajou UniversitySuwon16499Republic of Korea Seoul Center Korea Basic Science InstituteSeoul02841Republic of Korea Department of Physics Ajou UniversitySuwon16499Republic of Korea

The conversion efficiency of energy-harvesting devices can be increased by utilizing hot-carriers(HCs).However,due to ultrafast carrier-carrier scattering and the lack of carrier injection dynamics,HC-based devices have low *** the present work,we report the effective utilization of HCs at the nanoscale and their transfer dynamics from a non-noble metal to a metal oxide interface by means of real-space photocurrent mapping by using local probe techniques and conducting femtosecond transient absorption(TA)*** photocurrent maps obtained under white light unambiguously show that the HCs are injected into the metal oxide layer from the TiN layer,as also confirmed by conductive atomic force *** addition,the increased photocurrent in the bilayer structure indicates the injection of HCs from both layers due to the broadband absorption efficiency of TiN layer,passivation of the surface states by the top TiN layer,and smaller barrier height of the ***,electrostatic force microscopy and Kelvin probe force microscopy provide direct evidence of charge injection from TiN to the MoO_(x)film at the *** TA absorption spectra show a strong photo-bleaching signal over wide spectral range and ultrafast decaying behavior at the picosecond time scale,which indicate efficient electron transfer from TiN to MoO_(x).Thus,our simple and effective approach can facilitate HC collection under white light,thereby achieving high conversion efficiency for optoelectronic devices.

关键词： non-noble metal Hot carrier Real-space photocurrent mapping Local-probe force microscopy

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MXene based non-noble metal catalyst for overall water splitting in alkaline conditions

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Journal of Energy Chemistry 2023年第12期87卷 518-539,I0014页

作者： Dezheng Guo Qiwen Pan Thomas Vietor Weijun Lu Yuan Gao Automotive Institute Tongji UniversityShanghai 200000China Institute of Engineering Design Technische Universität BraunschweigBraunschweig 38106Germany

MXene,the two-dimensional transition metal carbide or nitride material,was first discovered in *** possess superior characteristics such as stability,electric conductivity,and electrochemical properties,that make them attract the attention of the energy engineering *** water splitting which generates hydrogen and oxygen,not only serves as a clean energy supply technology but also demonstrates the capacity for redistribution and integration of renewable *** based non-noble metal has demonstrated significant potential in terms of ***,the current focus is implementing targeted regulation at the micro level to render it effective comparable to the precious *** this context,the mechanisms of the hydrogen evolution reaction(HER) and the oxygen evolution reaction(OER) under the influence of MXene can be elucidated in terms of electron and ion transfer processes,hydrogen coverage,and regulation of terminal ***,the composition,structure,synthesis,and stability strategies of MXene are the subjects of comprehensive investigation from both theoretical calculations using density functional theory(DFT) and experimental *** addition,this review provides a comprehensive summary of MXene based non-noble metal and various modification *** methods encompass doping,vacancy engineering,hybrid structures,heterojunction formation,multi-scale engineering,surface engineering,and phase *** review also presents suggestions for designing high-performance MXene based on non-noble *** offers guidance on employing construction strategies for *** leveraging the unique properties and tunability of MXene and implementing these modification methods,researchers can enhance the catalytic activity,stability,selectivity,and efficiency of MXene based non-noble metal catalysts.

关键词： MXene Overall water splitting non-noble metal

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non‑noble metal Electrocatalysts for the Hydrogen Evolution Reaction in Water Electrolysis

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Electrochemical Energy Reviews 2021年第3期4卷 473-507页

作者： Huimin Wu Chuanqi Feng Lei Zhang Jiujun Zhang David P.Wilkinson Ministry‑of‑Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules College of Chemistry and Chemical EngineeringKey Laboratory of Regional Development and Environmental Response in Hubei ProvinceFaculty of Resources and Environmental ScienceHubei UniversityWuhan 430062HubeiChina Energy Mining and EnvironmentNational Research Council of CanadaVancouverBC V6T 1W5Canada Department of Chemical and Biochemical Engineering University of British ColumbiaVancouverBC V6T 1W5Canada College of Sciences Institute for Sustainable EnergyShanghai UniversityShanghai 200444China

Water electrolysis is a sustainable approach for hydrogen production by using electricity from clean energy ***,both the hydrogen evolution reaction(HER)and the oxygen evolution reaction(OER)associated with water electrolysis are kinetically sluggish,leading to low efficiency in corresponding electrolysis *** addition,current electrocatalysts that can catalyze both HER and OER to practical rates require noble metals such as platinum that are low in abundance and high in price,severely limiting *** a result,the development of high-performance and cost-effective non-noble metal electrocatalysts to replace noble ones has *** on this,this review will comprehensively present recent research in the design,synthesis,characterization and performance validation/optimization of non-noble metal HER electrocatalysts and analyze corresponding catalytic ***,several important types of non-noble metal electrocatalysts including zero-dimensional,one-dimensional,two-dimensional and three-dimensional materials are presented with an emphasis on morphology/structure,synergetic interaction between metal and support,catalytic property and HER activity/***,existing technical challenges are summarized and corresponding research directions are proposed toward practical application.

关键词： Water electrolysis non-noble metal Electrocatalysts Hydrogen evolution reaction Multidimensional material

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Recent Advances on MOF Derivatives for non-noble metal Oxygen Electrocatalysts in Zinc-Air Batteries

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Nano-Micro Letters 2021年第9期13卷 164-192页

作者： Yuting Zhu Kaihang Yue Chenfeng Xia Shahid Zaman Huan Yang Xianying Wang Ya Yan Bao Yu Xia School of Materials Science&Engineering University of Shanghai for Science and Technology516 Jungong RoadShanghai 200093People’s Republic of China Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service FailureWuhan National Laboratory for OptoelectronicsSchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)1037 Luoyu RoadWuhan 430074People’s Republic of China CAS Key Laboratory of Materials for Energy Conversion Shanghai Institute of CeramicsChinese Academy of Sciences(SICCAS)Shanghai 200050People’s Republic of China

Oxygen electrocatalysts are of great importance for the air electrode in zinc-air batteries(ZABs).Owing to the high specific surface area,controllable pore size and unsaturated metal active sites,metal-organic frameworks(MOFs)derivatives have been widely studied as oxygen electrocatalysts in *** date,many strategies have been developed to generate efficient oxygen electrocatalysts from MOFs for improving the performance of *** this review,the latest progress of the MOF-derived non-noble metal-oxygen electrocatalysts in ZABs is *** performance of these MOF-derived catalysts toward oxygen reduction,and oxygen evolution reactions is discussed based on the categories of metal-free carbon materials,single-atom catalysts,metal cluster/carbon composites and metal compound/carbon ***,we provide a comprehensive overview on the design strategies of various MOF-derived non-noble metal-oxygen electrocatalysts and their structure-performance ***,the challenges and perspectives are provided for further advancing the MOF-derived oxygen electrocatalysts in ZABs.

关键词： metal-organic framework non-noble metal Oxygen electrocatalysts Air electrode Zinc-air batteries

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Recent advances in carbonized non-noble metal–organic frameworks for electrochemical catalyst of oxygen reduction reaction

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Rare metals 2021年第10期40卷 2657-2689页

作者： Chan Li Dao-Hui Zhao Hua-Li Long Ming Li Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials Ministry-of-Education Key Laboratory for the Synthesis and Application of Organic Functional MoleculesHubei Key Laboratory of Polymer MaterialsCollege of Chemistry and Chemical EngineeringHubei UniversityWuhan 430062China

The non-noble metal oxygen reduction reaction(ORR) catalysts prepared by carbonization of metal–organic framework(MOF) have attracted more and more attentions in the fields of fuel cells and metal-air batteries due to their unique intrinsic advantages such as high catalytic activity, low price, simple synthesis and good adaptability. Different from the study of traditional high active noble metal catalysts, this review systematically summarizes recent developments on non-noble metal(Fe,Co, Cu, Ni, Mn and Mo) ORR catalysts prepared by various MOFs carbonization in different metal centers. The effects of synthesis strategies and pyrolysis conditions on the catalyst properties are discussed. Meanwhile, the key parameters of catalytic performances(including active sites, dispersed state and specific surface area) are discussed and the prospect is presented. It is expected that this review will provide effective guidance for future studies on carbonized non-noble MOFs for ORR electrochemical catalyst.

关键词： non-noble metal MOF Pyrolysis Catalyst ORR

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磷钨酸负载的非贵金属单原子催化剂:乙烯环氧化的理论研究

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Science China Materials 2020年第6期63卷 1003-1014页

作者： Shamraiz Hussain Talib 于小虎于琦 Sambath Baskaran 李隽 Department of Chemistry and Key Laboratory of Organic Optoelectronics&Molecular Engineering of Ministry of Education Tsinghua UniversityBeijing 100084China Shaanxi Key Laboratory of Catalysis and School of Chemical&Environment Sciences Shaanxi University of TechnologyHanzhong 723000China School of Materials Science and Engineering and Institute of Graphene at Shaanxi Key Laboratory of Catalysis Shaanxi University of TechnologyHanzhong 723001China Department of Chemistry Southern University of Science and TechnologyShenzhen 518055China

基于第一性原理,本文系统研究了过渡金属单原子(铁,钴,镍,钌,铑,钯,锇,铱,铂)负载在磷钨酸(PTA)催化剂上的几何和电子结构,并进一步研究了乙烯环氧化在铁单原子催化剂上的可能反应机理.我们发现PTA最可能结合过渡金属单原子的位置是四... 详细信息

基于第一性原理,本文系统研究了过渡金属单原子(铁,钴,镍,钌,铑,钯,锇,铱,铂)负载在磷钨酸(PTA)催化剂上的几何和电子结构,并进一步研究了乙烯环氧化在铁单原子催化剂上的可能反应机理.我们发现PTA最可能结合过渡金属单原子的位置是四配位中空位.乙烯环氧化催化活性的理论计算表明,非贵金属Fe1-PTA具有可观的吸附能,这是引发此催化循环的关键物理量.我们进一步进行了铁单原子和PTA结合的成键分析,发现电荷从铁单原子转移到PTA团簇,并且强烈的Fe–O共价金属-载体相互作用(CMSI)是其高稳定性的基础.在催化剂Fe1-PTA上可能的乙烯环氧化催化机理共包括三步:1)氧气分子通过电荷转移吸附在Fe1-PTA上;2)第一个乙烯分子攻击吸附在Fe1-PTA上的氧气分子,随后形成C2H4O;3)表面吸附的氧原子和第二个乙烯分子生成C2H4O,完成催化循环.本研究发现,Fe1-PTA对于乙烯环氧化主要通过Eley-Rideal机理进行.本工作为发展高效多相非贵金属单原子乙烯环氧化催化剂提供了理论依据.

关键词： single-atom catalyst non-noble metal phosphotungstic acid ethylene epoxidation computational modeling

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Constructing ultrafine monodispersed Co_(2)P/(0.59-Cu_(3)P)on Cu doped CoZn-ZIF derived porous N-doped carbon for highly efficient dehydrogenation of ammonia borane

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Nano Research 2023年第5期16卷 6687-6700页

作者： Yinze Yang Liqing Zhao Xiangyang Gao Yafei Zhao School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Environmental Engineering and Chemistry Luoyang Institute of Science and TechnologyLuoyang 471023China Key Laboratory of Artificial Micro Nano-structures of Ministry of EducationSchool of Physics and TechnologyWuhan UniversityWuhan 430072China

Rational construction of highly dispersed,small size,low cost catalysts for release of hydrogen from ammonia borane(AB)is regarded as a prospective approach for promoting the development of upcoming hydrogen ***,the high price and scarcity of precious metal catalysts impose restrictions on their large-scale *** this end,with the aid of a Cu doped CoZn-zeolitic imidazolate frameworks(ZIFs)template strategy,we successfully construct ultrafine monodispersed Co_(2)P/(0.59-Cu_(3)P)on CoZn-ZIF derived porous N-doped carbon(Co_(2)P/(0.59-Cu_(3)P)-NC)as an efficient non-noble-metal ***,Co and Cu atoms can be geometrically separated to high degree due to the presence of Zn in the CuCoZn-ZIF precursor,evaporation of Zn during pyrolysis can generate porous structure with the framework well *** results show that porous Co_(2)P/(0.59-Cu_(3)P)-NC bimetallic phosphide exhibits large specific surface area,hierarchical pore structure,well-exposed active *** on the kinetics analyses and ion effects,the catalyst has achieved an unprecedentedly high total turnover frequency(TOF)of 798 mol·molcat^(−1)·min^(−1)in 0.4 M NaOH solution at 298 K,which surpasses all the ever-reported transition-metal phosphides catalysts for hydrogen generation from *** and theoretical studies confirm that the highly porous structure of the support,the ultrafine and high dispersion of nanoparticles,the N/P doping and their synergistic effects(e.g.,M-P,M-N,N-C,M-M',M-support)jointly induce strong electron transfer,which can reduce the reaction energy barrier and enhance their interaction with AB,thus correspondingly obtaining excellent catalytic *** mechanism and strategy presented in this work pave an avenue for the design of non-noble metal catalyst for hydrogen energy system.

关键词： non-noble metal transition-metal phosphides porous N-doped carbon hydrogen evolution ammonia borane catalytic hydrolysis

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Interfacial coupling of sea urchin-like(Mo4O11-MoS2-VO_(2)) promoted electron redistributions for significantly boosted hydrogen evolution reaction

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Chinese Chemical Letters 2023年第4期34卷 368-373页

作者： Yupeng Xing Na Li Shipeng Qiu Gang Zhao Shuhua Hao Baojie Zhang Laboratory of Functional Micro-nano Materials and Devices School of Physics and TechnologyUniversity of JinanJi’nan 250022China

Developing efficient electrocatalysts for hydrogen evolution reaction(HER) is of great importance in contemporary water electrolysis technology. Here, a novel hierarchically sea urchin-like electrocatalyst(Mo_(4)O_(11)-MoS_(2)-VO_(2)) is synthesized by hydrothermal deposition and post-annealing strategy. The optimized electrocatalyst behaves as a high active hydrogen evolution electrode in 0.5 mol/L H_(2)SO_(4). This electrode needs overpotential of only 43 m V to achieve 10 m A/cm^(2)with a Tafel slope of 37 m V/dec and maintains its catalytic activity for at least 36 h. Better than most previously reported non-noble metal electrocatalysts anchored on carbon cloth. It is worth mentioning that the hierarchical sea urchin-like structure promotes the redistribution of electrons and provides more catalytic active sites. This strategy shows a way for the construction of inexpensive non-noble metal electrocatalysts in the future.

关键词： non-noble metal Hierarchical sea urchin-like (Mo4O11-MoS2-VO_(2)) Interfacial coupling Electron redistribution HER

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Electrosynthesis of Co3O4 and Co（OH）2 ultrathin nanosheet arrays for efficient electrocatalytic water splitting in alkaline and neutral media

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Nano Research 2018年第1期11卷 323-333页

作者： Lin Zhang Bingrui Liu Ning Zhang Mingming Ma CAS Key Laboratory of Soft Matter Chemistry iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Department of Chemistry University of Science and Technology of China Hefei 230026 China Department of Biology and Environmental Engineering Hefei University Hefei230022 China

The dimensional confinement endows ultrathin nanosheets with unique physical and chemical properties, which have been widely studied for the purpose of developing active electrocatalysts for water splitting. Ultrathin nanosheets are generally synthesized by chemical vapor deposition, exfoliation, or surfactant- assisted synthesis, which either require special equipment and reaction conditions, or is limited by the low yields and the difficulty in controlling the lateral size and structure of the nanosheets. In addition, achieving a high loading of ultrathin nanosheets on the electrodes without compromising their catalytic activity still remains a challenge. Herein, we report a simple electrodeposition method for preparing C0304 and Co（OH）2 ultrathin nanosheet arrays （UNA） without using templates or surfactants. The obtained arrays exhibit high activity for oxygen and hydrogen evolution reactions, in both alkaline and neutral media. The electrolyzer based on Co304 and Co（OH）2 UNA shows superior activity and stability than that based on IrO2 and Pt/C, which demonstrates the potential of the present electrodeposition method for developing active and stable electrocatalysts for water splitting.

关键词： electrosynthesis water splitting electrocatalysts non-noble metal ultrathin nanosheets

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Single copper sites dispersed on hierarchically porous carbon for improving oxygen reduction reaction towards zinc-air battery

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Nano Research 2021年第4期14卷 998-1003页

作者： Wenjie Wu Yan Liu Dong Liu Wenxing Chen Zhaoyi Song Ximin Wang Yamin Zheng Ning Lu Chunxia Wang Junjie Mao Yadong Li State Key Laboratory of Heavy Oil Processing College of New Energy and MaterialsChina University of PetroleumBeijing 102249China Key Laboratory of Functional Molecular Solids Ministry of EducationAnhui Province Key Laboratory of Optoelectric Materials Science and Technology and Anhui Laboratory of Molecule-Based MaterialsAnhui Normal UniversityWuhu 241002China State key Lab of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Department of Chemistry Tsinghua UniversityBeijing 100084China

The demand for high-performance non-precious-metal electrocatalysts to replace the noble metal-based catalysts for oxygen reduction reaction(ORR)is intensively ***,single-atomic copper sites supported on N-doped three-dimensional hierarchically porous carbon catalyst(Cu_(1)/NC)was prepared by coordination pyrolysis ***,the Cu_(1)/NC-900 catalyst not only exhibits excellent ORR performance with a half-wave potential of 0.894 V(***)in alkaline media,outperforming those of commercial Pt/C(0.851 V)and Cu nanoparticles anchored on N-doped porous carbon(CuNPs/NC-900),but also demonstrates high stability and methanol ***,the Cu_(1)/NC-900 based Zn-air battery exhibits higher power density,rechargeability and cyclic stability than the one based on Pt/*** experimental and theoretical investigations demonstrated that the excellent performance of the as-obtained Cu_(1)/NC-900 could be attributed to the synergistic effect between copper coordinated by three N atoms active sites and the neighbouring carbon defect,resulting in elevated Cu d-band centers of Cu atoms and facilitating intermediate desorption for ORR *** study may lead towards the development of highly efficient non-noble metal catalysts for applications in electrochemical energy conversion.

关键词： single atomic sites catalysts nitrogen-doped carbon materials oxygen reduction reaction carbon defect non-noble metal

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