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Amorphous MoS_(3) enriched with sulfur vacancies for efficient electrocatalytic nitrogen reduction

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Journal of Energy Chemistry 2021年第2期30卷 132-138,I0005页

作者： Ke Chu Haifeng Nan Qingqing Li Yali Guo YeTian Wuming Liu School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070GansuChina Department of Physics College of ScienceHebei North UniversityZhangjiakou 075000HebeiChina Institute of Physics Chinese Academy of SciencesBeijing 100190China

Developing low-priced,yet effective and robust catalysts for the nitrogen reduction reaction(NRR) is of vital importance for scalable and renewable electrochemical NH3 ***,we provide the first demonstration of MoS_3 as an efficient and durable NRR catalyst in neutral *** prepared amorphous MoS_3 naturally possessed enriched S vacancies and delivered an NH3 yield of 51.7 μg h^(-1) mg^(-1)and a Faradaic efficiency of 12.8% at-0.3 V(RHE) in 0.5 M LiClO_4,considerably exceeding those of MoS_2 and most reported NRR *** functional theory calculations unraveled that S vacancies involved in MoS_3 played a crucial role in activating the NRR via a consecutive mechanism with a low energetics barrier and simultaneously suppressing the hydrogen evolution reaction.

关键词： Electrocatalytic N_2 reduction Amorphous materials Vacancy N_(2)activation

Amorphization activated FeB_(2) porous nanosheets enable efficient electrocatalytic N_(2) fixation

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Journal of Energy Chemistry 2021年第2期30卷 82-89,I0004页

作者： Ke Chu Weicong Gu Qingqing Li Yaping Liu Ye Tian Wuming Liu School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070GansuChina Department of Physics College of ScienceHebei North UniversityZhangjiakou 075000HebeiChina Institute of Physics Chinese Academy of SciencesBeijing 100190China

Designing active,robust and cost-effective catalysts for the nitrogen reduction reaction(NRR) is of paramount significance for sustainable electrochemical NH3 ***-metal diborides(TMB_2)have been recently theoretically predicted to be a new class of potential NRR catalysts,but direct experimental evidence is still ***,we present the first experimental demonstration that amorphous FeB_2 porous nanosheets(a-FeB_2 PNSs) could be a highly efficient NRR catalyst,which exhibited an NH3 yield of 39.8 μg h^(-1) mg^(-1)(-0.3 V) and a Faradaic efficiency of 16.7%(-0.2 V),significantly outperforming their crystalline counterpart and most of existing NRR ***-principle calculations unveiled that the amorphization could induce the upraised d-band center of a-FeB_2 to boost d-2π~* coupling between the active Fe site and ~*N_2 H intermediate,resulting in enhanced ~*N_2 H stabilization and reduced reaction *** study may facilitate the development and understanding of earth-abundant TMB_2-based catalysts for electrocatalytic N_2 fixation.

关键词： Electrocatalytic nitrogen fixation Transition-metal diborides Amorphization Density functional theory

FeTe_(2) as an earth-abundant metal telluride catalyst for electrocatalytic nitrogen fixation

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Journal of Energy Chemistry 2021年第5期30卷 259-263页

作者： Yali Guo Yonghua Cheng Qingqing Li Ke Chu School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070GansuChina

Design of cost-effective,yet highly active electrocatalysts for nitrogen reduction reaction(NRR)is of vital significance for sustainable electrochemical NH_(3) ***,we have demonstrated,from both computational and experimental perspectives,that FeTe_(2) can be an efficient and durable NRR *** computations unveil that FeTe_(2) possesses abundant surface-terminated and low-coordinate Fe sites that can activate the NRR with a low limiting potential(-0.84 V)and currently impede the competing hydrogen evolution *** a proof-of-concept prototype,we synthesized FeTe_(2) nanoparticles supported on reduced graphene oxide(FeTe_(2)/RGO),which exhibited a high NRR activity with the exceptional combination of NH_(3) yield(39.2 lg h^(-1) mg^(-1))and Faradaic efficiency(18.1%),thus demonstrating the feasibility of using FeTe_(2) and other earth-abundant metal tellurides for electrocatalytic N_(2) fixation.

关键词： Electrocatalytic nitrogen reduction Fe catalysts Tellurides Density functional theory

Zn nanosheets:An earth-abundant metallic catalyst for efficient electrochemical ammonia synthesis

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Journal of Energy Chemistry 2021年第3期30卷 318-322页

作者： Qingqing Li Jing Wang Yonghua Cheng Ke Chu School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070GansuChina

Ammonia(NH_(3)),a critical raw material for various industrial chemicals,is also recognized as a clean and efficient energy carrier for the future energy economy[1].However,the industrial-scale production of NH_(3) strongly relies on the Haber-Bosch process,which involves massive fuel consumption and enormous greenhouse gas emissions[2].Therefore,there is an urgent need to develop sustainable and energy-saving alternative routes for artificial NH3 production.

关键词： Electrocatalytic nitrogen fixation Metallic catalysts Zn nanosheets N2 activation First-principle calculations

High ionic conductive protection layer on Zn metal anode for enhanced aqueous zinc-ion batteries

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Chinese Chemical Letters 2023年第6期34卷 563-566页

作者： Xianyu Liu Qiongqiong Lu Aikai Yang Yitai Qian School of Chemical Engineering Lanzhou City UniversityLanzhou 730070China Leibniz Institute for Solid State and Materials Research(IFW)Dresden e.V. Helmholtzstraβe 2001069 DresdenGermany Materials Synthesis and Processing(IEK-1) Institute of Energy and Climate ResearchForschungszentrum Jülich GmbH52425JülichGermany Hefei National Laboratory for Physical Science at the Microscale Department of Applied ChemistryUniversity of Science and Technology of ChinaHefei 230026China

Aqueous zinc-ion batteries(ZIBs)has been regarded as a promising energy storage system for large-scale application due to the advantages of low cost and high ***,the growth of Zn dendrite,hydrogen evolution and passivation issues induce the poor electrochemical performance of ***,a Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)protection layer with high ionic conductivity of 2.94 m S/cm on Zn metal anode was fabricated by drop casting *** protection layer prevents Zn dendrites formation,hydrogen evolution as well as passivation,and facilitates a fast Zn~(2+)*** a result,the symmetric cells based on NZSP-coated Zn show a stable cycling over 1360 h at 0.5 m A/cm^(2)with 0.5 m Ah/cm^(2) and 1000 h even at a high current density of 5 m A/cm^(2) with 2 m Ah/cm^(2).Moreover,the full cells combined with V_(2)O_(5)-based cathode displays high capacities and high rate *** work offers a facile and effective approach to stabilizing Zn metal anode for enhanced ZIBs.

关键词： Na_(3)Zr_(2)Si_(2)PO_(12) High ionic conductivity Drop casting Surface coating Zinc metal anode Aqueous zinc-ion batteries