Compressive strain in Cu catalysts:Enhancing generation of C2+products in electrochemical CO2 reduction

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外文摘要：Elastic strain in Cu catalysts enhances their selectivity for the electrochemical CO2 reduction reaction(eCO2RR),particularly toward the formation of multicarbon(C2+)products.However,the reasons for this selectivity and the effect of catalyst precursors have not yet been clarified.Hence,we employed a redox strategy to induce strain on the surface of Cu nanocrystals.Oxidative transformation was employed to convert Cu nanocrystals to CuxO nanocrystals;these were subsequently electrochemically reduced to form Cu catalysts,while maintaining their compressive strain.Using a flow cell configuration,a current density of 1 A/cm2 and Faradaic efficiency exceeding 80％were realized for the C2+products.The selec-tivity ratio of C2+/C1 was also remarkable at 9.9,surpassing that observed for the Cu catalyst under tensile strain by approximately 7.6 times.In-situ Raman and infrared spectroscopy revealed a decrease in the coverage of K+ion-hydrated water(K·H2O)on the compressively strained Cu catalysts,consistent with molecular dynamics simulations and density functional theory calculations.Finite element method sim-ulations confirmed that reducing the coverage of coordinated K·H2O water increased the probability of intermediate reactants interacting with the surface,thereby promoting efficient C-C coupling and enhancing the yield of C2+products.These findings provide valuable insights into targeted design strate-gies for Cu catalysts used in the eCO2RR.

外文关键词：

Strain effectCO2 electroreduction to C2+Catalytic selectivityCopper catalystWater coverage

作者：

Qikui Fan、Pengxu Yan、Fuzhu Liu、Zhongshuang Xu、Pengfei Liang、Xi Cao、Chenliang Ye、Moxuan Liu、Lingyi Zhao、Shan Ren、Huanran Miao、Xiai Zhang、Zhimao Yang、Xiangdong Ding、Jian Yang、Chuncai Kong、Yuen Wu

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作者单位：

MOE Key Laboratory for Non-Equilibrium Synthesis and Modulation of Condensed Matter,Key Laboratory for Advanced Materials and Mesoscopic Physics of Shaanxi Province,School of Physics,Xi'an Jiaotong University,Xi'an 710049,China

State-key Laboratory for Mechanical Behavior of Materials,Xi'an Jiaotong University,Xi'an 710049,China

College of Chemistry and Materials Science,Anhui Normal University,Wuhu 241002,China

Department of Power Engineering,North China Electric Power University,Beijing 102206,China

College of Chemistry and Chemical Engineering,Xi'an University of Science and Technology,Xi'an 710054,China

Center for Materials and Interfaces,Shenzhen Institutes of Advanced Technology,Chinese Academy of Sciences,Shenzhen 518055,China

Hefei National Laboratory for Physical Sciences at the Microscale,Collaborative Innovation Center of Chemistry for Energy Materials(iChEM),School of Chemistry and Materials Science,and National Synchrotron Radiation Laboratory,University of Science and Technology of China,Hefei 230026,China

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基金：

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaShccig-Qinling ProgramShaanxi Fundamental Science Research Project in the fields of Mathematics and PhysicsChina Postdoctoral Science FoundationFundamental Research Funds for the Central UniversitiesChina Manned Space Station ProgramShenzhen Science and Technology ProgramShaanxi Province Natural Science Basic Research ProgramQinChuangYuan Scientist and Engineer Program

项目编号：

92266107221011822021JLM-2722JSQ0082022M722506JCYJ202103240952020062024JC-YBQN-03942022KXJ-175HZ

出版年：

2024

DOI：

10.1016/j.scib.2024.06.031

科学通报(英文版)

中国科学院

科学通报(英文版)

CSTPCD

ISSN：1001-6538

年,卷(期)：2024.69(18)

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