科学通报(英文版)2024,Vol.69Issue(18) :2881-2891.DOI:10.1016/j.scib.2024.06.031

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

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
科学通报(英文版)2024,Vol.69Issue(18) :2881-2891.DOI:10.1016/j.scib.2024.06.031

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

Qikui Fan 1Pengxu Yan 1Fuzhu Liu 2Zhongshuang Xu 1Pengfei Liang 1Xi Cao 3Chenliang Ye 4Moxuan Liu 5Lingyi Zhao 1Shan Ren 6Huanran Miao 1Xiai Zhang 1Zhimao Yang 1Xiangdong Ding 2Jian Yang 3Chuncai Kong 1Yuen Wu7
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作者信息

  • 1. 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
  • 2. State-key Laboratory for Mechanical Behavior of Materials,Xi'an Jiaotong University,Xi'an 710049,China
  • 3. College of Chemistry and Materials Science,Anhui Normal University,Wuhu 241002,China
  • 4. Department of Power Engineering,North China Electric Power University,Beijing 102206,China
  • 5. College of Chemistry and Chemical Engineering,Xi'an University of Science and Technology,Xi'an 710054,China
  • 6. Center for Materials and Interfaces,Shenzhen Institutes of Advanced Technology,Chinese Academy of Sciences,Shenzhen 518055,China
  • 7. 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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Abstract

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.

Key words

Strain effect/CO2 electroreduction to C2+/Catalytic selectivity/Copper catalyst/Water coverage

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基金项目

National Natural Science Foundation of China(92266107)

National Natural Science Foundation of China(22101182)

Shccig-Qinling Program(2021JLM-27)

Shaanxi Fundamental Science Research Project in the fields of Mathematics and Physics(22JSQ008)

China Postdoctoral Science Foundation(2022M722506)

Fundamental Research Funds for the Central Universities()

China Manned Space Station Program()

Shenzhen Science and Technology Program(JCYJ20210324095202006)

Shaanxi Province Natural Science Basic Research Program(2024JC-YBQN-0394)

QinChuangYuan Scientist and Engineer Program(2022KXJ-175HZ)

出版年

2024
科学通报(英文版)
中国科学院

科学通报(英文版)

CSTPCD
ISSN:1001-6538
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