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

SCIENCE BULLETIN 2024年第18期69卷 2881-2891页

作者： Fan, Qikui Yan, Pengxu Liu, Fuzhu Xu, Zhongshuang Liang, Pengfei Cao, Xi Ye, Chenliang Liu, Moxuan Zhao, Lingyi Ren, Shan Miao, Huanran Zhang, Xiai Yang, Zhimao Ding, Xiangdong Yang, Jian Kong, Chuncai Wu, Yuen Xi An Jiao Tong Univ Sch Phys MOE Key Lab Nonequilibrium Synth & Modulat Condens Key Lab Adv Mat & Mesoscop Phys Shaanxi Prov Xian 710049 Peoples R China Xi An Jiao Tong Univ State Key Lab Mech Behav Mat Xian 710049 Peoples R China Anhui Normal Univ Coll Chem & Mat Sci Wuhu 241002 Peoples R China North China Elect Power Univ Dept Power Engn Beijing 102206 Peoples R China Xian Univ Sci & Technol Coll Chem & Chem Engn Xian 710054 Peoples R China Chinese Acad Sci Shenzhen Inst Adv Technol Ctr Mat & Interfaces Shenzhen 518055 Peoples R China Univ Sci & Technol China Collaborat Innovat Ctr Chem Energy Mat iChEM Sch Chem & Mat Sci Hefei Natl Lab Phys Sci Microscale Hefei 230026 Peoples R China Univ Sci & Technol China Natl Synchrotron Radiat Lab Hefei 230026 Peoples R China

Elastic strain in Cu catalysts enhances their selectivity for the electrochemical CO2 reduction reaction (eCO(2)RR), 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/cm(2) and Faradaic efficiency exceeding 80% were realized for the C2+ products. The selectivity 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 (KH2O) on the compressively strained Cu catalysts, consistent with molecular dynamics simulations and density functional theory calculations. Finite element method simulations confirmed that reducing the coverage of coordinated KH2O 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 strategies for Cu catalysts used in the eCO(2)RR. (c) 2024 Science China Press. Published by Elsevier B.V. and Science China Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.

关键词： Strain effect CO2 electroreduction to C2+ Catalytic selectivity Copper catalyst Water coverage spectroscopy reveals CARBON-MONOXIDE COPPER SELECTIVITY ETHYLENE OPERANDO

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