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Promoting Water Activation via Molecular Engineering Enables Efficient Asymmetric C–C Coupling during CO2 Electroreduction
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    Promoting Water Activation via Molecular Engineering Enables Efficient Asymmetric C–C Coupling during CO2 Electroreduction
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    • Zi-Yu Du
      Zi-Yu Du
      State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, China
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    • Si-Bo Li
      Si-Bo Li
      State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, China
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    • Ge-Hao Liang
      Ge-Hao Liang
      State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, China
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    • Yi-Meng Xie
      Yi-Meng Xie
      State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, China
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    • Yao-Lin A
      Yao-Lin A
      State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, China
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    • Yi Zhang
      Yi Zhang
      State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, China
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    • Hua Zhang*
      Hua Zhang
      State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, China
      *Email: [email protected]
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    • Jing-Hua Tian
      Jing-Hua Tian
      Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Xiamen 361005, China
    • Shisheng Zheng*
      Shisheng Zheng
      State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, China
      *Email: [email protected]
    • Qing-Na Zheng
      Qing-Na Zheng
      State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, China
    • Zhou Chen*
      Zhou Chen
      State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, China
      *Email: [email protected]
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    • Weng Fai Ip
      Weng Fai Ip
      Department of Physics and Chemistry, Faculty of Science and Technology, University of Macau, Macao 999078, China
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    • Jinxuan Liu*
      Jinxuan Liu
      State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian 116024, P. R. China
      Leicester International Institute, Dalian University of Technology, Panjin 124221, P. R. China
      *Email: [email protected]
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    • Jian-Feng Li*
      Jian-Feng Li
      State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, China
      Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Xiamen 361005, China
      College of Chemistry, Chemical Engineering and Environment, Minnan Normal University, Zhangzhou 363000, China
      *Email: [email protected]
      More by Jian-Feng Li
    Other Access OptionsSupporting Information (1)

    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2024, 146, 47, 32870–32879
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    https://doi.org/10.1021/jacs.4c14299
    Published November 13, 2024
    Copyright © 2024 American Chemical Society

    Abstract

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    Water activation plays a crucial role in CO2 reduction, but improving the electrocatalytic performance through controlled water activation presents a significant challenge. Herein, we achieved electrochemical CO2 reduction to ethene and ethanol with high selectivity by promoting water dissociation and asymmetric C–C coupling by engineering Cu surfaces with N–H-rich molecules. Direct spectroscopic evidence, coupled with density functional theory calculations, demonstrates that the N–H-rich molecules accelerate interfacial water dissociation via hydrogen-bond interactions, and the generated hydrogen species facilitate the conversion of *CO to *CHO. This enables the efficient asymmetric *CHO–*CO coupling to C2 products with a faradaic efficiency (FE) ∼ 30% higher than that of the unmodified catalyst. Moreover, by adjustment of the relative *CHO/*CO coverage via Cu surface facet regulation, the selectivity can be entirely switched between C2 products and CH4. These mechanistic insights further guided the development of a more efficient catalyst by directly modifying Cu2O nanocubes with the N–H-rich molecule, achieving remarkable C2 product (mainly ethene and ethanol) FEs of 85.7% at a current density of 800 mA cm–2 and excellent stability under nearing industrial conditions. This study advances our understanding of the CO2 reduction mechanisms and offers an effective and general strategy for enhancing electrocatalytic performance by accelerating water dissociation.

    Copyright © 2024 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.4c14299.

    • Further experimental details; characterization; additional electrochemical data; theoretical simulations results; in situ Raman data including Figures S1–S30 (PDF)

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    This article is cited by 3 publications.

    1. Ze-Xian Chen, Yuan-Jun Song, Ruo-Zhou Li, Si-Jie Guo, Lei Shi, Zong-Ru Yang, Xiao-Mei Xue, Tong Zhang. Advances in copper nanocrystals: Synthesis, anti-oxidation strategies, and multiple applications. Coordination Chemistry Reviews 2025, 529 , 216455. https://doi.org/10.1016/j.ccr.2025.216455
    2. Ruyang Song, Lin Gu, Chuanyue Sun, Huaxing Li, Abdullah N. Alodhayb, Yunyun Dong, Jinsheng Zhao. Towards Efficient Oxygen Reduction Reaction: One-Step Synthesis of Co-N Catalysts with Polyhexamethylene Guanidine as Nitrogen Precursor. Catalysts 2025, 15 (1) , 5. https://doi.org/10.3390/catal15010005
    3. Xiao-Wan Xiong, Xin-Yue Wu, Yuan-Sheng Cheng, Delei Yu, Xu-Dong Xu, Yuwen Cheng, Fang-Hui Wu, Xian-Wen Wei. Construction of stable Cu + /Cu 0 sites at the fullerene/Cu(OH)F interface to boost the electroreduction of CO 2 to C 2+ products. Chemical Communications 2025, 119 https://doi.org/10.1039/D4CC03987D

    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2024, 146, 47, 32870–32879
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.4c14299
    Published November 13, 2024
    Copyright © 2024 American Chemical Society

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