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Gold Single Atom Doped Defective Nanoporous Copper Octahedrons for Electrocatalytic Reduction of Carbon Dioxide to Ethylene

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    Gold Single Atom Doped Defective Nanoporous Copper Octahedrons for Electrocatalytic Reduction of Carbon Dioxide to Ethylene
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    • Yang Zhao
      Yang Zhao
      Songshan Lake Materials Laboratory (SLAB), Dongguan 523808, P. R. China
      Institute of Physics, Chinese Academy of Sciences, Beijing 100090, P. R. China
      More by Yang Zhao
    • Yanan Wang
      Yanan Wang
      Songshan Lake Materials Laboratory (SLAB), Dongguan 523808, P. R. China
      More by Yanan Wang
      Orcidhttps://orcid.org/0000-0002-8436-0374
    • Zhipeng Yu
      Zhipeng Yu
      Songshan Lake Materials Laboratory (SLAB), Dongguan 523808, P. R. China
      More by Zhipeng Yu
      Orcidhttps://orcid.org/0000-0002-3208-649X
    • Chao Song
      Chao Song
      Songshan Lake Materials Laboratory (SLAB), Dongguan 523808, P. R. China
      More by Chao Song
    • Jingwei Wang
      Jingwei Wang
      Songshan Lake Materials Laboratory (SLAB), Dongguan 523808, P. R. China
      Institute of Physics, Chinese Academy of Sciences, Beijing 100090, P. R. China
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    • Haoliang Huang
      Haoliang Huang
      Songshan Lake Materials Laboratory (SLAB), Dongguan 523808, P. R. China
      More by Haoliang Huang
      Orcidhttps://orcid.org/0000-0002-0993-1536
    • Lijian Meng
      Lijian Meng
      Centre of Innovation in Engineering and Industrial Technology, Instituto Superior de Engenharia do Porto, Instituto Politecnico do Porto, 4249-015 Porto, Portugal
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    • Miao Liu*
      Miao Liu
      Songshan Lake Materials Laboratory (SLAB), Dongguan 523808, P. R. China
      Institute of Physics, Chinese Academy of Sciences, Beijing 100090, P. R. China
      *Email: [email protected]
      More by Miao Liu
    • Lifeng Liu*
      Lifeng Liu
      Songshan Lake Materials Laboratory (SLAB), Dongguan 523808, P. R. China
      *Email: [email protected]
      More by Lifeng Liu
      Orcidhttps://orcid.org/0000-0003-2732-7399
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    ACS Nano

    Cite this: ACS Nano 2025, 19, 4, 4505–4514
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    https://doi.org/10.1021/acsnano.4c13961
    Published January 24, 2025
    Copyright © 2025 American Chemical Society
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    Abstract

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    Electrocatalytic CO2 reduction into high-value multicarbon products offers a sustainable approach to closing the anthropogenic carbon cycle and contributing to carbon neutrality, particularly when renewable electricity is used to power the reaction. However, the lack of efficient and durable electrocatalysts with high selectivity for multicarbons severely hinders the practical application of this promising technology. Herein, a nanoporous defective Au1Cu single-atom alloy (De-Au1Cu SAA) catalyst is developed through facile low-temperature thermal reduction in hydrogen and a subsequent dealloying process, which shows high selectivity toward ethylene (C2H4), with a Faradaic efficiency of 52% at the current density of 252 mA cm–2 under a potential of −1.1 V versus reversible hydrogen electrode (RHE). In situ spectroscopy measurements and density functional theory (DFT) calculations reveal that the high C2H4 product selectivity results from the synergistic effect between Au single atoms and defective Cu sites on the surface of catalysts, where Au single atoms promote *CO generation and Cu defects stabilize the key intermediate *OCCO, which altogether enhances C–C coupling kinetics. This work provides important insights into the catalyst design for electrochemical CO2 reduction to multicarbon products.

    Copyright © 2025 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/acsnano.4c13961.

    • Supplementary methods; SEM image of Cu2O octahedra; XRD and SEM examination results of np-Cu; N2 adsorption/desorption isotherms of samples; Raman spectra and supplementary XAS data of samples; scheme of flow cells; calibration data of GC; Supporting Information of Faradaic efficiencies of various samples; CO2 adsorption data; cyclic voltammetry data; EIS Nyquist plots; SEM, EDS, and TEM data of De-Au1Cu SAA after the stability test; schemes illustrating the configurations of DEMS and ATR-SEIRAS measurements; in situ ATR-SEIRAS spectra of np-Cu; models used for DFT calculations; PDOS of 2*CO-adsorbed surfaces of different samples; tables summarizing the EXAFS fitting, ICP-OES, and EIS fitting data; table comparing the CO2RR performance of SAA catalysts reported in the literature (PDF)

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    This article is cited by 1 publications.

    1. Yanteng Xiao, Fuqing Yu, Chenfeng Xia, Deyu Zhu, Jiwen Chen, Nengji Liu, Yuye Zhao, Ruijuan Qi, Wei Guo, Bo You, Tao Yao, Yuanjie Pang, Ziyun Wang, Hongming Wang, Fei Song, Bao Yu Xia. Asymmetric CO–CHO Coupling over Pr Single-Atom Alloy Enables Industrial-Level Electrosynthesis of Ethylene. Journal of the American Chemical Society 2025, 147 (18) , 15654-15665. https://doi.org/10.1021/jacs.5c02896
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    ACS Nano

    Cite this: ACS Nano 2025, 19, 4, 4505–4514
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.4c13961
    Published January 24, 2025
    Copyright © 2025 American Chemical Society
    Request reuse permissions

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