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Transplanting Gold Active Sites into Non-Precious-Metal Nanoclusters for Efficient CO2-to-CO Electroreduction

  • Hoeun Seong
    Hoeun Seong
    Department of Chemistry, Yonsei University, Seoul 03722, Republic of Korea
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  • Yongsung Jo
    Yongsung Jo
    Department of Chemistry, Yonsei University, Seoul 03722, Republic of Korea
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  • Vladimir Efremov
    Vladimir Efremov
    Department of Chemical Engineering, University of Seoul, Seoul 02504, Republic of Korea
  • Yujin Kim
    Yujin Kim
    Department of Chemistry, Pohang University of Science and Technology (POSTECH), Pohang 37673, Republic of Korea
    More by Yujin Kim
  • Sojung Park
    Sojung Park
    Department of Energy Engineering/KENTECH Institute for Environmental and Climate Technology, Korea Institute of Energy Technology (KENTECH), Naju 58330, Republic of Korea
    More by Sojung Park
  • Sang Myeong Han
    Sang Myeong Han
    Department of Chemistry, Yonsei University, Seoul 03722, Republic of Korea
  • Kiyoung Chang
    Kiyoung Chang
    Department of Chemistry, Yonsei University, Seoul 03722, Republic of Korea
  • Jiwoo Park
    Jiwoo Park
    Department of Chemistry, Yonsei University, Seoul 03722, Republic of Korea
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  • Woojun Choi
    Woojun Choi
    Department of Chemistry and Medical Chemistry, Yonsei University, Wonju, Gangwon 26493, Republic of Korea
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  • Wooyul Kim*
    Wooyul Kim
    Department of Energy Engineering/KENTECH Institute for Environmental and Climate Technology, Korea Institute of Energy Technology (KENTECH), Naju 58330, Republic of Korea
    *Email: [email protected]
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  • Chang Hyuck Choi*
    Chang Hyuck Choi
    Department of Chemistry, Pohang University of Science and Technology (POSTECH), Pohang 37673, Republic of Korea
    *Email: [email protected]
  • Jong Suk Yoo*
    Jong Suk Yoo
    Department of Chemical Engineering, University of Seoul, Seoul 02504, Republic of Korea
    *Email: [email protected]
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  • , and 
  • Dongil Lee*
    Dongil Lee
    Department of Chemistry, Yonsei University, Seoul 03722, Republic of Korea
    *Email: [email protected]
    More by Dongil Lee
Cite this: J. Am. Chem. Soc. 2023, 145, 4, 2152–2160
Publication Date (Web):January 19, 2023
https://doi.org/10.1021/jacs.2c09170
Copyright © 2023 American Chemical Society

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    Abstract

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    Electrocatalytic CO2 reduction reaction (CO2RR) is greatly facilitated by Au surfaces. However, large fractions of underlying Au atoms are generally unused during the catalytic reaction, which limits mass activity. Herein, we report a strategy for preparing efficient electrocatalysts with high mass activities by the atomic-level transplantation of Au active sites into a Ni4 nanocluster (NC). While the Ni4 NC exclusively produces H2, the Au-transplanted NC selectively produces CO over H2. The origin of the contrasting selectivity observed for this NC is investigated by combining operando and theoretical studies, which reveal that while the Ni sites are almost completely blocked by the CO intermediate in both NCs, the Au sites act as active sites for CO2-to-CO electroreduction. The Au-transplanted NC exhibits a remarkable turnover frequency and mass activity for CO production (206 molCO/molNC/s and 25,228 A/gAu, respectively, at an overpotential of 0.32 V) and high durability toward the CO2RR over 25 h.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.2c09170.

    • Experimental and computational methods, photographic images, TEM images, XPS data, mass spectrum, EXAFS spectra, cell configurations, electrochemical data, DFT calculations, and crystallographic data (Figures S1–S22 and Tables S1–S5) and X-ray crystallographic data for Ni4(SEtPh)8 and Au4Ni2(SEtPh)8 (CCDC 2178719 and 2114549, respectively) (PDF)

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    CCDC 2114549 and 2178719 contain the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk/data_request/cif, or by emailing [email protected], or by contacting The Cambridge Crystallographic Data Centre, 12 Union Road, Cambridge CB2 1EZ, UK; fax: +44 1223 336033.

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    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    This article is cited by 1 publications.

    1. Xu Liu, Xiao Cai, Yan Zhu. Catalysis Synergism by Atomically Precise Bimetallic Nanoclusters Doped with Heteroatoms. Accounts of Chemical Research 2023, 56 (12) , 1528-1538. https://doi.org/10.1021/acs.accounts.3c00118

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