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Trace-Level Cobalt Dopants Enhance CO2 Electroreduction and Ethylene Formation on Copper

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    Trace-Level Cobalt Dopants Enhance CO2 Electroreduction and Ethylene Formation on Copper
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    • Beomil Kim
      Beomil Kim
      Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology, 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
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      Orcidhttps://orcid.org/0000-0002-3247-0205
    • Ying Chuan Tan
      Ying Chuan Tan
      Institute of Sustainability for Chemicals, Energy and Environment (ISCE2), A*STAR, 2 Fusionopolis Way, Singapore 138634, Singapore
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      Orcidhttps://orcid.org/0000-0003-3281-0350
    • Yeonkyeong Ryu
      Yeonkyeong Ryu
      Department of Energy Science and Engineering, Daegu Gyeongbuk Institute of Science & Technology (DGIST), Daegu 42988, Republic of Korea
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    • Kyuseon Jang
      Kyuseon Jang
      Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology, 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
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    • Hafiz Ghulam Abbas
      Hafiz Ghulam Abbas
      Department of Chemistry, Korea University, Seoul 02841, Republic of Korea
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    • Taehyeok Kang
      Taehyeok Kang
      Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology, 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
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    • Hyeonuk Choi
      Hyeonuk Choi
      Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology, 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
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    • Kug-Seung Lee
      Kug-Seung Lee
      Pohang Accelerator Laboratory, Pohang University of Science and Technology, Pohang 37673, Republic of Korea
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    • Sojung Park
      Sojung Park
      Department of Energy Engineering, Institute for Environmental and Climate Technology, Korea Institute of Energy Technology (KENTECH), Naju 58330, Republic of Korea
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    • Wooyul Kim
      Wooyul Kim
      Department of Energy Engineering, Institute for Environmental and Climate Technology, Korea Institute of Energy Technology (KENTECH), Naju 58330, Republic of Korea
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      Orcidhttps://orcid.org/0000-0002-8130-5441
    • Pyuck-Pa Choi*
      Pyuck-Pa Choi
      Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology, 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0001-9920-0755
    • Stefan Ringe*
      Stefan Ringe
      Department of Energy Science and Engineering, Daegu Gyeongbuk Institute of Science & Technology (DGIST), Daegu 42988, Republic of Korea
      Department of Chemistry, Korea University, Seoul 02841, Republic of Korea
      *Email: [email protected]
      More by Stefan Ringe
      Orcidhttps://orcid.org/0000-0002-7804-1406
    • Jihun Oh*
      Jihun Oh
      Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology, 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
      *Email: [email protected]
      More by Jihun Oh
      Orcidhttps://orcid.org/0000-0001-6465-6736
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    ACS Energy Letters

    Cite this: ACS Energy Lett. 2023, 8, 8, 3356–3364
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    https://doi.org/10.1021/acsenergylett.3c00418
    Published July 14, 2023
    Copyright © 2023 American Chemical Society
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    Abstract

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    The development of Cu-based catalysts for electrochemical CO2 reduction reaction (CO2RR) with stronger CO-binding elements had been unsuccessful in improving multicarbon production from the CO2RR due to CO-poisoning. Here, we discover that trace doping levels of Co atoms in Cu, termed CoCu single-atom alloy (SAA), achieve up to twice the formation rate of CO as compared to bare Cu and further demonstrate a high jC2H4 of 282 mA cm–2 at −1.01 VRHE in a neutral electrolyte. From DFT calculations, Cu sites neighboring CO-poisoned Co atomic sites accelerate CO2-to-CO conversion and enhance the coverage of *CO intermediates required for the formation of multicarbon products. Furthermore, CoCu SAA also exhibits active sites that favor the deoxygenation of *HOCCH, which increases the selectivity toward ethylene over ethanol. Ultimately, CoCu SAA can simultaneously boost the formation of *CO intermediates and modulate the selectivity toward ethylene, resulting in one of the highest ethylene yields of 15.6%.

    Copyright © 2023 American Chemical Society

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    • Experimental details, characterization of catalysts, electrochemical CO2RR measurements, DFT calculations, stability tests (PDF)

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    ACS Energy Letters

    Cite this: ACS Energy Lett. 2023, 8, 8, 3356–3364
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsenergylett.3c00418
    Published July 14, 2023
    Copyright © 2023 American Chemical Society
    Request reuse permissions

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