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Unraveling the rate-determining step of C2+ products during electrochemical CO reduction

Author

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  • Wanyu Deng

    (Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
    International Campus of Tianjin University, Binhai New City
    Technical University of Denmark)

  • Peng Zhang

    (Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
    International Campus of Tianjin University, Binhai New City)

  • Yu Qiao

    (Technical University of Denmark)

  • Georg Kastlunger

    (Technical University of Denmark)

  • Nitish Govindarajan

    (Technical University of Denmark)

  • Aoni Xu

    (Technical University of Denmark)

  • Ib Chorkendorff

    (Technical University of Denmark)

  • Brian Seger

    (Technical University of Denmark)

  • Jinlong Gong

    (Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
    International Campus of Tianjin University, Binhai New City)

Abstract

The electrochemical reduction of CO has drawn a large amount of attention due to its potential to produce sustainable fuels and chemicals by using renewable energy. However, the reaction’s mechanism is not yet well understood. A major debate is whether the rate-determining step for the generation of multi-carbon products is C-C coupling or CO hydrogenation. This paper conducts an experimental analysis of the rate-determining step, exploring pH dependency, kinetic isotope effects, and the impact of CO partial pressure on multi-carbon product activity. Results reveal constant multi-carbon product activity with pH or electrolyte deuteration changes, and CO partial pressure data aligns with the theoretical formula derived from *CO-*CO coupling as the rate-determining step. These findings establish the dimerization of two *CO as the rate-determining step for multi-carbon product formation. Extending the study to commercial copper nanoparticles and oxide-derived copper catalysts shows their rate-determining step also involves *CO-*CO coupling. This investigation provides vital kinetic data and a theoretical foundation for enhancing multi-carbon product production.

Suggested Citation

  • Wanyu Deng & Peng Zhang & Yu Qiao & Georg Kastlunger & Nitish Govindarajan & Aoni Xu & Ib Chorkendorff & Brian Seger & Jinlong Gong, 2024. "Unraveling the rate-determining step of C2+ products during electrochemical CO reduction," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-45230-1
    DOI: 10.1038/s41467-024-45230-1
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    References listed on IDEAS

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    1. Jing Li & Xiaoxia Chang & Haochen Zhang & Arnav S. Malkani & Mu-jeng Cheng & Bingjun Xu & Qi Lu, 2021. "Electrokinetic and in situ spectroscopic investigations of CO electrochemical reduction on copper," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    2. Aditya M. Limaye & Joy S. Zeng & Adam P. Willard & Karthish Manthiram, 2021. "Bayesian data analysis reveals no preference for cardinal Tafel slopes in CO2 reduction electrocatalysis," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    3. Haeun Shin & Kentaro U. Hansen & Feng Jiao, 2021. "Techno-economic assessment of low-temperature carbon dioxide electrolysis," Nature Sustainability, Nature, vol. 4(10), pages 911-919, October.
    4. Wanyu Deng & Peng Zhang & Brian Seger & Jinlong Gong, 2022. "Unraveling the rate-limiting step of two-electron transfer electrochemical reduction of carbon dioxide," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
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