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pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper

Author

Listed:
  • Xinyan Liu

    (Stanford University
    SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory)

  • Philomena Schlexer

    (Stanford University
    SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory)

  • Jianping Xiao

    (Stanford University
    Westlake University)

  • Yongfei Ji

    (Stanford University
    SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
    Guangzhou University)

  • Lei Wang

    (Stanford University
    SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory)

  • Robert B. Sandberg

    (Stanford University
    SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory)

  • Michael Tang

    (Stanford University
    SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory)

  • Kristopher S. Brown

    (Stanford University
    SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory)

  • Hongjie Peng

    (Stanford University
    SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory)

  • Stefan Ringe

    (Stanford University
    SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory)

  • Christopher Hahn

    (SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory)

  • Thomas F. Jaramillo

    (Stanford University
    SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory)

  • Jens K. Nørskov

    (Stanford University
    SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
    Technical University of Denmark)

  • Karen Chan

    (SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
    Technical University of Denmark)

Abstract

We present a microkinetic model for CO(2) reduction (CO(2)R) on Cu(211) towards C2 products, based on energetics estimated from an explicit solvent model. We show that the differences in both Tafel slopes and pH dependence for C1 vs C2 activity arise from differences in their multi-step mechanisms. We find the depletion in C2 products observed at high overpotential and high pH to arise from the 2nd order dependence of C-C coupling on CO coverage, which decreases due to competition from the C1 pathway. We further demonstrate that CO(2) reduction at a fixed pH yield similar activities, due to the facile kinetics for CO2 reduction to CO on Cu, which suggests C2 products to be favored for CO2R under alkaline conditions. The mechanistic insights of this work elucidate how reaction conditions can lead to significant enhancements in selectivity and activity towards higher value C2 products.

Suggested Citation

  • Xinyan Liu & Philomena Schlexer & Jianping Xiao & Yongfei Ji & Lei Wang & Robert B. Sandberg & Michael Tang & Kristopher S. Brown & Hongjie Peng & Stefan Ringe & Christopher Hahn & Thomas F. Jaramillo, 2019. "pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-018-07970-9
    DOI: 10.1038/s41467-018-07970-9
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    Cited by:

    1. Cheng Du & Joel P. Mills & Asfaw G. Yohannes & Wei Wei & Lei Wang & Siyan Lu & Jian-Xiang Lian & Maoyu Wang & Tao Guo & Xiyang Wang & Hua Zhou & Cheng-Jun Sun & John Z. Wen & Brian Kendall & Martin Co, 2023. "Cascade electrocatalysis via AgCu single-atom alloy and Ag nanoparticles in CO2 electroreduction toward multicarbon products," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Sung-Fu Hung & Aoni Xu & Xue Wang & Fengwang Li & Shao-Hui Hsu & Yuhang Li & Joshua Wicks & Eduardo González Cervantes & Armin Sedighian Rasouli & Yuguang C. Li & Mingchuan Luo & Dae-Hyun Nam & Ning W, 2022. "A metal-supported single-atom catalytic site enables carbon dioxide hydrogenation," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    3. Zheng Chen & Zhangyun Liu & Xin Xu, 2023. "Accurate descriptions of molecule-surface interactions in electrocatalytic CO2 reduction on the copper surfaces," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    4. Ke Ye & Tian-Wen Jiang & Hyun Dong Jung & Peng Shen & So Min Jang & Zhe Weng & Seoin Back & Wen-Bin Cai & Kun Jiang, 2024. "Molecular level insights on the pulsed electrochemical CO2 reduction," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    5. Jing Li & Haocheng Xiong & Xiaozhi Liu & Donghuan Wu & Dong Su & Bingjun Xu & Qi Lu, 2023. "Weak CO binding sites induced by Cu–Ag interfaces promote CO electroreduction to multi-carbon liquid products," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    6. Stefan Ringe, 2023. "The importance of a charge transfer descriptor for screening potential CO2 reduction electrocatalysts," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    7. Hong-Jie Peng & Michael T. Tang & Joakim Halldin Stenlid & Xinyan Liu & Frank Abild-Pedersen, 2022. "Trends in oxygenate/hydrocarbon selectivity for electrochemical CO(2) reduction to C2 products," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    8. Jiajie Hou & Bingjun Xu & Qi Lu, 2024. "Influence of electric double layer rigidity on CO adsorption and electroreduction rate," Nature Communications, Nature, vol. 15(1), pages 1-10, December.

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