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Coverage enhancement accelerates acidic CO2 electrolysis at ampere-level current with high energy and carbon efficiencies

Author

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  • Xiaohan Yu

    (Nanjing University)

  • Yuting Xu

    (University of Massachusetts Lowell)

  • Le Li

    (Nanjing University)

  • Mingzhe Zhang

    (Nanjing University)

  • Wenhao Qin

    (Nanjing University)

  • Fanglin Che

    (University of Massachusetts Lowell)

  • Miao Zhong

    (Nanjing University)

Abstract

Acidic CO2 electroreduction (CO2R) using renewable electricity holds promise for high-efficiency generation of storable liquid chemicals with up to 100% CO2 utilization. However, the strong parasitic hydrogen evolution reaction (HER) limits its selectivity and energy efficiency (EE), especially at ampere-level current densities. Here we present that enhancing CO2R intermediate coverage on catalysts promotes CO2R and concurrently suppresses HER. We identified and engineered robust Cu6Sn5 catalysts with strong *OCHO affinity and weak *H binding, achieving 91% Faradaic efficiency (FE) for formic acid (FA) production at 1.2 A cm−2 and pH 1. Notably, the single-pass carbon efficiency reaches a new benchmark of 77.4% at 0.5 A cm−2 over 300 hours. In situ electrochemical Fourier-transform infrared spectroscopy revealed Cu6Sn5 enhances *OCHO coverage ~2.8× compared to Sn at pH 1. Using a cation-free, solid-state-electrolyte-based membrane-electrode-assembly, we produce 0.36 M pure FA at 88% FE over 130 hours with a marked full-cell EE of 37%.

Suggested Citation

  • Xiaohan Yu & Yuting Xu & Le Li & Mingzhe Zhang & Wenhao Qin & Fanglin Che & Miao Zhong, 2024. "Coverage enhancement accelerates acidic CO2 electrolysis at ampere-level current with high energy and carbon efficiencies," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-45988-4
    DOI: 10.1038/s41467-024-45988-4
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    1. Kang Yang & Ming Li & Tianqi Gao & Guoliang Xu & Di Li & Yao Zheng & Qiang Li & Jingjing Duan, 2024. "An acid-tolerant metal-organic framework for industrial CO2 electrolysis using a proton exchange membrane," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

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