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Stable, active CO2 reduction to formate via redox-modulated stabilization of active sites

Author

Listed:
  • Le Li

    (Nanjing University)

  • Adnan Ozden

    (University of Toronto)

  • Shuyi Guo

    (Nanjing University)

  • F. Pelayo Garcı́a de Arquer

    (University of Toronto)

  • Chuanhao Wang

    (Nanjing University)

  • Mingzhe Zhang

    (Nanjing University)

  • Jin Zhang

    (Nanjing University)

  • Haoyang Jiang

    (Nanjing University)

  • Wei Wang

    (Nanjing University)

  • Hao Dong

    (Nanjing University)

  • David Sinton

    (University of Toronto)

  • Edward H. Sargent

    (University of Toronto)

  • Miao Zhong

    (Nanjing University)

Abstract

Electrochemical reduction of CO2 (CO2R) to formic acid upgrades waste CO2; however, up to now, chemical and structural changes to the electrocatalyst have often led to the deterioration of performance over time. Here, we find that alloying p-block elements with differing electronegativities modulates the redox potential of active sites and stabilizes them throughout extended CO2R operation. Active Sn-Bi/SnO2 surfaces formed in situ on homogeneously alloyed Bi0.1Sn crystals stabilize the CO2R-to-formate pathway over 2400 h (100 days) of continuous operation at a current density of 100 mA cm−2. This performance is accompanied by a Faradaic efficiency of 95% and an overpotential of ~ −0.65 V. Operating experimental studies as well as computational investigations show that the stabilized active sites offer near-optimal binding energy to the key formate intermediate *OCHO. Using a cation-exchange membrane electrode assembly device, we demonstrate the stable production of concentrated HCOO– solution (3.4 molar, 15 wt%) over 100 h.

Suggested Citation

  • Le Li & Adnan Ozden & Shuyi Guo & F. Pelayo Garcı́a de Arquer & Chuanhao Wang & Mingzhe Zhang & Jin Zhang & Haoyang Jiang & Wei Wang & Hao Dong & David Sinton & Edward H. Sargent & Miao Zhong, 2021. "Stable, active CO2 reduction to formate via redox-modulated stabilization of active sites," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-25573-9
    DOI: 10.1038/s41467-021-25573-9
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    Cited by:

    1. Jin Zhang & Chenxi Guo & Susu Fang & Xiaotong Zhao & Le Li & Haoyang Jiang & Zhaoyang Liu & Ziqi Fan & Weigao Xu & Jianping Xiao & Miao Zhong, 2023. "Accelerating electrochemical CO2 reduction to multi-carbon products via asymmetric intermediate binding at confined nanointerfaces," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    2. Haifeng Shen & Huanyu Jin & Haobo Li & Herui Wang & Jingjing Duan & Yan Jiao & Shi-Zhang Qiao, 2023. "Acidic CO2-to-HCOOH electrolysis with industrial-level current on phase engineered tin sulfide," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    3. Mingfang Chi & Jingwen Ke & Yan Liu & Miaojin Wei & Hongliang Li & Jiankang Zhao & Yuxuan Zhou & Zhenhua Gu & Zhigang Geng & Jie Zeng, 2024. "Spatial decoupling of bromide-mediated process boosts propylene oxide electrosynthesis," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    4. Jiexin Zhu & Jiantao Li & Ruihu Lu & Ruohan Yu & Shiyong Zhao & Chengbo Li & Lei Lv & Lixue Xia & Xingbao Chen & Wenwei Cai & Jiashen Meng & Wei Zhang & Xuelei Pan & Xufeng Hong & Yuhang Dai & Yu Mao , 2023. "Surface passivation for highly active, selective, stable, and scalable CO2 electroreduction," Nature Communications, Nature, vol. 14(1), pages 1-13, December.

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