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<p>Electrocatalytic CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) to formate offers a promising pathway for storing renewable electricity in chemical fuels and enabling carbon recycling. The development of efficient and stable catalysts for this specific pathway, however, remains a central challenge. Heteroatom doping can significantly tune the interaction between active sites and key intermediates, boosting catalytic performance. Conventional doping in Bi-based catalysts often relies on uncontrollable <i>in-situ</i> electrochemical processes, leading to ineffective bulk incorporation. Here, we present a simple pre-doping strategy that enables precise doping at surface active sites, thereby enhancing electrochemical performance. The resulting catalyst achieves &gt;95% Faradaic efficiency for formate across 100–500 mA cm<sup>−2</sup> in a flow cell and maintains &gt;95% efficiency for over 70 h at 100 mA cm<sup>−2</sup> in a membrane electrode assembly, outperforming pure Bi and Bi<sub>2</sub>S<sub>3</sub>. A solar-driven system further demonstrates a 4.4% solar-to-formate conversion efficiency. Mechanistic studies reveal that sulfur doping increases electron density, stabilizes the key *OCHO intermediate, and suppresses hydrogen evolution. These findings provide valuable insights into the precise predoping modulation of surface active sites for designing highly efficient and stable CO<sub>2</sub>RR catalysts.</p>

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Trace sulfur pre-doped bismuth electrocatalysts for stable and efficient CO2 reduction to formate

  • 期刊论文

  • 发表日期：

    2026年4月13日

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  • Zhengjie Yao,
  • Yitao Wang,
  • Chenglong Qiu,
  • Yiwen Wang,
  • Lijia Liu,
  • Wei Chen,
  • Zhenjie Cheng,
  • Jiacheng Wang,
  • Lili Zhang

摘要

Electrocatalytic CO2 reduction reaction (CO2RR) to formate offers a promising pathway for storing renewable electricity in chemical fuels and enabling carbon recycling. The development of efficient and stable catalysts for this specific pathway, however, remains a central challenge. Heteroatom doping can significantly tune the interaction between active sites and key intermediates, boosting catalytic performance. Conventional doping in Bi-based catalysts often relies on uncontrollable in-situ electrochemical processes, leading to ineffective bulk incorporation. Here, we present a simple pre-doping strategy that enables precise doping at surface active sites, thereby enhancing electrochemical performance. The resulting catalyst achieves >95% Faradaic efficiency for formate across 100–500 mA cm−2 in a flow cell and maintains >95% efficiency for over 70 h at 100 mA cm−2 in a membrane electrode assembly, outperforming pure Bi and Bi2S3. A solar-driven system further demonstrates a 4.4% solar-to-formate conversion efficiency. Mechanistic studies reveal that sulfur doping increases electron density, stabilizes the key *OCHO intermediate, and suppresses hydrogen evolution. These findings provide valuable insights into the precise predoping modulation of surface active sites for designing highly efficient and stable CO2RR catalysts.