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<p>The electrochemical reduction of carbon dioxide (CO<sub>2</sub>) to carbon monoxide (CO) is challenged by a selectivity decline at high current densities. Here we report a class of indigo-based molecular promoters with redox-active CO<sub>2</sub> binding sites to enhance the high-rate conversion of CO<sub>2</sub> to CO on silver (Ag) catalysts. Theoretical calculations and in situ spectroscopy analyses demonstrate that the synergistic effect at the interface of indigo-derived compounds and Ag nanoparticles could activate CO<sub>2</sub> molecules and accelerate the formation of key intermediates (*CO<sub>2</sub><sup>–</sup> and *COOH) in the CO pathway. Indigo derivatives with electron-withdrawing groups further reduce the overpotential for CO production upon optimizing the interfacial CO<sub>2</sub> binding affinity. By integrating the molecular design of redox-active centres with the defect engineering of Ag structures, we achieve a Faradaic efficiency for CO exceeding 90% across a current density range of 0.10 − 1.20 A cm<sup>–2</sup>. The Ag mass activity toward CO increases to 174 A mg<sup>–1</sup><sub>Ag</sub>. This work showcases that employing redox-active CO<sub>2</sub> sorbents as surface modification agents is a highly effective strategy to intensify the reactivity of electrochemical CO<sub>2</sub> reduction.</p>

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Electro-activated indigos intensify ampere-level CO2 reduction to CO on silver catalysts

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年4月3日

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  • Zhengyuan Li,
  • Xing Li,
  • Ruoyu Wang,
  • Astrid Campos Mata,
  • Carter S. Gerke,
  • Shuting Xiang,
  • Anmol Mathur,
  • Lingyu Zhang,
  • Dian-Zhao Lin,
  • Tianchen Li,
  • Krish N. Jayarapu,
  • Andong Liu,
  • Lavanya Gupta,
  • Anatoly I. Frenkel,
  • V. Sara Thoi,
  • Pulickel M. Ajayan,
  • Soumyabrata Roy,
  • Yuanyue Liu,
  • Yayuan Liu

摘要

The electrochemical reduction of carbon dioxide (CO2) to carbon monoxide (CO) is challenged by a selectivity decline at high current densities. Here we report a class of indigo-based molecular promoters with redox-active CO2 binding sites to enhance the high-rate conversion of CO2 to CO on silver (Ag) catalysts. Theoretical calculations and in situ spectroscopy analyses demonstrate that the synergistic effect at the interface of indigo-derived compounds and Ag nanoparticles could activate CO2 molecules and accelerate the formation of key intermediates (*CO2– and *COOH) in the CO pathway. Indigo derivatives with electron-withdrawing groups further reduce the overpotential for CO production upon optimizing the interfacial CO2 binding affinity. By integrating the molecular design of redox-active centres with the defect engineering of Ag structures, we achieve a Faradaic efficiency for CO exceeding 90% across a current density range of 0.10 − 1.20 A cm–2. The Ag mass activity toward CO increases to 174 A mg–1Ag. This work showcases that employing redox-active CO2 sorbents as surface modification agents is a highly effective strategy to intensify the reactivity of electrochemical CO2 reduction.