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<p>Current catalysts face challenges with low formate selectivity at high current densities during the CO<sub>2</sub> electroreduction. Here, we showcase a versatile strategy to enhance the formate production on <i>p</i>-block metal-based catalysts by incorporating noble metal atoms on their surface, refining oxygen affinity, and tuning adsorption of the critical oxygen-bound *OCHO intermediate. The formate yield is observed to afford a volcano-like dependence on the *OCHO binding strength across a series of modified catalysts. The rhodium-dispersed indium oxide (Rh/In<sub>2</sub>O<sub>3</sub>) catalyst exhibits impressive performances, achieving Faradaic efficiencies (FEs) of formate exceeding 90% across a broad current density range of 0.20 to 1.21 A cm<sup>−2</sup>. In situ Raman spectroscopy and theoretical calculations reveal that the oxophilic Rh site facilitates *OCHO formation by optimizing its adsorption energy, placing Rh/In<sub>2</sub>O<sub>3</sub> near the volcano-shaped apex. A bipolar electrosynthesis system, coupling the CO<sub>2</sub> reduction at the cathode with the formaldehyde oxidative dehydrogenation at the anode, further&#xa0;boosts the FE of formate to nearly 190% with pure hydrogen generation under an ampere-level current density and a low cell voltage of 2.5 V in a membrane electrode assembly cell.</p>

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Ampere-level co-electrosynthesis of formate from CO2 reduction paired with formaldehyde dehydrogenation reactions

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年5月25日

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  • Zhengyuan Li,
  • Peng Wang,
  • Guanqun Han,
  • Shize Yang,
  • Soumyabrata Roy,
  • Shuting Xiang,
  • Juan D. Jimenez,
  • Vamsi Krishna Reddy Kondapalli,
  • Xiang Lyu,
  • Jianlin Li,
  • Alexey Serov,
  • Ruizhi Li,
  • Vesselin Shanov,
  • Sanjaya D. Senanayake,
  • Anatoly I. Frenkel,
  • Pulickel M. Ajayan,
  • Yujie Sun,
  • Thomas P. Senftle,
  • Jingjie Wu

摘要

Current catalysts face challenges with low formate selectivity at high current densities during the CO2 electroreduction. Here, we showcase a versatile strategy to enhance the formate production on p-block metal-based catalysts by incorporating noble metal atoms on their surface, refining oxygen affinity, and tuning adsorption of the critical oxygen-bound *OCHO intermediate. The formate yield is observed to afford a volcano-like dependence on the *OCHO binding strength across a series of modified catalysts. The rhodium-dispersed indium oxide (Rh/In2O3) catalyst exhibits impressive performances, achieving Faradaic efficiencies (FEs) of formate exceeding 90% across a broad current density range of 0.20 to 1.21 A cm−2. In situ Raman spectroscopy and theoretical calculations reveal that the oxophilic Rh site facilitates *OCHO formation by optimizing its adsorption energy, placing Rh/In2O3 near the volcano-shaped apex. A bipolar electrosynthesis system, coupling the CO2 reduction at the cathode with the formaldehyde oxidative dehydrogenation at the anode, further boosts the FE of formate to nearly 190% with pure hydrogen generation under an ampere-level current density and a low cell voltage of 2.5 V in a membrane electrode assembly cell.