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<p>Electrochemical CO<sub>2</sub> and nitrite co-reduction provides a sustainable urea synthesis route but remains limited by low selectivity and an undecided C–N coupling mechanism. Here, we report co-sputtered bimetallic Cu–Co catalysts that facilitate urea formation via a tandem relay mechanism. The optimal Cu:Co ratio of 1:1 achieves a urea yield rate of 61 ± 6 mmol h⁻<sup>1</sup>g<sub>cat</sub>⁻<sup>1</sup> at –1.2 V vs. RHE under neutral pH, emphasizing the importance of proton balance in sustaining proton-coupled electron transfer. In situ synchrotron-based infrared and Raman spectroscopy monitor the dynamic evolution of *CO, *NH<sub>2</sub>, and C‒N intermediates. In situ X-ray absorption spectroscopy indicates the structural stability of metallic Cu and Co active sites. Density functional theory calculations suggest that *COOH + *NH<sub>2</sub> coupling initiates urea pathway, with *NH<sub>2</sub>CO formation as the potential-determining step. This study integrates rational catalyst design and in situ spectroelectrochemical analysis to advance understanding of electrochemical C–N coupling for urea synthesis.</p>

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Spectroelectrochemical insight into copper cobalt catalysts for CO2 and nitrite co-electroreduction to urea

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月17日

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  • Putri Ramadhany,
  • Thành Trần-Phú,
  • Jodie A. Yuwono,
  • Rosalie K. Hocking,
  • Zhipeng Ma,
  • Xuan Minh Chau Ta,
  • Priyank Kumar,
  • Denny Gunawan,
  • Bernt Johannessen,
  • Antonio Tricoli,
  • Alexandr N. Simonov,
  • Rose Amal,
  • Rahman Daiyan

摘要

Electrochemical CO2 and nitrite co-reduction provides a sustainable urea synthesis route but remains limited by low selectivity and an undecided C–N coupling mechanism. Here, we report co-sputtered bimetallic Cu–Co catalysts that facilitate urea formation via a tandem relay mechanism. The optimal Cu:Co ratio of 1:1 achieves a urea yield rate of 61 ± 6 mmol h⁻1gcat⁻1 at –1.2 V vs. RHE under neutral pH, emphasizing the importance of proton balance in sustaining proton-coupled electron transfer. In situ synchrotron-based infrared and Raman spectroscopy monitor the dynamic evolution of *CO, *NH2, and C‒N intermediates. In situ X-ray absorption spectroscopy indicates the structural stability of metallic Cu and Co active sites. Density functional theory calculations suggest that *COOH + *NH2 coupling initiates urea pathway, with *NH2CO formation as the potential-determining step. This study integrates rational catalyst design and in situ spectroelectrochemical analysis to advance understanding of electrochemical C–N coupling for urea synthesis.