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<p>The electrochemical co-reduction of CO<sub>2</sub> and nitrate provides a sustainable route for urea synthesis via C–N coupling, yet kinetic limitations and poor intermediate interactions hinder urea yields. Here, we engineer a nano-confined CuRu bimetallic catalyst within mesoporous carbon hollow spheres (MCHS) to overcome these barriers. By spatially confining reactants and intermediates, the catalyst achieves a urea yield of 12.51 g h<sup>–1</sup> g<sub>cat</sub><sup>–1</sup> at 250 mA cm<sup>–2</sup>, with 125-hour stability. In situ spectroscopy and computational analyses reveal that nano-confinement switches the C–N coupling pathway from the thermodynamically favored *COOH–*NH<sub>2</sub> to kinetically driven *OCO–*NO intermediates, bypassing energy barriers. Precise pore-size engineering (4–11 nm) demonstrates that optimal confinement simultaneously enhances reactant transport and intermediate retention, boosting selectivity. This work establishes nano-confinement as a versatile approach for controlling multi-step electrocatalytic processes, enabling sustainable chemical synthesis.</p>

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Nano-confinement engineering boosts C–N coupling for urea electrosynthesis

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月26日

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  • Jiaxin Du,
  • Yunshuo Wu,
  • Siyu Fang,
  • Daliang Xu,
  • Min Liu,
  • Heng Liang,
  • Zhongbiao Wu,
  • Gaoqing Max Lu,
  • Xuanhao Wu

摘要

The electrochemical co-reduction of CO2 and nitrate provides a sustainable route for urea synthesis via C–N coupling, yet kinetic limitations and poor intermediate interactions hinder urea yields. Here, we engineer a nano-confined CuRu bimetallic catalyst within mesoporous carbon hollow spheres (MCHS) to overcome these barriers. By spatially confining reactants and intermediates, the catalyst achieves a urea yield of 12.51 g h–1 gcat–1 at 250 mA cm–2, with 125-hour stability. In situ spectroscopy and computational analyses reveal that nano-confinement switches the C–N coupling pathway from the thermodynamically favored *COOH–*NH2 to kinetically driven *OCO–*NO intermediates, bypassing energy barriers. Precise pore-size engineering (4–11 nm) demonstrates that optimal confinement simultaneously enhances reactant transport and intermediate retention, boosting selectivity. This work establishes nano-confinement as a versatile approach for controlling multi-step electrocatalytic processes, enabling sustainable chemical synthesis.