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<p>The electrocatalytic C−N coupling of the greenhouse gas carbon dioxide and N<sub>2</sub>/nitrate presents a promising approach to the conventional Bosch-Meiser method for environmentally friendly urea synthesis. Two-dimensional (2D) materials exhibit significant advantages in electrocatalysis due to their unique ultrathin structure and physicochemical properties as a platform Substrates for atomic modification. Here, this review focuses on the Surface functionalization of 2D electrocatalysts (Oxides, Sulfide, MOFs, Mxene, et al.) through heteroatom doping, defect engineering, and Surface molecule functionalization to enhance the catalyst conductivity, lower the reaction barrier, and improve its cycling stability. Then, we provide a Summary of surface modified 2D electrocatalysts (the single-atom site, synergistic effects of dual-active-sites, et al.) towards C−N coupling reaction of N<sub>2</sub> /NO<sub>x</sub> and CO<sub>2</sub> for urea synthesis, analyze the catalysis origins through combination of DFT calculations, which are widely adopted to offer a precise description of the electronic structure of catalysts and the relationship between catalytic activity and catalysts. The reaction mechanisms researches reveals the optimization of reaction pathways by the dynamic evolution of the catalyst surface, providing a new direction for the design of adaptive catalytic materials.Finally, challenges and perspectives in the field are presented.</p>

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Surface-functionalized two-dimensional materials towards electrocatalytic C−N coupling reaction for urea

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年9月22日

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  • Yue Shang,
  • Dawei Chen,
  • Chen Chen,
  • Shuangyin Wang

摘要

The electrocatalytic C−N coupling of the greenhouse gas carbon dioxide and N2/nitrate presents a promising approach to the conventional Bosch-Meiser method for environmentally friendly urea synthesis. Two-dimensional (2D) materials exhibit significant advantages in electrocatalysis due to their unique ultrathin structure and physicochemical properties as a platform Substrates for atomic modification. Here, this review focuses on the Surface functionalization of 2D electrocatalysts (Oxides, Sulfide, MOFs, Mxene, et al.) through heteroatom doping, defect engineering, and Surface molecule functionalization to enhance the catalyst conductivity, lower the reaction barrier, and improve its cycling stability. Then, we provide a Summary of surface modified 2D electrocatalysts (the single-atom site, synergistic effects of dual-active-sites, et al.) towards C−N coupling reaction of N2 /NOx and CO2 for urea synthesis, analyze the catalysis origins through combination of DFT calculations, which are widely adopted to offer a precise description of the electronic structure of catalysts and the relationship between catalytic activity and catalysts. The reaction mechanisms researches reveals the optimization of reaction pathways by the dynamic evolution of the catalyst surface, providing a new direction for the design of adaptive catalytic materials.Finally, challenges and perspectives in the field are presented.