<p>Nitrate pollution and carbon emissions, driven by anthropogenic nitrogen cycle imbalance and fossil fuel overuse, pose serious threats to environmental and human health. Electrocatalytic C-N coupling of CO<sub>2</sub> with nitrogen-containing species offers a sustainable route for urea synthesis, contributing to nitrogen recycling and carbon neutrality. However, developing electro-catalysts with high activity, selectivity, and stability remains challenging. Recent advances in rationally designed copper (Cu)-based catalysts have deepened the understanding of C-N coupling mechanisms and structure-performance relationships. This review highlights recent progress in Cu-based electrocatalysts for urea synthesis (mainly for CO<sub>2</sub> and nitrate coupling), focusing on three key strategies: electronic structure modulation, defect engineering, and multi-site synergy. The reaction pathways are first summarized, followed by discussions on catalyst design principles aimed at optimizing intermediate adsorption, lowering C-N coupling barriers, and facilitating proton-coupled electron transfer. In-situ characterizations are employed to elucidate the mechanistic roles of these strategies. Finally, the key challenges and future directions for the application of Cu-based catalysts are outlined.</p>

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Recent advances in Cu-based catalysts for urea electrosynthesis from CO2 and nitrate coupling

  • Zhong Cheng,
  • Peilian Hou,
  • Chen Chen,
  • Shuangyin Wang

摘要

Nitrate pollution and carbon emissions, driven by anthropogenic nitrogen cycle imbalance and fossil fuel overuse, pose serious threats to environmental and human health. Electrocatalytic C-N coupling of CO2 with nitrogen-containing species offers a sustainable route for urea synthesis, contributing to nitrogen recycling and carbon neutrality. However, developing electro-catalysts with high activity, selectivity, and stability remains challenging. Recent advances in rationally designed copper (Cu)-based catalysts have deepened the understanding of C-N coupling mechanisms and structure-performance relationships. This review highlights recent progress in Cu-based electrocatalysts for urea synthesis (mainly for CO2 and nitrate coupling), focusing on three key strategies: electronic structure modulation, defect engineering, and multi-site synergy. The reaction pathways are first summarized, followed by discussions on catalyst design principles aimed at optimizing intermediate adsorption, lowering C-N coupling barriers, and facilitating proton-coupled electron transfer. In-situ characterizations are employed to elucidate the mechanistic roles of these strategies. Finally, the key challenges and future directions for the application of Cu-based catalysts are outlined.