Electrocatalytic urea synthesis emerged as the promising alternative of Haber–Bosch process and industrial urea synthetic protocol. Here, we report that a diatomic catalyst with bonded Fe–Ni pairs can significantly improve the efficiency of electrochemical urea synthesis. Compared with isolated diatomic and single-atom catalysts, the bonded Fe–Ni pairs act as the efficient sites for coordinated adsorption and activation of multiple reactants, enhancing the crucial C–N coupling thermodynamically and kinetically. The performance for urea synthesis up to an order of magnitude higher than those of single-atom and isolated diatomic electrocatalysts, a high urea yield rate of 20.2 mmol h⁻¹ g⁻¹ with corresponding Faradaic efficiency of 17.8% has been successfully achieved. A total Faradaic efficiency of about 100% for the formation of value-added urea, CO, and NH₃ was realized. This work presents an insight into synergistic catalysis towards sustainable urea synthesis via identifying and tailoring the atomic site configurations.

电催化尿素合成成为 Haber-Bosch 工艺和工业尿素合成方案的有前途的替代方案。在这里，我们报道了具有键合的 Fe-Ni 对的双原子催化剂可以显着提高电化学尿素合成的效率。与孤立的双原子和单原子催化剂相比，键合的 Fe-Ni 对作为协调吸附和活化多种反应物的有效位点，在热力学和动力学上增强了关键的 C-N 偶联。尿素合成的性能比单原子和孤立的双原子电催化剂高一个数量级，尿素产率为 20.2 mmol h ⁻¹ g ⁻¹成功实现了相应的 17.8% 的法拉第效率。实现了形成增值尿素、CO 和 NH ₃的总法拉第效率约为 100% 。这项工作通过识别和调整原子位点配置，展示了对可持续尿素合成的协同催化作用。