Identifying and tailoring C–N coupling site for efficient urea synthesis over diatomic Fe–Ni catalyst

• DOI: 10.1038/s41467-022-33066-6
• Publication Date: 2022-09-10T18:02:44Z
• Authors: Xiaoran Zhang; Xiaorong Zhu; Shuowen Bo; Chen Chen; Mengyi Qiu; Xiaoxiao Wei; Nihan He; Chao Xie; Wei Chen; Jianyun Zheng; Pinsong Chen; San Ping Jiang; Yafei Li; Qinghua Liu; Shuangyin Wang
• Keywords: Electrochemical Reduction of CO2 to Fuels; Science; Ammonia Synthesis and Electrocatalysis; Electrode; Organic chemistry; Yield (engineering); 01 natural sciences; Article; Catalysis; Chemical engineering; Engineering; Electrochemistry; Coupling (piping); Urea; Diatomic molecule; Atom (system on chip); Embedded system; FOS: Chemical engineering; Artificial Nitrogen Fixation; Energy; Renewable Energy, Sustainability and the Environment; Q; Molecule; Chemical Engineering; Computer science; Materials science; 0104 chemical sciences; Chemistry; Physical chemistry; Faraday efficiency; Physical Sciences; Heterogeneous Electrocatalysts; Metallurgy; Electrocatalysis for Energy Conversion; Adsorption; Electrocatalysis; Nanocatalysts; Inorganic chemistry

AbstractElectrocatalytic 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.