Ambient Electrosynthesis of Urea with Nitrate and Carbon Dioxide over Iron‐Based Dual‐Sites
Jing Geng, Sihan Ji, Meng Jin, Chao Zhang, Min Xu, Guozhong Wang, Changhao Liang, Haimin Zhang
Abstract
Abstract The development of efficient electrocatalysts to generate key *NH 2 and *CO intermediates is crucial for ambient urea electrosynthesis with nitrate (NO 3 − ) and carbon dioxide (CO 2 ). Here we report a liquid‐phase laser irradiation method to fabricate symbiotic graphitic carbon encapsulated amorphous iron and iron oxide nanoparticles on carbon nanotubes (Fe(a)@C‐Fe 3 O 4 /CNTs). Fe(a)@C‐Fe 3 O 4 /CNTs exhibits superior electrocatalytic activity toward urea synthesis using NO 3 − and CO 2 , affording a urea yield of 1341.3±112.6 μg h −1 mg cat −1 and a faradic efficiency of 16.5±6.1 % at ambient conditions. Both experimental and theoretical results indicate that the formed Fe(a)@C and Fe 3 O 4 on CNTs provide dual active sites for the adsorption and activation of NO 3 − and CO 2 , thus generating key *NH 2 and *CO intermediates with lower energy barriers for urea formation. This work would be helpful for design and development of high‐efficiency dual‐site electrocatalysts for ambient urea synthesis.