Ambient Electrosynthesis of Urea with Nitrate and Carbon Dioxide over Iron‐Based Dual‐Sites

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.