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

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.