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

Abstract

The development of efficient electrocatalysts to generate key *NH₂ and *CO intermediates is crucial for ambient urea electrosynthesis with nitrate (NO₃ ^- ) and carbon dioxide (CO₂ ). 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-Fe₃ O₄ /CNTs). Fe(a)@C-Fe₃ O₄ /CNTs exhibits superior electrocatalytic activity toward urea synthesis using NO₃ ^- and CO₂ , 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 Fe₃ O₄ on CNTs provide dual active sites for the adsorption and activation of NO₃ ^- and CO₂ , thus generating key *NH₂ 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.