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Ambient Electrosynthesis of Urea with Nitrate and Carbon Dioxide over Iron-Based Dual-Sites |
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| Authors: | Jing Geng Sihan Ji Dr Meng Jin Dr Chao Zhang Min Xu Prof Guozhong Wang Prof Changhao Liang Prof Haimin Zhang |
| Institution: | 1. Key Laboratory of Materials Physics, Centre for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei, 230031 China
University of Science and Technology of China, Hefei, 230026 China These authors contributed equally to this work.;2. Key Laboratory of Materials Physics, Centre for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei, 230031 China University of Science and Technology of China, Hefei, 230026 China;3. University of Science and Technology of China, Hefei, 230026 China;4. Key Laboratory of Materials Physics, Centre for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei, 230031 China |
| 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-Fe3O4/CNTs). Fe(a)@C-Fe3O4/CNTs exhibits superior electrocatalytic activity toward urea synthesis using NO3? and CO2, affording a urea yield of 1341.3±112.6 μg h?1 mgcat?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 Fe3O4 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. |
| Keywords: | Amorphous Fe Nanoparticles C?N Coupling Reaction Dual Active Sites Fe3O4 Nanoparticles Urea |