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Ambient Electrosynthesis of Ammonia: Electrode Porosity and Composition Engineering
Authors:Dr Hong Wang  Dr Lu Wang  Dr Qiang Wang  Shuyang Ye  Dr Wei Sun  Yue Shao  Zhiping Jiang  Dr Qiao Qiao  Dr Yimei Zhu  Prof Pengfei Song  Dr Debao Li  Prof Le He  Prof Xiaohong Zhang  Prof Jiayin Yuan  Prof Tom Wu  Prof Geoffrey A Ozin
Affiliation:1. Key Laboratory of Functional Polymer Materials of the Ministry of Education, Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin, P. R. China;2. Materials Chemistry and Nanochemistry Research Group, Solar Fuels Cluster, Centre for Inorganic and Polymeric Nanomaterials, Departments of Chemistry, Chemical Engineering and Applied Chemistry, and Electrical and Computing Engineering, University of Toronto, Toronto, Ontario, Canada;3. Institute of Functional Nano & Soft Materials, Soochow University, Jiangsu, P. R. China;4. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, The Chinese Academy of Sciences, Taiyuan, China;5. Department of Physics, Temple University, Philadelphia, PA, USA;6. Condensed Matter Physics and Materials Science Department, Brookhaven National Laboratory, Upton, NY, USA;7. College of Chemistry and Chemical Engineering, Northwest Normal University, Lanzhou, P. R. China;8. Department of Materials and Environmental Chemistry, Stockholm University, Stockholm, Sweden;9. School of Materials Science and Engineering, UNSW Australia, Sydney, NSW, Australia
Abstract:Ammonia, a key precursor for fertilizer production, convenient hydrogen carrier, and emerging clean fuel, plays a pivotal role in sustaining life on Earth. Currently, the main route for NH3 synthesis is by the heterogeneous catalytic Haber–Bosch process (N2+3 H2→2 NH3), which proceeds under extreme conditions of temperature and pressure with a very large carbon footprint. Herein we report that a pristine nitrogen‐doped nanoporous graphitic carbon membrane (NCM) can electrochemically convert N2 into NH3 in an acidic aqueous solution under ambient conditions. The Faradaic efficiency and rate of production of NH3 on the NCM electrode reach 5.2 % and 0.08 g m?2 h?1, respectively. Functionalization of the NCM with Au nanoparticles dramatically enhances these performance metrics to 22 % and 0.36 g m?2 h?1, respectively. As this system offers the potential to be scaled to industrial levels it is highly likely that it might displace the century‐old Haber–Bosch process.
Keywords:electrocatalysis  functionalization  nitrogen fixation  poly(ionic liquid)  porous carbon membrane
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