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Bio-Inspired Aerobic-Hydrophobic Janus Interface on Partially Carbonized Iron Heterostructure Promotes Bifunctional Nitrogen Fixation |
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| Authors: | Wei Zong Haiqi Gao Yue Ouyang Kaibin Chu Hele Guo Leiqian Zhang Wei Zhang Ruwei Chen Yuhang Dai Fei Guo Jiexin Zhu Zhenfang Zhang Chumei Ye Dr Yue-E Miao Prof Johan Hofkens Dr Feili Lai Prof Tianxi Liu |
| Institution: | 1. Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, International Joint Research Laboratory for Nano Energy Composites, Jiangnan University, Wuxi, 214122 P. R. China
State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620 P. R. China Christopher Ingold Laboratory, Department of Chemistry, University College London, 20 Gordon Street, London, WC1H 0AJ UK These authors contributed equally to this work.;2. State Key Laboratory of Organic Electronics and Information Displays&Institute of Advanced Materials (IAM), Nanjing University of Posts&Telecommunications, Nanjing, 210023 P. R. China These authors contributed equally to this work.;3. State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620 P. R. China These authors contributed equally to this work.;4. Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, International Joint Research Laboratory for Nano Energy Composites, Jiangnan University, Wuxi, 214122 P. R. China Department of Chemistry, KU Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium;5. Department of Chemistry, KU Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium;6. Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, International Joint Research Laboratory for Nano Energy Composites, Jiangnan University, Wuxi, 214122 P. R. China;7. Christopher Ingold Laboratory, Department of Chemistry, University College London, 20 Gordon Street, London, WC1H 0AJ UK;8. Department of Materials Science and Metallurgy, University of Cambridge, Cambridge, CB3 0FS UK;9. State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620 P. R. China;10. Department of Chemistry, KU Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium Department of Molecular Spectroscopy, Max Planck Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany |
| Abstract: | Competition from hydrogen/oxygen evolution reactions and low solubility of N2 in aqueous systems limited the selectivity and activity on nitrogen fixation reaction. Herein, we design an aerobic-hydrophobic Janus structure by introducing fluorinated modification on porous carbon nanofibers embedded with partially carbonized iron heterojunctions (Fe3C/Fe@PCNF-F). The simulations prove that the Janus structure can keep the internal Fe3C/Fe@PCNF-F away from water infiltration and endow a N2 molecular-concentrating effect, suppressing the competing reactions and overcoming the mass-transfer limitations to build a robust “quasi-solid–gas” state micro-domain around the catalyst surface. In this proof-of-concept system, the Fe3C/Fe@PCNF-F exhibits excellent electrocatalytic performance for nitrogen fixation (NH3 yield rate up to 29.2 μg h?1 mg?1cat. and Faraday efficiency (FE) up to 27.8 % in nitrogen reduction reaction; NO3? yield rate up to 15.7 μg h?1 mg?1cat. and FE up to 3.4 % in nitrogen oxidation reaction). |
| Keywords: | Aerobic-Hydrophobic Bio-Inspired Janus Nitrogen Fixation Quasi-Solid–Gas State |