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Boosting Electroreduction Kinetics of Nitrogen to Ammonia via Atomically Dispersed Sn Protuberance |
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| Authors: | Dr Lijuan Zhang Hanfeng Zhou Prof Xiaoju Yang Dr Shengbo Zhang Prof Haimin Zhang Xuan Yang Prof Xintai Su Prof Jiangwei Zhang Prof Zhang Lin |
| Institution: | 1. School of Environment and Energy, Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling, South China University of Technology, Guangzhou, Guangdong, 510006 P. R. China
SCNU Environmental Research Institute, Guangdong Provincial Key Laboratory of Chemical Pollution and Environmental Safety & MOE Key Laboratory of Theoretical Chemistry of Environment, South China Normal University, Guangzhou, 510006 China These authors contributed equally to this work.;2. School of Environment and Energy, Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling, South China University of Technology, Guangzhou, Guangdong, 510006 P. R. China These authors contributed equally to this work.;3. School of Chemistry and Chemical Engineering, Hubei Engineering Research Center for Biomaterials and Medical Protective Materials, Huazhong University of Science and Technology (HUST), 1037 Luoyu Rd, Wuhan, 430074 China These authors contributed equally to this work.;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, Chinese Academy of Sciences (China);5. School of Chemistry and Chemical Engineering, Hubei Engineering Research Center for Biomaterials and Medical Protective Materials, Huazhong University of Science and Technology (HUST), 1037 Luoyu Rd, Wuhan, 430074 China;6. School of Environment and Energy, Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling, South China University of Technology, Guangzhou, Guangdong, 510006 P. R. China;7. Science Center of Energy Material and Chemistry, College of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot, 010021 China |
| Abstract: | Atomically dispersed metal catalysts show potential advantages in N2 reduction reaction (NRR) due to their excellent activity and efficient metal utilization. Unfortunately, the reported catalysts usually exhibit unsatisfactory NRR activity due to their poor N2 adsorption and activation. Herein, we report a novel Sn atomically dispersed protuberance (ADP) by coordination with substrate C and O to induce positive charge accumulation on Sn site for improving its N2 adsorption, activation and NRR performance. The extended X-ray absorption fine structure (EXAFS) spectra confirmed the local coordination structure of the Sn ADPs. NRR activity was significantly promoted via Sn ADPs, exhibiting a remarkable NH3 yield (RNH3) of 28.3 μg h−1 mgcat−1 (7447 μg h−1 mgSn−1) at −0.3 V. Furthermore, the enhanced N2Hx intermediates was verified by in situ experiments, yielding consistent results with DFT calculation. This work opens a new avenue to regulate the activity and selectivity of N2 fixation. |
| Keywords: | Atomically Dispersed Sn Hydrogen Evolution Suppression Main-Group Elements (MGEs) N2 Reduction Reaction p-Electron Backdonation |