Piezoelectricity regulated ohmic contact in M/BaTiO3 (M = Ru,Pd, Pt) for charge collision and hydrogen free radical production in ammonia electrosynthesis |
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| Affiliation: | 1. Department of Materials Science and Engineering, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon 999077, Hong Kong, China;2. Hong Kong Center for Cerebro-Cardiovascular Health Engineering (COCHE), Shatin, NT, Hong Kong Special Administrative Region;3. Centre for Functional Photonics, City University of Hong Kong, Kowloon, Hong Kong;4. Hong Kong Institute for Clean Energy, City University of Hong Kong, Kowloon 999077, Hong Kong;1. College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, China;2. School of Biological and Chemical Engineering, NingboTech University, No.1 South Qianhu Road, Ningbo 315100, China;3. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing; International School of Materials Science and Engineering; School of Materials Science and Microelectronics, Wuhan University of Technology, Hubei, Wuhan 430070, P. R. China;1. Radcliffe Department of Medicine, University of Oxford, OX3 7BN, United Kingdom;2. Technical University of Munich (TUM), School of Natural Sciences and Catalysis Research Center, Department of Chemistry, Chair of Inorganic and Metal-Organic Chemistry, Lichtenbergstraße 4, 85748 Garching, Germany;3. Technical University of Munich (TUM), School of Natural Sciences, Department of Chemistry, Chair of Medicinal and Bioinorganic Chemistry, 85748 Garching, Germany;4. Munich Data Science Institute (MDSI), Technical University of Munich (TUM), 85748 Garching, Germany;1. Institute of Solar Energy, Shanghai University of Electric Power, Shanghai 200090, China;2. School of Electrical and Energy Power Engineering, Yangzhou University, Yangzhou 225002, China;3. School of Energy and Power, Jiangsu University of Science and Technology, Zhenjiang, Jiangsu 212003, China;4. Research Center for Combustion and Environment Technology, Shanghai Jiao Tong University, 800 Dong Chuan Road, Shanghai 200240, China;1. Beijing Key Lab of Cryo-Biomedical Engineering and Key Lab of Cryogenics, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, China;2. Department of Biomedical Engineering, School of Medicine, Tsinghua University, Beijing 100084, China;3. School of Engineering Science, University of Chinese Academy of Sciences, Beijing 100049, China |
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| Abstract: | Electrochemical nitrate reduction reaction (NO3RR) is a promising alternative technique for NH3 generation toward the energy-consuming Haber-Bosch process. Nevertheless, it remains hindered by the competitive hydrogen evolution reaction (HER). Herein, the piezoelectric effect of electron-rich BaTiO3 with oxygen vacancies is introduced to promote NO3RR performance. Combining with metal particles (Ru, Pd and Pt), the catalyst achieves a maximal Faradaic efficiency of 95.3% and NH3 yield rate of 6.87 mg h−1 mgcat.−1. Upon piezoelectricity, the interface between metal nanoparticles and BaTiO3 is effectively modulated from Schottky contact to ohmic contact, which leads to unobstructed electron transfer. Abundant hydrogen radicals (·H) can be then produced from the collision between plentiful electrons and polar water molecules adsorbed on the polar surface. Such ·H can significantly facilitate the hydrogenation of reaction intermediates in NO3RR. Meanwhile, this process suppresses the Volmer-Heyrovsky step, therefore inhibiting the HER within a wide range of external potential. This work suggests a new strategy for promoting the performance of multi-electron-involved catalytic reactions. |
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| Keywords: | Piezoelectric effect Ohmic contact Charge collision Hydrogen radicals |
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