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Engineering Platinum–Oxygen Dual Catalytic Sites via Charge Transfer towards Highly Efficient Hydrogen Evolution
Authors:Fei Lu  Dr Ding Yi  Dr Shoujie Liu  Dr Fei Zhan  Dr Bo Zhou  Prof Lin Gu  Prof Dmitri Golberg  Prof Xi Wang  Prof Jiannian Yao
Institution:1. Key Laboratory of Luminescence and Optical Information, Ministry of Education, Department of Physics, School of Science, Beijing Jiaotong University, Beijing, 100044 P. R. China

Key Laboratory of Photochemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China

These authors contributed equally to this work.;2. Key Laboratory of Luminescence and Optical Information, Ministry of Education, Department of Physics, School of Science, Beijing Jiaotong University, Beijing, 100044 P. R. China

These authors contributed equally to this work.;3. Chemistry and Chemical Engineering Guangdong Laboratory, Shantou, 515031 P. R. China

Institute of Molecular Plus, Tianjin University, Tianjin, 300072 P. R. China;4. Chemistry and Chemical Engineering Guangdong Laboratory, Shantou, 515031 P. R. China;5. Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190 P. R. China;6. Centre for Materials Science, Queensland University of Technology (QUT), 2 George St., Brisbane, QLD, 4000 Australia

School of Chemistry and Physics, Science and Engineering Faculty Science and Engineering Faculty, Queensland University of Technology (QUT), 2 George St., Brisbane, QLD, 4000 Australia

International Centre for Materials Nanoarhitectonics (MANA), National Institute for Materials Science (NIMS), Namiki 1-1, Tsukuba, Ibaraki, 3050044 Japan;7. Key Laboratory of Luminescence and Optical Information, Ministry of Education, Department of Physics, School of Science, Beijing Jiaotong University, Beijing, 100044 P. R. China;8. Key Laboratory of Photochemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China

Abstract:A dual-site catalyst allows for a synergetic reaction in the close proximity to enhance catalysis. It is highly desirable to create dual-site interfaces in single-atom system to maximize the effect. Herein, we report a cation-deficient electrostatic anchorage route to fabricate an atomically dispersed platinum–titania catalyst (Pt1O1/Ti1?xO2), which shows greatly enhanced hydrogen evolution activity, surpassing that of the commercial Pt/C catalyst in mass by a factor of 53.2. Operando techniques and density functional calculations reveal that Pt1O1/Ti1?xO2 experiences a Pt?O dual-site catalytic pathway, where the inherent charge transfer within the dual sites encourages the jointly coupling protons and plays the key role during the Volmer–Tafel process. There is almost no decay in the activity of Pt1O1/Ti1?xO2 over 300 000 cycles, meaning 30 times of enhancement in stability compared to the commercial Pt/C catalysts (10 000 cycles).
Keywords:charge transfer  dual-site catalysts  hydrogen evolution reaction  operando techniques  synergy
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