Revealing the Active Species for Aerobic Alcohol Oxidation by Using Uniform Supported Palladium Catalysts |
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| Authors: | Pingyu Xin Prof?Dr Jia Li Yu Xiong Xi Wu Dr Juncai Dong Dr Wenxing Chen Prof?Dr Yu Wang Prof?Dr Lin Gu Prof?Dr Jun Luo Dr Hongpan Rong Prof?Dr Chen Chen Prof?Dr Qing Peng Prof?Dr Dingsheng Wang Prof?Dr Yadong Li |
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| Institution: | 1. Department of Chemistry, Tsinghua University, Beijing, China;2. Institute of Advanced Materials, Graduate School at Shenzhen, Tsinghua University, Shenzhen, China;3. College of Chemistry and Chemical Engineering, Central South University, Hunan, China;4. Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, China;5. Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Science, Shanghai, China;6. Institute of Physics, Chinese Academy of Science, Beijing, China;7. Center for Electron Microscopy, Tianjin University of Technology, Tianjin, China |
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| Abstract: | The active species in supported metal catalysts are elusive to identify, and large quantities of inert species can cause significant waste. Herein, using a stoichiometrically precise synthetic method, we prepare atomically dispersed palladium–cerium oxide (Pd1/CeO2) and hexapalladium cluster–cerium oxide (Pd6/CeO2), as confirmed by spherical‐aberration‐corrected transmission electron microscopy and X‐ray absorption fine structure spectroscopy. For aerobic alcohol oxidation, Pd1/CeO2 shows extremely high catalytic activity with a TOF of 6739 h?1 and satisfactory selectivity (almost 100 % for benzaldehyde), while Pd6/CeO2 is inactive, indicating that the true active species are single Pd atoms. Theoretical simulations reveal that the bulkier Pd6 clusters hinder the interactions between hydroxy groups and the CeO2 surface, thus suppressing synergy of Pd‐Ce perimeter. |
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| Keywords: | aerobic oxidation benzyl alcohol palladium clusters single atom catalysts supported catalysts |
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