Size dependence in solvent-free aerobic oxidation of alcohols catalyzed by zeolite-supported palladium nanoparticles |
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| Authors: | Feng Li Qinghong Zhang Ye Wang |
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| Affiliation: | 1. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, PR China;2. University of Chinese Academy of Sciences, Beijing 100039, PR China;3. Department of Chemistry, University of Wisconsin-Madison,1101 University Avenue, Madison, WI 53706, United States;4. Key Laboratory of Carbon Materials, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, PR China;1. Department of Chemistry and Industrial Chemistry, University of Pisa, Via G. Moruzzi 3, 56124 Pisa, Italy;2. Department of Molecular Sciences and Nanosystems, University Ca’ Foscari of Venice, Dorsoduro 2137, 30123 Venice, Italy;3. Department of Chemical Sciences, University of Padua, Via Marzolo 1, 35131 Padua, Italy;4. ICCOM CNR, via G. Moruzzi 1, 56124 Pisa, Italy;5. Department of Civil and Industrial Engineering, Largo Lucio Lazzarino 2, 56126 Pisa, Italy;6. Department of Industrial Chemistry “Toso Montanari”, University of Bologna, Viale Risorgimento 4, 41036 Bologna, Italy;1. College of Materials & Environmental Engineering, Hangzhou Dianzi University, Hangzhou 310036, Zhejiang, China;2. Key Lab of Applied Chemistry of Zhejiang Province, Department of Chemistry, Zhejiang University, Hangzhou 310027, Zhejiang, China;3. Department of Chemistry and Materials Technology, Kyoto Institute of Technology, Matsugasaki, Sakyo-ku, Kyoto 606-8585, Japan;1. National Synchrotron Radiation Research Center, Hsinchu 30076, Taiwan;2. Department of Chemistry, National Tsing Hua University, Hsinchu 30013, Taiwan;1. Key Lab of Applied Chemistry of Zhejiang Province, Department of Chemistry, Zhejiang University, Hangzhou 310027, Zhejiang, China;2. Department of Chemistry and Materials Technology, Kyoto Institute of Technology, Kyoto 606-8585, Kyoto Prefecture, Japan |
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| Abstract: | The size dependence in the palladium nanoparticle-catalyzed solvent-free aerobic oxidation of alcohols was studied. Palladium nanoparticles with tunable mean sizes in a range of 2.0–10.5 nm were prepared over NaX zeolite by ion exchange of Na+ with an ionic Pd precursor followed by calcination and H2 reduction. The calcination temperature was found to be a crucial factor in determining the mean size of Pd nanoparticles. Pd/NaX catalysts with proper mean sizes of Pd could catalyze the solvent-free aerobic oxidation of various alcohols, and were particularly efficient for the oxidation of benzylic alcohols without substituents in benzene ring. Detailed studies using the Pd/NaX catalysts with different mean sizes of Pd revealed that the solvent-free aerobic oxidation of benzyl alcohol was structure-sensitive, and the intrinsic turnover frequency (TOF) reached a maximum at a medium mean size of Pd (2.8 nm). On the other hand, for the oxidation of geraniol or 2-octanol without delocalized π-ring, the reaction was structure-insensitive, and the intrinsic TOF did not change significantly with the mean size of Pd particles. |
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