Development of [60] fullerene supported on silica catalysts for the photo-oxidation of alkenes |
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| Authors: | George D. Panagiotou Manolis D. Tzirakis John Vakros Loukia Loukatzikou Michael Orfanopoulos Christos Kordulis Alexis Lycourghiotis |
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| Affiliation: | 1. Department of Chemistry, University of Patras, GR-26500 Patras, Greece;2. Department of Chemistry, University of Crete, GR-71003 Voutes, Crete, Greece;3. Department of Chemistry, University of Ioannina, GR-45110 Ioannina, Greece;4. Institute of Chemical Engineering and High-Temperature Chemical Processes (FORTH/ICE-HT), GR-26500 Patras, Greece;1. International Center for Young Scientists (ICYS), Tsukuba, Ibaraki 305-0047, Japan;2. Photocatalytic Material Center, National Institute for Materials Science (NIMS), 1-2-1 Sengen, Tsukuba, Ibaraki 305-0047, Japan;3. Fullerene Engineering, Advanced Nano Materials Laboratory, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan;1. Institute of Catalysis for Energy and Environment, College of Chemistry and Chemical Engineering, Shenyang Normal University, Shenyang, 110034, PR China;2. Department of Chemistry, College of Science, Sultan Qaboos University, Muscat, Oman;3. Department of Chemical Engineering, Kwangwoon University, Seoul 139-701, Korea;4. Department of Chemistry and the Tianjin Key Lab of Metal and Molecule-based Material Chemistry, Nankai University, Tianjin 300071, PR China;5. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, S-106 91 Stockholm, Sweden;6. Laboratory of Green Chemistry, LUT Savo Sustainable Technologies, Lappeenranta University of Technology, Sammonkatu 12, FI-50130 Mikkeli, Finland;1. Key Laboratory of Green Catalysis of Higher Education Institutes of Sichuan, College of Chemistry and Environmental Engineering, Sichuan University of Science and Engineering, Zigong 643000, PR China;2. Research Center of Laser Fusion, China Academy of Engineering Physics, Mianyang 621010, PR China;3. The State Key Laboratory Cultivation Base for Nonmetal Composites and Functional Materials, Southwest University of Science and Technology, Mianyang 621010, PR China;4. Key Laboratory of Photochemistry, Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, PR China;1. College of Environmental Science and Engineering, Hunan University and Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082, PR China;2. State Key Laboratory of Water Resources and Hydropower Engineering Science, Wuhan University, Wuhan, Hubei 430072, PR China;1. Laboratory of Green Chemistry, Faculty of Technology, Lappeenranta University of Technology, Mikkeli FI-50100, Finland;2. Instituto de Ciencia de Materiales, Centro Mixto Universidad de Sevilla- CSIC, C/Américo Vespucio, 49, 41092 Sevilla, Spain |
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| Abstract: | Simple or successive incipient wetness impregnation followed by heating at 180 °C is proved an efficient preparation method for dispersing effectively onto the silica surface various amounts of C60 in the range 1–4% (w/w). BET, XRD, DRS, TGA, microelectrophoresis and photoluminescence have been used to characterize the photocatalysts prepared. A high dispersion was obtained for the quite stable supported C60 phase, comprised mainly from relatively small or medium size C60 clusters/aggregates. The photocatalytic activity was assessed in the singlet oxygen oxidation of alkenes by examining the photo-oxygenation of 2-methyl-2-heptene as a probe reaction. The catalytic tests were carried out at 0–5 °C in CH3CN, under oxygen atmosphere and using a 300 W xenon lamp as the light source. The heterogeneous catalysts obtained were proved to be active in the photocatalytic oxidation of olefins via a 1O2 ene reaction. The catalysts exhibited significant conversion, turnover number and turnover frequency values, substantially higher than those achieved over the unsupported C60. The conversion increases with the amount of the supported C60 up to a value equal to 3% (w/w) and then it decreases whereas turnover number and turnover frequency decreases monotonically as the amount of the supported C60 increases. The easy separation of these solid catalysts from the reaction mixture, the high activity and stability as well as the retained activity in subsequent catalytic cycles, make these supported catalysts suitable for a small-scale synthesis of fine chemicals. |
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