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On the involvement of radical oxygen species O− in catalytic oxidation of benzene to phenol by nitrous oxide
Affiliation:1. Boreskov Institute of Catalysis, Novosibirsk 630090, Russia;2. Solutia Inc., P.O. Box 97, Gonzales, FL 32560-0097, USA;1. College of Chemistry, Chemical Engineering and Biotechnology, Donghua University, 2999 North Renmin Lu, Shanghai 201620, China;2. Key Laboratory of Organofluorine Chemistry, Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences, 345 Lingling Road, Shanghai 200032, China;1. Key Laboratory of Marine Environment and Ecology, Ministry of Education, Qingdao 266100, China;2. College of Environmental Science and Engineering, Ocean University of China, Qingdao 266100, China;3. Shandong Provincial Key Laboratory of Marine Environment and Geological Engineering (MEGE), Qingdao 266100, China;4. China City Environment Protection Engineering Limited Company, Wuhan 430071, China;1. Department of General and Inorganic Chemistry, Faculty of Chemical Technology, University of Pardubice, Studentská 573, 532 10 Pardubice, Czech Republic;2. Institute of Chemistry and Technology of Macromolecular Materials, Faculty of Chemical Technology, University of Pardubice, Studentská 573, 532 10 Pardubice, Czech Republic;3. Department of Analytical Chemistry, Faculty of Chemical Technology, University of Pardubice, Studentská 573, 532 10 Pardubice, Czech Republic;1. Department of Chemistry, Lafayette College, Easton, PA 18042, United States;2. Department of Chemistry, Villanova University, Villanova, PA 19085, United States
Abstract:
Catalytic oxidation of benzene to phenol by nitrous oxide over Fe-MFI zeolites was studied in relation to the active oxygen species taking part in the oxidation. A linear dependence of the reaction rate on the concentration of independently identified active sites generating O radicals (α sites) was obtained within a broad range of values. The dependence is interpreted as convincing evidence of the O involvement in the catalytic (not only stoichiometric) oxidation of benzene to phenol. This conclusion is of particular importance in connection with a long discussion in the literature on a possible role of O radicals in selective oxidation catalysis over V and Mo oxides. Reliable evidence of the catalytic role of O obtained with zeolites may renew general interest in the once-suggested but not recognized role of radical oxygen in oxidation over widely used metal oxide catalysts.
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