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Selective epoxidation of styrene with air catalyzed by CoOx and CoOx/SiO2 without any reductant
Affiliation:1. Ministry-of-Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules, School of Chemistry and Chemical Engineering, Hubei University, Wuhan 430062, China;2. Jingmen Technical College, Jingmen 448000, China;1. Centro de Investigaciones en Catálisis-CICAT, Universidad Industrial de Santander, Escuela de Química, Km 2 vía El Refugio, Piedecuesta, Santander, Colombia;2. Laboratório de Química Atmosférica (LQA), Universidade Católica do Río de Janeiro, Rua Marquês de Sao Vicente, 225, Gávea-Rio de Janeiro, RJ, Brazil;3. Institut de Chimie des Milieux et Matériaux de Poitiers (IC2MP), Université de Poitiers, CNRS, ENSIP, B1, 1 rue M. Doré, F-86073 Poitiers, France;4. Estado Sólido y Catálisis Ambiental (ESCA), Universidad Nacional de Colombia, Carrera 30 No. 45-03, Bogotá, Colombia;5. Laboratorio de Resonancia Magnética Nuclear, Universidad Industrial de Santander, Km 2 vía El Refugio, Piedecuesta, Colombia;6. Chirosciences UMR CNRS 7313 Institut des Sciences Moléculaires de Marseille (iSm2), Aix-Marseille Université, Campus St Jérôme, 13397 Marseille, France;1. Materials Science Institute and Inorganic Chemistry Department, Alicante University, Ap. 99, E-03080 Alicante, Spain;2. Research Technical Services, Alicante University, Ap. 99, E-03080 Alicante, Spain;3. Materials Science Institute and Physical Chemistry Department, Alicante University, Ap. 99, E-03080 Alicante, Spain;1. Institute of Environmental and Analytical Sciences, College of Chemistry and Chemical Engineering, Henan University, Kaifeng, Henan, 475004, PR China;2. College of Environment and Chemical Engineering, Dalian University, Dalian, 116622, PR China;1. The Key Laboratory of Advanced Materials of Ministry of Education, School of Materials Science and Engineering, Tsinghua University, Beijing City, 100084, China;2. International Graduate School at Shenzhen, Tsinghua University, Shenzhen City, 518055, China;3. College of Materials Science and Hydrogen Energy, Foshan University, Foshan City, 528000, China;4. College of Wenzheng, Soochow University, Suzhou City, 215104, China
Abstract:Cobalt oxide (CoOx) prepared by a direct calcination of cobalt nitrate was considerably active for the epoxidation of styrene with air in DMF under mild conditions. A substrate conversion of 75.8 mol% with an epoxide selectivity of 82.1% was achieved at 353 K over 10 mg of cobalt oxide catalyst. Once CoOx was loaded on the support SiO2 through a simple procedure consisting of wet impregnation, drying and calcination, the as-prepared catalyst presented higher catalytic activity and epoxide selectivity than cobalt oxide itself. Over the optimized catalyst CoOx/SiO2 (1.0 wt% Co), 85.7 mol% of styrene was effectively converted at 363 K within 4 h, with a high epoxide selectivity up to 86.0%. The results showed that many factors influenced the performance of the catalyst, such as the Co loading, the support, the temperature and the atmosphere, etc. The leaching of cobalt from the catalyst CoOx/SiO2 was negligible, indicating the applicability of the catalyst CoOx/SiO2 as a true heterogeneous catalyst. The control test and UV–vis spectra revealed a synergic interaction among solvent, oxygen and substrate over CoOx/SiO2.
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