Hydroformylation of olefins by Au/Co3O4 catalysts |
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| Authors: | Xiaohao Liu Baoshan Hu Kaoru Fujimoto Masatake Haruta Makoto Tokunaga |
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| Affiliation: | 1. Department of Chemistry, Graduate School of Science, Kyushu University, Higashi-ku, Fukuoka 812-8581, Japan;2. Department of Chemical Processes and Environments, Faculty of Environmental Engineering, The University of Kitakyushu, 1-1 Hibikino, Wakamatsu-ku, Kitakyushu 808-0135, Japan;3. Department of Applied Chemistry, Graduate School of Urban Environmental Sciences, Tokyo Metropolitan University, 1-1 Minami-osawa, Hachioji, Tokyo 192-0397, Japan;4. Japan Science and Technology Agency (JST), CREST, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012, Japan;1. Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian 116023, China;2. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian 116023, China;3. University of Chinese Academy of Sciences, 19 Yuquan Road, Shijingshan District, Beijing 100049, China;1. Department of Petroleum Chemistry and Organic Catalysis, Faculty of Chemistry, Moscow State University, Moscow 1, GSP-1, 1-3 Leninskiye Gory, Moscow 119991, the Russian Federation;2. Topchiev Institute of Petrochemical Synthesis RAS, Moscow 119991, the Russian Federation;3. The Smart Materials Research Institute, Southern Federal University, Sladkova Street 178/24, Rostov-on-Don 344090, the Russian Federation;4. University of Artois, CNRS, Centrale Lille, University of Lille, UMR 8181-UCCS–Unité de Catalyse et Chimie du Solide, Lens F-62300, France;1. Key Laboratory for Green Chemical Technology of Ministry of Education, R&D Center for Petrochemical Technology, Tianjin University, Tianjin 300072, China;2. Zhejiang Institute of Tianjin University, Ningbo, Zhejiang, 315201, China;3. State Key Laboratory of Engines, Tianjin University, Tianjin 300072, China |
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| Abstract: | The hydroformylation of olefins over supported gold catalysts in an autoclave reactor under mild conditions (100–140 °C, 3–5 MPa) has been studied. Over Au/AC (activated carbon), Au/PVP (polyvinylpyrrolidone), Au/Al2O3, Au/TiO2, Au/Fe2O3, Au/ZnO, Au/CeO2 and Co3O4, 1-olefin mainly remained unchanged and the major products were isomerized olefins or hydrogenated paraffin. In contrast, Au nanoparticles deposited on Co3O4 led to remarkably high catalytic activities in hydroformylation reaction with selectivities above 85% to desired aldehydes. The hydroformylation of olefins proceeds preferentially at temperatures below 140 °C, above which the reactions of olefins gradually shifted to isomerization and then to hydrogenation. It appeared that the activity and selectivity of hydroformylation reaction strongly depend on the molecular structure of olefins, which could be ascribed to steric constraints as internal olefins are relatively inappropriate to form alkyl group and subsequent acyl group by insertion of CO. The Au/Co3O4 catalyst can be recycled by simple decantation with slight decrease in catalytic activity along with an increase in recycle times, which is a great advantage over homogeneous catalysts. The role of gold nanoparticles can be assumed to dissociate hydrogen molecule into atomic species which reduce Co3O4 to Co metal under mild reaction conditions. |
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| Keywords: | Hydroformylation Gold catalyst Cobalt catalyst 1-Hexene Heterogeneous catalysis |
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