Water-tolerant graphene oxide as a high-efficiency catalyst for the synthesis of propylene carbonate from propylene oxide and carbon dioxide |
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| Affiliation: | 1. State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, Hunan, China;2. Department of Chemistry, Hong Kong Baptist University, Kowloon Tong, Hong Kong;1. Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, School of Petrochemical Engineering, Changzhou University, Changzhou 213164, Jiangsu, PR China;2. Key Laboratory of Coal Processing and Efficient Utilization (Ministry of Education), China University of Mining & Technology, Xuzhou 221116, Jiangsu, PR China;1. Department of Chemical Engineering, Lee Kong Chian Faculty of Engineering and Science, Universiti Tunku Abdul Rahman, Bandar Sungai Long, Jalan Sungai Long, 43000 Kajang, Selangor, Malaysia;2. Department of Chemical Engineering, Faculty of Engineering and Built Environment, National University of Malaysia, 43600 UKM Bangi, Selangor, Malaysia;3. Department of Polymer Engineering, Faculty of Chemical Engineering, Universiti Teknologi Malaysia, 81310 UTM Skudai, Johor, Malaysia;1. Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy, Dalian 116023, Liaoning, China;2. State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian 116012, Liaoning, China;3. University of Chinese Academy of Sciences, Beijing 100049, China;1. Department of Chemistry, Lomonosov Moscow State University, 1 Leninskie Gory, GSP-2, 119992 Moscow, Russia;2. Instituto de Síntesis Orgánica (ISO) and Departamento de Química Orgánica, Facultad de Ciencias, Universidad de Alicante, Apdo. 99, 03080, Alicante, Spain |
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| Abstract: | Graphene oxide (GO) was found to be a metal-free, water-tolerant and high-efficiency catalyst towards the cycloaddition of carbon dioxide (CO2) to propylene oxide (PO) for the synthesis of propylene carbonate (PC) at room temperature (RT) and atmospheric pressure without the need for a solvent. Using GO as catalyst and tetrabutylammonium bromide (Bu4NBr) as co-catalyst, PO is rapidly converted to PC with 96% yield and 100% selectivity under relatively mild conditions (100 °C, 2.25 MPa, 1 h). The effects of catalyst amount, temperature, time and water (H2O) addition on the reaction were investigated. It is found that the presence of a proper amount of H2O enhances the conversion of epoxide remarkably. A comparison of the catalytic activities of a number of reduced graphene oxide (r-GO) samples under similar reaction conditions revealed that it is the hydroxyl groups (rather than the carboxyl groups) on GO that form hydrogen bonds with PO, and act synergistically with halide anions to promote the cycloaddition reaction. A possible mechanism is proposed. |
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