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In situ FTIR studies of methanol adsorption and dehydrogenation over Cu/SiO2 catalyst
Affiliation:1. School of Chemical Science, University of Chinese Academy of Sciences, Beijing 100049, China;2. Beijing Key Laboratory of Ionic Liquids Clean Process, Key Laboratory of Green Process and Engineering, Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China;3. Zhongke Langfang, Institute of Process Engineering, Chinese Academic of Sciences, Hebei 065000, China;1. National Engineering Laboratory for Methanol to Olefins, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, P.O. Box 110, 116023 Dalian, PR China;2. Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, PR China;3. Graduate University of Chinese Academy of Sciences, Beijing 100049, PR China;1. Faculty of Chemistry, Vinh University, Vinh, Viet Nam;2. Faculty of Chemistry and Center for Computational Science, Hanoi National University of Education, Hanoi, Viet Nam;3. School of Chemical Engineering, Hanoi University of Science and Technology, Hanoi, Viet Nam;1. Department of Chemical and Biological Engineering, Tufts University, 4 Colby Street, Medford, MA 02155, United States;2. X-ray Science Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, Illinois 60439, USA;1. Institut für Funktionelle Grenzflächen, Karlsruher Institut für Technologie, 76021 Karlsruhe, Germany;2. Institut für Chemie, Humboldt-Universität zu Berlin, Unter den Linden 6, 10099 Berlin, Germany
Abstract:In situ FTIR spectroscopy was used to identify the adsorbed species and the intermediates during methanol dehydrogenation over Cu/SiO2 catalyst, and a schematic reaction network was proposed. Methoxy species on copper, which were derived from adsorbed methanol, dehydrogenated into formaldehyde. Then several competitive pathways took place. The adsorbed formaldehyde could desorb to the gas phase, or react with another adsorbed methoxy group to form methyl formate, and/or undergo further dehydrogenation to CO and H2. Carbon monoxide formed from the decomposition first adsorbed on high-index planes of copper, and then on low-index planes as the reaction progressed. With the increase of temperature, the concentration of formaldehyde and CO in gas phase increased, and that of methyl formate decreased.
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