期刊
ACS CATALYSIS
卷 12, 期 14, 页码 8279-8290出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c01700
关键词
tandem catalysis; oxygenates; CO2; ethane; DFT calculations
资金
- U.S. Department of Energy (DOE), Office of Basic Energy Sciences, Catalysis Science Program [DE-SC0012704]
- U.S. DOE Office of Science User Facilities [DE-SC0012704]
- Synchrotron Catalysis Consortium under U.S. DOE, Office of Basic Energy Sciences [DESC0012653]
- Office of Science of the U.S. DOE [DE-AC0205CH11231]
The study identified the desired ethylene/CO/H-2 ratios by analyzing different combinations of main and side reactions of CO2 and ethane, and found that the PtSn3/gamma-Al2O3 catalyst has promising potential for the tandem hydroformylation reaction. Experimental and theoretical studies revealed the importance of Pt cluster/SnOx interfacial structures in the conversion of ethane into C3 oxygenates.
The strategy of the tandem hydroformylation reaction for C3 oxygenate production from CO, and ethane represents an opportunity to simultaneously upgrade greenhouse gas CO2 and the large-reserved shale gas into value-added liquid products. One of the challenges is how to tune and achieve the appropriate ethylene/CO/H-2 ratios for the downstream hydroformylation. Herein, we analyze and identify the desired ethylene/ CO/H-2 ratios by considering different combinations of main and side reactions of CO2 and ethane, based on which the PtSn3/gamma-Al2O3 catalyst was identified as promising to enable the catalytic tandem hydroformylation reaction. The combined studies of reactor evaluation, in situ and ex situ characterizations, and theoretical calculations revealed that the Pt cluster/SnOx interfacial structures dominated the simultaneous dehydrogenation and dry reforming of ethane, thereby allowing the coformation of ethylene, CO, and H-2 that were subsequently converted into C3 oxygenates in the tandem hydroformylation reactor. The current work not only demonstrates the design principles of suitable catalysts for the tandem-reactor strategy but also highlights the utilization of CO2 and shale gas to produce value-added oxygenate products.
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