4.5 Review

Carbon dioxide reduction in tandem with light-alkane dehydrogenation

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NATURE REVIEWS CHEMISTRY
卷 3, 期 11, 页码 638-649

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NATURE PUBLISHING GROUP
DOI: 10.1038/s41570-019-0128-9

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  1. U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Biosciences, and Geosciences [DE-SC0012704]
  2. U.S. National Science Foundation [DGE-16-44869]
  3. Gates Millennium Scholarship Foundation

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A greenhouse gas and mild oxidant, CO2 can effect the oxidative dehydrogenation (CO2-ODH) of light alkanes over heterogeneous catalysts. These catalysts are bifunctional in that they mediate CO2 reduction while oxidizing the alkanes, most notably the C-2-C-4 components in shale gas. In this way, one obtains CO and alkenes as value-added products. Although desirable, this transformation has proven challenging in terms of catalyst design, with most catalysts for the CO2-ODH being metal oxides that typically undergo rapid deactivation. More recently, bimetallic catalysts have been identified as promising systems to activate alkanes by either selectively cleaving C-H bonds to produce alkenes or breaking all the C-C and C-H bonds to produce the dry reforming products CO and H-2. This Review describes general trends in the CO2-ODH of light alkanes. We will also outline how to use a combined approach involving flow reactor experiments, in operando characterization and density functional theory to determine whether a catalyst is intrinsically active for CO2-ODH or dry reforming.

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