Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 54, Issue 51, Pages 15501-15505Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201508128
Keywords
CO2; ethane; heterogeneous catalysis; surface chemistry; X-ray absorption
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Funding
- U.S. Department of Energy, Office of Basic Energy Sciences [DE-SC0012704]
- US Department of Energy
- National Energy Research Scientific Computing Center (NERSC) - Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
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The recent shale gas boom combined with the requirement to reduce atmospheric CO2 have created an opportunity for using both raw materials (shale gas and CO2) in a single process. Shale gas is primarily made up of methane, but ethane comprises about 10% and reserves are underutilized. Two routes have been investigated by combining ethane decomposition with CO2 reduction to produce products of higher value. The first reaction is ethane dry reforming which produces synthesis gas (CO+H-2). The second route is oxidative dehydrogenation which produces ethylene using CO2 as a soft oxidant. The results of this study indicate that the Pt/CeO2 catalyst shows promise for the production of synthesis gas, while Mo2C-based materials preserve the C-C bond of ethane to produce ethylene. These findings are supported by density functional theory (DFT) calculations and X-ray absorption near-edge spectroscopy (XANES) characterization of the catalysts under in situ reaction conditions.
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