Conversion of Methane to Methanol and Ethanol over Nickel Oxide on Ceria-Zirconia Catalysts in a Single Reactor
Abstract
Abstract The conversion of methane into alcohols under moderate reaction conditions is a promising technology for converting stranded methane reserves into liquids that can be transported in pipelines and upgraded to value‐added chemicals. We demonstrate that a catalyst consisting of small nickel oxide clusters supported on ceria–zirconia (NiO/CZ) can convert methane to methanol and ethanol in a single, steady‐state process at 723 K using O 2 as an abundantly available oxidant. The presence of steam is required to obtain alcohols rather than CO 2 as the product of catalytic combustion. The unusual activity of this catalyst is attributed to the synergy between the small Lewis acidic NiO clusters and the redox‐active CZ support, which also stabilizes the small NiO clusters.
- Authors:
-
[1]
- Georgia Inst. of Technology, Atlanta, GA (United States)
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- National Renewable Energy Laboratory (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1395093
- Alternate Identifier(s):
- OSTI ID: 1394849
- Report Number(s):
- NREL/JA-5100-69074
Journal ID: ISSN 1433-7851
- Grant/Contract Number:
- AC36-08GO28308; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition); Journal Volume: 56; Journal Issue: 44; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 09 BIOMASS FUELS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; C-H activation; heterogeneous catalysis; Lewis acid; methane; nickel
Citation Formats
Okolie, Chukwuemeka, Belhseine, Yasmeen F., Lyu, Yimeng, Yung, Matthew M., Engelhard, Mark H., Kovarik, Libor, Stavitski, Eli, and Sievers, Carsten. Conversion of Methane to Methanol and Ethanol over Nickel Oxide on Ceria-Zirconia Catalysts in a Single Reactor. United States: N. p., 2017.
Web. doi:10.1002/anie.201704704.
Okolie, Chukwuemeka, Belhseine, Yasmeen F., Lyu, Yimeng, Yung, Matthew M., Engelhard, Mark H., Kovarik, Libor, Stavitski, Eli, & Sievers, Carsten. Conversion of Methane to Methanol and Ethanol over Nickel Oxide on Ceria-Zirconia Catalysts in a Single Reactor. United States. https://doi.org/10.1002/anie.201704704
Okolie, Chukwuemeka, Belhseine, Yasmeen F., Lyu, Yimeng, Yung, Matthew M., Engelhard, Mark H., Kovarik, Libor, Stavitski, Eli, and Sievers, Carsten. Tue .
"Conversion of Methane to Methanol and Ethanol over Nickel Oxide on Ceria-Zirconia Catalysts in a Single Reactor". United States. https://doi.org/10.1002/anie.201704704. https://www.osti.gov/servlets/purl/1395093.
@article{osti_1395093,
title = {Conversion of Methane to Methanol and Ethanol over Nickel Oxide on Ceria-Zirconia Catalysts in a Single Reactor},
author = {Okolie, Chukwuemeka and Belhseine, Yasmeen F. and Lyu, Yimeng and Yung, Matthew M. and Engelhard, Mark H. and Kovarik, Libor and Stavitski, Eli and Sievers, Carsten},
abstractNote = {Abstract The conversion of methane into alcohols under moderate reaction conditions is a promising technology for converting stranded methane reserves into liquids that can be transported in pipelines and upgraded to value‐added chemicals. We demonstrate that a catalyst consisting of small nickel oxide clusters supported on ceria–zirconia (NiO/CZ) can convert methane to methanol and ethanol in a single, steady‐state process at 723 K using O 2 as an abundantly available oxidant. The presence of steam is required to obtain alcohols rather than CO 2 as the product of catalytic combustion. The unusual activity of this catalyst is attributed to the synergy between the small Lewis acidic NiO clusters and the redox‐active CZ support, which also stabilizes the small NiO clusters.},
doi = {10.1002/anie.201704704},
journal = {Angewandte Chemie (International Edition)},
number = 44,
volume = 56,
place = {United States},
year = {Tue Aug 08 00:00:00 EDT 2017},
month = {Tue Aug 08 00:00:00 EDT 2017}
}
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