Low temperature catalytic conversion of CH4, CO2, and C2H4 to value-added C3 oxygenates and olefins via C1-C2 coupling on Pd-Au/CeO2
Abstract
The catalytic conversion of CH4 and CO2 in the presence of more reactive co-reactants C2H4 and O2 on Pd-Au/CeO2 is achieved at 200 °C and elevated pressures. Propene and acetone were produced from the catalyzed reaction of CH4 +C2H4 +O2; addition of CO2 to the reactant stream produced methyl acetate (MAc) but it significantly reduced the C-selectivities of propene and acetone. DRIFTS experiments confirmed the formation of methoxy species from CH4 +CO2 at 200 °C, which is an intermediate in the formation of MAc. Here, control experiments with blanks, and with CeO2 did not show any propene, acetone, or MAc products. The complete oxidation of C2H4 was avoided; the catalyst is stable, and reactant conversions and product yields were sustained for the observed 1200 min time-on-stream, indicating that there is little or no carbon deposition and sintering. This direct coupling of CH4 and C2H4 intermediates to higher carbon-number products at 200 °C is significant.
- Authors:
-
[1];
- Louisiana State Univ., Baton Rouge, LA (United States)
- National Energy Technology Lab. (NETL), Pittsburgh, PA (United States)
- Publication Date:
- Research Org.:
- National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)
- Sponsoring Org.:
- USDOE Office of Fossil Energy (FE)
- OSTI Identifier:
- 1899584
- Report Number(s):
- DOE/NETL-2022/3327
Journal ID: ISSN 0926-3373
- Grant/Contract Number:
- FE0026825; 5956-LSU-DOE-6825
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Applied Catalysis. B, Environmental
- Additional Journal Information:
- Journal Volume: 322; Journal ID: ISSN 0926-3373
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CH4 CO2; C-C coupling; Oxygenates; Low temperature; Pd-Au/CeO2
Citation Formats
Aurnob, A.K.M. Kazi, Ding, Kunlun, Kauffman, Douglas R., and Spivey, James J. Low temperature catalytic conversion of CH4, CO2, and C2H4 to value-added C3 oxygenates and olefins via C1-C2 coupling on Pd-Au/CeO2. United States: N. p., 2022.
Web. doi:10.1016/j.apcatb.2022.122107.
Aurnob, A.K.M. Kazi, Ding, Kunlun, Kauffman, Douglas R., & Spivey, James J. Low temperature catalytic conversion of CH4, CO2, and C2H4 to value-added C3 oxygenates and olefins via C1-C2 coupling on Pd-Au/CeO2. United States. https://doi.org/10.1016/j.apcatb.2022.122107
Aurnob, A.K.M. Kazi, Ding, Kunlun, Kauffman, Douglas R., and Spivey, James J. Fri .
"Low temperature catalytic conversion of CH4, CO2, and C2H4 to value-added C3 oxygenates and olefins via C1-C2 coupling on Pd-Au/CeO2". United States. https://doi.org/10.1016/j.apcatb.2022.122107. https://www.osti.gov/servlets/purl/1899584.
@article{osti_1899584,
title = {Low temperature catalytic conversion of CH4, CO2, and C2H4 to value-added C3 oxygenates and olefins via C1-C2 coupling on Pd-Au/CeO2},
author = {Aurnob, A.K.M. Kazi and Ding, Kunlun and Kauffman, Douglas R. and Spivey, James J.},
abstractNote = {The catalytic conversion of CH4 and CO2 in the presence of more reactive co-reactants C2H4 and O2 on Pd-Au/CeO2 is achieved at 200 °C and elevated pressures. Propene and acetone were produced from the catalyzed reaction of CH4 +C2H4 +O2; addition of CO2 to the reactant stream produced methyl acetate (MAc) but it significantly reduced the C-selectivities of propene and acetone. DRIFTS experiments confirmed the formation of methoxy species from CH4 +CO2 at 200 °C, which is an intermediate in the formation of MAc. Here, control experiments with blanks, and with CeO2 did not show any propene, acetone, or MAc products. The complete oxidation of C2H4 was avoided; the catalyst is stable, and reactant conversions and product yields were sustained for the observed 1200 min time-on-stream, indicating that there is little or no carbon deposition and sintering. This direct coupling of CH4 and C2H4 intermediates to higher carbon-number products at 200 °C is significant.},
doi = {10.1016/j.apcatb.2022.122107},
journal = {Applied Catalysis. B, Environmental},
number = ,
volume = 322,
place = {United States},
year = {Fri Oct 28 00:00:00 EDT 2022},
month = {Fri Oct 28 00:00:00 EDT 2022}
}
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