Controlling selectivities in CO2 reduction through mechanistic understanding
Abstract
Catalytic CO2 conversion to energy carriers and intermediates is of utmost importance to energy and environmental goals. However, the lack of fundamental understanding of the reaction mechanism renders designing a selective catalyst inefficient. We performed operando FTIR/SSITKA experiments to understand the correlation between the kinetics of product formation and that of surface species conversion during CO2 reduction over Pd/Al2O3 catalysts. We found that the rate-determining step for CO formation is the conversion of adsorbed formate, while that for CH4 formation is the hydrogenation of adsorbed carbonyl. The balance of the hydrogenation kinetics between adsorbed formates and carbonyls governs the selectivities to CH4 and CO. As a result, we demonstrated how this knowledge can be used to design catalysts to achieve high selectivities to desired products.
- Authors:
-
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1406770
- Report Number(s):
- PNNL-SA-123127
Journal ID: ISSN 2041-1723; KC0302010
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Wang, Xiang, Shi, Hui, and Szanyi, Janos. Controlling selectivities in CO2 reduction through mechanistic understanding. United States: N. p., 2017.
Web. doi:10.1038/s41467-017-00558-9.
Wang, Xiang, Shi, Hui, & Szanyi, Janos. Controlling selectivities in CO2 reduction through mechanistic understanding. United States. https://doi.org/10.1038/s41467-017-00558-9
Wang, Xiang, Shi, Hui, and Szanyi, Janos. Mon .
"Controlling selectivities in CO2 reduction through mechanistic understanding". United States. https://doi.org/10.1038/s41467-017-00558-9. https://www.osti.gov/servlets/purl/1406770.
@article{osti_1406770,
title = {Controlling selectivities in CO2 reduction through mechanistic understanding},
author = {Wang, Xiang and Shi, Hui and Szanyi, Janos},
abstractNote = {Catalytic CO2 conversion to energy carriers and intermediates is of utmost importance to energy and environmental goals. However, the lack of fundamental understanding of the reaction mechanism renders designing a selective catalyst inefficient. We performed operando FTIR/SSITKA experiments to understand the correlation between the kinetics of product formation and that of surface species conversion during CO2 reduction over Pd/Al2O3 catalysts. We found that the rate-determining step for CO formation is the conversion of adsorbed formate, while that for CH4 formation is the hydrogenation of adsorbed carbonyl. The balance of the hydrogenation kinetics between adsorbed formates and carbonyls governs the selectivities to CH4 and CO. As a result, we demonstrated how this knowledge can be used to design catalysts to achieve high selectivities to desired products.},
doi = {10.1038/s41467-017-00558-9},
journal = {Nature Communications},
number = 1,
volume = 8,
place = {United States},
year = {2017},
month = {9}
}
Web of Science
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