Abstract
The decarboxylation pathway in ethanol steam reforming ultimately favors higher selectivity to hydrogen over the decarbonylation mechanism. The addition of an optimized amount of Cs to Pt/m-ZrO2 catalysts increases the basicity and promotes the decarboxylation route, converting ethanol to mainly H2, CO2, and CH4 at low temperature with virtually no decarbonylation being detected. This offers the potential to feed the product stream into a conventional methane steam reformer for the production of hydrogen with higher selectivity. DRIFTS and the temperatureprogrammed reaction of ethanol steam reforming, as well as fixed bed catalyst testing, revealed that the addition of just 2.9% Cs was able to stave off decarbonylation almost completely by attenuating the metallic function. This occurs with a decrease in ethanol conversion of just 16% relative to the undoped catalyst. In comparison with our previous work with Na, this amount is—on an equivalent atomic basis—just 28% of the amount of Na that is required to achieve the same effect. Thus, Cs is a much more efficient promoter than Na in facilitating decarboxylation.
| Original language | English |
|---|---|
| Article number | 1104 |
| Journal | Catalysts |
| Volume | 11 |
| Issue number | 9 |
| DOIs | |
| State | Published - Sep 2021 |
Bibliographical note
Publisher Copyright:© 2021 by the authors. Licensee MDPI, Basel, Switzerland.
Funding
Acknowledgments: Argonne’s research was supported in part by the U.S. Department of Energy (DOE), Office of Fossil Energy, National Energy Technology Laboratory (NETL). Advanced photon source was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract number DE-AC02-06CH11357. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. CAER research was supported by the Commonwealth of Kentucky. Caleb D. Watson would like to acknowledge funding from a UTSA College of Engineering Scholarship. Gary Jacobs would like to thank UTSA and the State of Texas for financial support through startup funds. We also thank Shelley D. Hopps at the University of Kentucky Center for Applied Energy Research for assistance with the X-ray diffraction measurements. Caleb D. Watson would like to acknowledge support from the Undergraduate NSF Research Program, supported by the National Science Foundation through grant award #1832388.
| Funders | Funder number |
|---|---|
| Southwest Texas State University | |
| Office of Fossil Energy and Carbon Management | |
| The University of Texas Health Science Center at San Antonio | |
| U.S. Department of Energy | |
| Office of Science Programs | |
| National Energy Technology Laboratory | |
| National Science Foundation Arctic Social Science Program | 1832388 |
| DOE Basic Energy Sciences | DE-AC02-06CH11357 |
Keywords
- Cs doping
- Decarbonylation
- Decarboxylation
- DRIFTS
- Ethanol steam reforming (ESR)
- Zirconia
ASJC Scopus subject areas
- Catalysis
- General Environmental Science
- Physical and Theoretical Chemistry
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