Influence of Cs Promoter on Ethanol Steam-Reforming Selectivity of Pt/m-ZrO<sub>2</sub> Catalysts at Low Temperature

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-ZrO<sub>2</sub> catalysts increases the basicity and promotes the decarboxylation route, convertin...

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Main Authors: Zahra Rajabi, Li Jones, Michela Martinelli, Dali Qian, Donald C. Cronauer, A. Jeremy Kropf, Caleb D. Watson, Gary Jacobs
Format: Article
Language:English
Published: MDPI AG 2021-09-01
Series:Catalysts
Subjects:
Online Access:https://www.mdpi.com/2073-4344/11/9/1104
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author Zahra Rajabi
Li Jones
Michela Martinelli
Dali Qian
Donald C. Cronauer
A. Jeremy Kropf
Caleb D. Watson
Gary Jacobs
author_facet Zahra Rajabi
Li Jones
Michela Martinelli
Dali Qian
Donald C. Cronauer
A. Jeremy Kropf
Caleb D. Watson
Gary Jacobs
author_sort Zahra Rajabi
collection DOAJ
description 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-ZrO<sub>2</sub> catalysts increases the basicity and promotes the decarboxylation route, converting ethanol to mainly H<sub>2</sub>, CO<sub>2</sub>, and CH<sub>4</sub> 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 temperature-programmed 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.
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spelling doaj.art-d370712b0c1d42bba45c52ee5e7822d62023-11-22T12:21:27ZengMDPI AGCatalysts2073-43442021-09-01119110410.3390/catal11091104Influence of Cs Promoter on Ethanol Steam-Reforming Selectivity of Pt/m-ZrO<sub>2</sub> Catalysts at Low TemperatureZahra Rajabi0Li Jones1Michela Martinelli2Dali Qian3Donald C. Cronauer4A. Jeremy Kropf5Caleb D. Watson6Gary Jacobs7Department of Biomedical Engineering and Chemical Engineering, University of Texas at San Antonio, One UTSA Circle, San Antonio, TX 78249, USADepartment of Biomedical Engineering and Chemical Engineering, University of Texas at San Antonio, One UTSA Circle, San Antonio, TX 78249, USAUniversity of Kentucky Center for Applied Energy Research, 2540 Research Park Drive, Lexington, KY 40511, USAUniversity of Kentucky Electron Microscopy Center, University of Kentucky, ASTeCC Building—Room A004, Lexington, KY 40508, USAArgonne National Laboratory, Lemont, IL 60439, USAArgonne National Laboratory, Lemont, IL 60439, USADepartment of Biomedical Engineering and Chemical Engineering, University of Texas at San Antonio, One UTSA Circle, San Antonio, TX 78249, USADepartment of Biomedical Engineering and Chemical Engineering, University of Texas at San Antonio, One UTSA Circle, San Antonio, TX 78249, USAThe 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-ZrO<sub>2</sub> catalysts increases the basicity and promotes the decarboxylation route, converting ethanol to mainly H<sub>2</sub>, CO<sub>2</sub>, and CH<sub>4</sub> 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 temperature-programmed 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.https://www.mdpi.com/2073-4344/11/9/1104ethanol steam reforming (ESR)DRIFTSCs dopingzirconiadecarboxylationdecarbonylation
spellingShingle Zahra Rajabi
Li Jones
Michela Martinelli
Dali Qian
Donald C. Cronauer
A. Jeremy Kropf
Caleb D. Watson
Gary Jacobs
Influence of Cs Promoter on Ethanol Steam-Reforming Selectivity of Pt/m-ZrO<sub>2</sub> Catalysts at Low Temperature
Catalysts
ethanol steam reforming (ESR)
DRIFTS
Cs doping
zirconia
decarboxylation
decarbonylation
title Influence of Cs Promoter on Ethanol Steam-Reforming Selectivity of Pt/m-ZrO<sub>2</sub> Catalysts at Low Temperature
title_full Influence of Cs Promoter on Ethanol Steam-Reforming Selectivity of Pt/m-ZrO<sub>2</sub> Catalysts at Low Temperature
title_fullStr Influence of Cs Promoter on Ethanol Steam-Reforming Selectivity of Pt/m-ZrO<sub>2</sub> Catalysts at Low Temperature
title_full_unstemmed Influence of Cs Promoter on Ethanol Steam-Reforming Selectivity of Pt/m-ZrO<sub>2</sub> Catalysts at Low Temperature
title_short Influence of Cs Promoter on Ethanol Steam-Reforming Selectivity of Pt/m-ZrO<sub>2</sub> Catalysts at Low Temperature
title_sort influence of cs promoter on ethanol steam reforming selectivity of pt m zro sub 2 sub catalysts at low temperature
topic ethanol steam reforming (ESR)
DRIFTS
Cs doping
zirconia
decarboxylation
decarbonylation
url https://www.mdpi.com/2073-4344/11/9/1104
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