Methanol Synthesis by Hydrogenation of Hybrid CO2−CO Feeds

The impact of carbon monoxide on CO2‐to‐methanol catalysts has been scarcely investigated, although CO will comprise up to half of the carbon feedstock, depending on the origin of CO2 and process configuration. In this study, copper‐based systems and ZnO−ZrO2 are assessed in cycling experiments with...

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Published in:ChemSusChem Vol. 14; no. 14; pp. 2914 - 2923
Main Authors: Araújo, Thaylan Pinheiro, Hergesell, Adrian H., Faust‐Akl, Dario, Büchele, Simon, Stewart, Joseph A., Mondelli, Cecilia, Pérez‐Ramírez, Javier
Format: Journal Article
Language:English
Published: Weinheim Wiley Subscription Services, Inc 22.07.2021
Subjects:
Carbon
Carbon dioxide
Carbon monoxide
Catalysts
Copper
heterogeneous catalysis
hybrid feeds
Hydrogenation
Indium oxides
Methanol
methanol synthesis
Zinc oxide
Zirconium dioxide
ISSN:1864-5631, 1864-564X, 1864-564X
Online Access:Get full text
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Summary:The impact of carbon monoxide on CO2‐to‐methanol catalysts has been scarcely investigated, although CO will comprise up to half of the carbon feedstock, depending on the origin of CO2 and process configuration. In this study, copper‐based systems and ZnO−ZrO2 are assessed in cycling experiments with hybrid CO2−CO feeds and their CO sensitivity is compared to In2O3‐based materials. All catalysts are found to be promoted upon CO addition. Copper‐based systems are intrinsically more active in CO hydrogenation and profit from exploiting this carbon source for methanol production, whereas CO induces surplus formation of oxygen vacancies (i. e., the catalytic sites) on ZnO−ZrO2, as in In2O3‐based systems. Mild‐to‐moderate deactivation occurs upon re‐exposure to CO2‐rich streams, owing to water‐induced sintering for all catalysts except ZnO−ZrO2, which responds reversibly to feed variations, likely owing to its more hydrophobic nature and the atomic mixing of its metal components. Catalytic systems are categorized for operation in hybrid CO2−CO feeds, emphasizing the significance of catalyst and process design to foster advances in CO2 utilization technologies. CO gives and takes: The impact of CO on copper and ZnO−ZrO2 catalysts for CO2‐to‐methanol is assessed in cycling tests with hybrid CO2−CO feeds and contrasted to In2O3‐based systems. CO addition promotes all catalyst families for structural and mechanistic reasons. Mild‐to‐moderate deactivation is observed upon its removal for copper‐ and In2O3‐based catalysts, owing to sintering, whereas ZnO−ZrO2 stands out for its fully reversible behavior.
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ISSN:1864-5631
1864-564X
1864-564X
DOI:10.1002/cssc.202100859