Effect of operating parameters on H2/CO2 conversion to methanol over Cu-Zn oxide supported on ZrO2 polymorph catalysts: Characterization and kinetics

Kinetic aspects of the operating parameters for the catalytic conversion of H2/CO2 to methanol over two novel catalysts were evaluated to understand the effect of the polymorphic ZrO2 phase composed of Cu0/+-ZnO sites at the atomic level and its impact on the reaction mechanism. The catalysts were c...

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Bibliographic Details
Published in:Chemical engineering journal (Lausanne, Switzerland : 1996) Switzerland : 1996), 2021-06, Vol.427
Main Authors: Marcos, Francielle C. F., Cavalcanti, Fabio M., Petrolini, Davi D., Lin, Lili, Betancourt, Luis E., Senanayake, Sanjaya D., Rodriguez, José A., Assaf, José M., Giudici, Reinaldo, Assaf, Elisabete M.
Format: Article
Language:English
Subjects:
carbon dioxide
CO2 hydrogenation
copper
hydrogen
kinetics
MATERIALS SCIENCE
methanol
reaction mechanism
zinc oxide
zirconia polymorphs
zirconia-supported catalysts
zirconium oxide
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Summary:Kinetic aspects of the operating parameters for the catalytic conversion of H2/CO2 to methanol over two novel catalysts were evaluated to understand the effect of the polymorphic ZrO2 phase composed of Cu0/+-ZnO sites at the atomic level and its impact on the reaction mechanism. The catalysts were characterized by in situ and ex-situ XRD, N2 adsorption/desorption isotherms, FRX, TPR, TPD-N2O, in situ XANES, TPD-CO2, and in situ DRIFTS techniques. The influence of different reaction variables such as the GHSV, temperature, pressure, and H2/CO2 ratio were studied using a fixed bed continuous plug flow reactor. The Cu-ZnO catalyst supported on the tetragonal zirconia polymorph exhibited the highest methanol yield due to the lower activation energy when compared to the catalyst with a greater amount of the monoclinic phase. In addition, the catalysts were reused for 8 cycles of 6 hours to evaluate their stability, which can translate into lower costs for large-scale methanol production. As a result, the estimation of the kinetic parameters over Cu-Zn oxide supported on ZrO2 polymorphs was significant for understanding the reaction mechanism, as well as to provide a pathway for scaling-up of the process.
ISSN:1385-8947
1873-3212