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

2021; Elsevier BV; Volume: 427; Linguagem: Inglês

10.1016/j.cej.2021.130947

1873-3212

Francielle Candian Firmino Marcos, Fábio Machado Cavalcanti, Davi D. Petrolini, Lili Lin, Luis E. Betancourt, Sanjaya D. Senanayake, José A. Rodríguez, José Mansur Assaf, Reinaldo Giudici, Elisabete M. Assaf,

CO2 Reduction Techniques and Catalysts

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 h to evaluate their stability, which can translate into lower costs for large-scale methanol production. The estimation of the kinetic parameters for the Cu-Zn oxide catalysts supported on ZrO2 polymorphs was important to understand the reaction mechanism, as well as to provide useful information for scaling up the process.