Dual experimental and computational approach to elucidate the effect of Ga on Cu/CeO2-ZrO2 catalyst for CO2 hydrogenation

Cu-Ga catalysts are potential candidates for activating the selective and stable hydrogenation of carbon dioxide to methanol and dimethyl ether. This work explores the structure-function relationship in specific Cu-Ga/ CeO2-ZrO2 catalysts with different Ga loadings. Combining experiments with density functional theory calcu-lations, we find the most well-balanced Cu-Ga interphase (structure) and promote specific mechanistic pathways of the reaction (function). The experiments yielded the highest selectivity of the desired products when the Cu and Ga amounts were equal. The experimental work and density functional theory calculations demonstrated that methanol is formed through the carboxyl pathway on the Cu catalyst, while Ga promotes the formate pathway. Consequently, the productivities of both methanol and dimethyl ether are enhanced. The experimental results match well with the theoretical calculations. Comparing our results with other Ga-promoting systems, we also prove that Cu achieves better balance than Ni and Co.

Automated summary

This study investigates the structure-function relationship of Cu-Ga/CeO2-ZrO2 catalysts through experiments and theoretical calculations, revealing the most balanced Cu-Ga interphase and specific mechanistic pathways for the reaction. The highest selectivity of the desired products is achieved when the amounts of Cu and Ga are equal. Comparing with other Ga-promoting systems, it is demonstrated that Cu achieves better balance.