Tuning CO2 hydrogenation selectivity via support interface types on Cu-based catalysts

Abstract

Growing interest has been shown in controlling the selectivity of CO2 hydrogenation to produce specific compounds and fuels with additional value. However, it is challenging to selectively generate target products due to the complexity and diversity of the products in CO2 hydrogenation reaction. Herein, we reported a finding in the CO2 hydrogenation reaction: selectivity could be totally reversed by just altering support interface types on Cu-based catalysts. Cu/ZnO-MgO catalysts showed high CH3OH selectivity, while Cu/ZnO-CoO catalysts exhibited good selectivity of CH4. According to in-depth characterization, varied basicity sites most likely as results of the different support interface types. Density functional theory (DFT) calculations pointed that support interface types altered the adsorption position of H2COO* on catalysts and affect the adsorption and activation of intermediates, and thus resulted in noticeably varied product selectivity. This study demonstrated the value of regulating CO2 hydrogenation selectivity via support interface types on Cu-based catalysts, which can aid in the rational design of catalysts for not only CO2 hydrogenation but also other significant reactions.