Mechanism and kinetics for methanol synthesis from CO₂/H₂ over Cu and Cu/oxide surfaces: Recent investigations by first-principles-based simulation

Abstract

The efficient fixation and utilization of CO₂ has been consistently pursued by chemists for decades. Although Cu-based catalysts, e.g., Cu/ZnO/Al₂O₃, have been widely used in industry for methanol synthesis from CO₂ hydrogenation (CO₂ + 3H₂→H₃COH+ H₂O), many issues on the mechanism and the kinetics remain largely uncertain. For example, the surface site for CO₂ activation and the synergetic effect between Cu and oxide have been hotly debated in literature. In the past few years, theoretical modeling on pure Cu surfaces and Cu/oxide interfaces has been utilized to provide insight into these important questions. Here we will review the recent theoretical advances on simulating this complex heterogeneous catalytic process with first principles density functional theory (DFT) calculations and kinetics modeling. The theoretical results on the mechanism and the kinetics are compared and summarized.

Keywords

density functional theory calculation / CO₂ hydrogenation / methanol synthesis / Cu-based catalysts / review

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