Catalytic hydrogenation of CO2 to DME on surface Cu via highly efficient electron redistribution at the Cu0/Cu+ interface

The activity of copper-based bifunctional catalysts for CO2 hydrogenation to dimethyl ether (DME) is generally constrained by the loss of Cu0 sites during the reaction. Previous studies have focused on introducing additional elements to improve the stability of active sites. In this study, an electron redistribution of the Cu/Cu2O interface was constructed. Surface Cu0 provides active sites for H2 adsorption and dissociation, and the Cu0/Cu+ interface sites are more beneficial for the activation and hydrogenation of CO2. The Ointer–H moieties that form at interface sites reduce the reaction energy barrier of CH3OH synthesis, and the decomposition of H2COOH* to CH2O* species is the rate-limiting step. In addition, the Cu0/Cu+ interface restricts the migration of copper species and protects the weak acid sites of HZSM-5 during the reaction. The present work provides an atomic-level description of H2 dissociation and CO2 activation by Cu0/Cu+ surface and interface sites.