Synergetic Interaction between Single-Atom Cu and Ga 2 O 3 Enhances CO 2 Hydrogenation to Methanol over CuGaZrO x

A Cu-based catalyst has prospects for practical use in selective hydrogenation of CO 2 to methanol. But the catalyst’s structural complexity renders the elucidation of the nature of active sites a challenge. This work reports CuGaZrO x solid solutions with tunable Cu size scales and synergetic interactions between active sites for methanol synthesis. Atomically dispersed Cu species (Cu 1 –O 3 ) adjacent to the Zr site contribute to enhanced capacity for CO 2 adsorption/activation, and Ga sites are primarily responsible for H 2 dissociation over the CuGaZrO x solid solution with isolated Cu species. Further experimental and density functional theory (DFT) calculations reveal that the synergy between Cu and Ga species favors the hydrogenation of CO 2 to form CH 3 OH via a formate pathway while suppressing undesired CO production. This work provides insight into the active site structure and mechanistic pathway over a CuGaZrO x solid solution and efficient catalyst design for CO 2 hydrogenation to methanol.