Boosting Hydrogenation of CO ₂ Using Cationic Cu Atomically Dispersed on 2D γ‐Al ₂ O ₃ Nanosheets

Abstract The continuous development of novel catalytic approaches is crucial for advancing efficient CO 2 hydrogenation processes. Drawing inspiration from single‐atom catalysis and 2D materials, we designed a new 2D single‐atom catalyst with excellent thermal stability by thermally treating Cu‐adsorbed γ‐AlOOH nanosheets, which yielded a Cu/γ‐Al 2 O 3 catalyst with high activity in the hydrogenation of CO 2 ‐yielding methanol (CH 3 OH), dimethyl ether (DME), and CO as products. The active Cu sites are monodispersed and highly stable due to their cationic oxidation state and their substitution for pentacoordinated aluminum (Al P ) sites on particle surfaces. This study demonstrates an efficient approach for achieving a high CO 2 hydrogenation rate (30.45 mol mol −1 h −1 ) using a catalyst system that lacks metallic Cu centers, traditionally considered essential for H₂ dissociation, and employs what was previously thought to be an inert metal oxide (γ‐Al 2 O 3 ) for CO and CH 3 OH production. Ongoing mechanistic studies aim to elucidate the synergy between cationic Cu single atoms and γ‐Al 2 O 3 , a Lewis acid support, in facilitating hydrogen (H 2 ) activation and methanol formation.