Boosting Hydrogenation of CO Using Cationic Cu Atomically Dispersed on 2D γ-AlO Nanosheets.

The continuous development of novel catalytic approaches is crucial for advancing efficient CO 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-AlO catalyst with high activity in the hydrogenation of CO-yielding methanol (CHOH), 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) sites on particle surfaces. This study demonstrates an efficient approach for achieving a high CO hydrogenation rate (30.45 mol mol h) 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-AlO) for CO and CHOH production. Ongoing mechanistic studies aim to elucidate the synergy between cationic Cu single atoms and γ-AlO, a Lewis acid support, in facilitating hydrogen (H) activation and methanol formation.