Boosting Hydrogenation of CO <sub>2</sub> Using Cationic Cu Atomically Dispersed on 2D γ‐Al <sub>2</sub> O <sub>3</sub> Nanosheets
Ping Chen, Yifeng Zhu, Hai‐Lin Zhang, Micah P. Prange, Duo Song, János Szanyi, Yining Wang, Ying Chen, Xiang Wang, Oliver Y. Gutiérrez, Zihua Zhu, Zhe-Ming Wang, Carolyn I. Pearce, Ping Li, Kevin M. Rosso, Honghong Shi, Xin Zhang
Abstract
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.