CO₂ Hydrogenation to Methanol over Catalysts Derived from Single Cationic Layer CuZnGa LDH Precursors

Ultrathin (1–3 cationic-layers) (CuZn)_1–xGa_x-CO₃ layered double hydroxide (LDH) nanosheets were synthesized following the aqueous miscible organic solvent treatment (AMOST) method and applied as catalyst precursors for methanol production from CO₂ hydrogenation. It is found that, upon reduction, the aqueous miscible organic solvent treated LDH (AMO-LDH) samples above a critical Ga³⁺ composition give consistently and significantly higher Cu surface areas and dispersions than the catalysts prepared from conventional hydroxyl-carbonate phases. Owing to the distinctive local steric and electrostatic stabilization of the ultrathin LDH structure, the newly formed active Cu­(Zn) metal atoms can be stably embedded in the cationic layers, exerting an enhancement to the catalytic reaction. The best catalyst in this study displayed methanol productivity with a space-time yield of 0.6 g_MeOH·g_cat^–1 h^–1 under typical reaction conditions, which, as far as we are aware, is higher than most reported Cu-based catalysts in the literature.