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

MollyM.-J. Li, Chunping Chen, Tuğçe Ayvalı, Hongri Suo, Jianwei Zheng, Ivo F. Teixeira, Lin Ye, Hanbo Zou, Dermot O’Hare, Shik Chi Edman Tsang

Index: 10.1021/acscatal.8b00474

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Abstract

Ultrathin (1–3 cationic-layers) (CuZn)1–xGax-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 gMeOH·gcat–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.