Layered Double Hydroxides/Metal–Organic Framework Composite Derived Ultrathin Cu/Co/Al Nanocatalyst for Syngas-to-Higher Alcohol Reaction

Direct synthesis of alcohols from carbon monoxide has attracted considerable attention due to their applications as fuel additives and key intermediates in various chemical processes. In this study, CoAl-LDH was employed as the catalyst support to design hierarchical 2-D flaky Cu/Co/Al nanocatalysts by compositing with a copper-based metal–organic framework for efficient higher alcohol production from CO. Uniform loading of Cu-BTC on the CoAl-LDH surface was achieved via in situ growth under mild conditions. Acetone pretreatment effectively exfoliated the CoAl-LDH layers, significantly increasing the specific surface area and Cu-BTC loading. After high-temperature calcination, Cu was uniformly dispersed on the acetone-treated CoAl-LDH derived oxide surface, and the strengthened Cu–Co interaction contributed to enhanced catalytic performance with increased surface hydroxylation and low-valence oxygen species. The optimal catalyst, CCA-ALDO, achieved a CO conversion of 35.2%, R–OH selectivity of 54.6%, with C2+ OH accounting for 85.2%, and a space-time yield of 0.184 g·gcat–1·h–1. This work highlights the role of CoAl-LDH as an effective support and shows that acetone exfoliation enhances catalyst dispersion and metal synergy, providing an efficient approach for CO-to-C2+OH conversion.