Synergy in Au-CuO Janus Structure for Catalytic Isopropanol Oxidative Dehydrogenation to Acetone

The controlled oxidation of alcohols to the corresponding ketones or aldehydes via selective cleavage of the beta-C-H bond of alcohols under mild conditions still remains a significant challenge. Although the metal/oxide interface is highly active and selective, the interfacial sites fall far behind the demand, due to the large and thick support. Herein, we successfully develop a unique Au-CuO Janus structure (average particle size=3.8 nm) with an ultrathin CuO layer (0.5 nm thickness) via a bimetal in situ activation and separation strategy. The resulting Au-CuO interfacial sites prominently enhance isopropanol adsorption and decrease the energy barrier of beta-C-H bond scission from 1.44 to 0.01 eV due to the strong affinity between the O atom of CuO and the H atom of isopropanol, compared with Au sites alone, thereby achieving ultrahigh acetone selectivity (99.3 %) over 1.1 wt % AuCu0.75/Al2O3 at 100 degrees C and atmospheric pressure with 97.5 % isopropanol conversion. Furthermore, Au-CuO Janus structures supported on SiO2, TiO2 or CeO2 exhibit remarkable catalytic performance, and great promotion in activity and acetone selectivity is achieved as well for other reducible oxides derived from Fe, Co, Ni and Mn. This study should help to develop strategies for maximized interfacial site construction and structure optimization for efficient beta-C-H bond activation.

Automated summary

In this study, a unique Au-CuO Janus structure is developed through a bimetal in situ activation and separation strategy. This structure exhibits enhanced acetone selectivity and improved alcohol conversion, making it a promising catalyst for controlled oxidation reactions.