Selective Hydrodeoxygenation of Aromatics to Cyclohexanols over Ru Single Atoms Supported on CeO2

Cyclohexanols are widely used chemicals, which are mainly produced by oxidation of fossil feedstocks. Selective hydrodeoxygenation of lignin derivatives has great potential for producing these chemicals but is challenging to obtain high yields. Here, we report that CeO2-supported Ru single-atom catalysts (SACs) enabled the hydrogenation of the benzene ring and catalyzed etheric C-O(R) bond cleavage without changing the C- O(H) bond, which could afford 99.9% yields of cyclohexanols. As far as we know, this is the first to report that SACs catalyze hydrogenation of the aromatic ring. The reaction mechanism was studied by control experiments and density functional theory calculations. In the catalysts, the Ru-O-Ce sites were formed and one Ru atom was coordinated with about four O atoms. These catalytic sites could realize both the hydrogenation and deoxygenation reactions efficiently, and thus desired cyclohexanols were generated. This work pioneers the single-atom catalysis in aromatic transformation and provides a novel route for synthesis of cyclohexanols.

Automated summary

CeO2-supported Ru single-atom catalysts enable the hydrogenation of the benzene ring and catalyze etheric C-O(R) bond cleavage, leading to high yields of cyclohexanols.