Modulating the Electroactivity of CuCo₂O₄ for Hydrogen Evolution Assisted by Benzyl Alcohol Oxidation via the...

The catalytic activity and morphological structure are closely related. Herein, the spinel structure CuCo₂O₄ with different morphologies was constructed as the research model for the electrocatalytic benzyl alcohol (BA) oxidation and hydrogen evolution reaction (HER). By modulating the morphological structure, oxygen vacancy, and the high valence active centers, the octahedral CuCo₂O₄ exhibited superior electrocatalytic activity and stability compared to other CuCo₂O₄ samples with nanoplate/nanowire morphologies. Meanwhile, density functional theory calculations elucidated that octahedral CuCo₂O₄ could significantly lower the reaction energy barriers of BA oxidation. Furthermore, the crystal orbital Hamilton population analysis was exploited to probe the intermediate adsorption/desorption on the vacancies. The morphology structure and vacancy effect contributed to the improved electrocatalytic performance. The present work demonstrated the important influence of the morphology structure and the accompanying electronic/vacancy effect on the catalytic activity experimentally and theoretically.