Ultrasound-assisted co-precipitation synthesis of mesoporous Co₃O₄–CeO₂ composite oxides for highly selective catalytic oxidation of cyclohexane

Abstract

The one-step highly selective oxidation of cyclohexane into cyclohexanone and cyclohexanol as the essential intermediates of nylon-6 and nylon-66 is considerably challenging. Therefore, an efficient and low-cost catalyst must be urgently developed to improve the efficiency of this process. In this study, a Co₃O₄–CeO₂ composite oxide catalyst was successfully prepared through ultrasound-assisted co-precipitation. This catalyst exhibited a higher selectivity to KA-oil, which was benefited from the synergistic effects between Co³⁺/Co²⁺ and Ce⁴⁺/Ce³⁺ redox pairs, than bulk CeO₂ and/or Co₃O₄. Under the optimum reaction conditions, 89.6% selectivity to KA-oil with a cyclohexane conversion of 5.8% was achieved over Co₃O₄–CeO₂. Its catalytic performance remained unchanged after five runs. Using the synergistic effects between the redox pairs of different transition metals, this study provides a feasible strategy to design high-performance catalysts for the selective oxidation of alkanes.

Key words： Co₃O₄–CeO₂ composite oxides; cyclohexanone; cyclohexanol; ultrasonic-assisted co-precipitation; selective oxidation; solvent-free

Acknowledgements

This work was financially supported by Key Research and Development Program in Hunan Province (Grant No. 2019GK2041), Hunan Provincial Natural Science Foundation of China (Grant No. 2019JJ50579), Scientific Research Fund of Hunan Provincial Education Department (Grant Nos. 18C0106 and 20B550), the fund of the Key Laboratory of Catalysis and Energy Materials Chemistry of Ministry of Education & Hubei Key Laboratory of Catalysis and Materials Science (Grant No. CHCL21004), National Training Program of Innovation and Entrepreneurship for Undergraduates (Grant No. S202010530022), and Hunan Key Laboratory of Environment Friendly Chemical Process Integrated Technology and Collaborative Innovation Center of New Chemical Technologies for Environmental Benignity and Efficient Resource Utilization.

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