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Cobalt-nitrogen co-doped porous carbon sphere as highly efficient catalyst for liquid-phase cyclohexane oxidation with molecular oxygen and the active sites investigation

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Abstract

The selective oxidation of cyclohexane to cyclohexanone and cyclohexanol (KA oil) is a challenging issue in the chemical industry. At present the industrial conversion of cyclohexane to cyclohexanone and cyclohexanol is normally controlled at less than 5% selectivity. Thus, the development of highly active and stable catalysts for the aerobic oxidation of cyclohexane is necessary to overcome this low-efficiency process. Therefore, we have developed a cobalt-nitrogen co-doped porous sphere catalyst, Co-NC-x (x is the Zn/Co molar ratio, where x = 0, 0.5, 1, 2, and 4) by pyrolyzing resorcinol-formaldehyde resin microspheres. It achieved 88.28% cyclohexanone and cyclohexanol selectivity and a cyclohexane conversion of 8.88% under Co-NC-2. The results showed that the introduction of zinc effectively alleviated the aggregation of Co nanoparticles and optimized the structural properties of the material. In addition, Co0 and pyridinic-N are proposed to be the possible active species, and their proportion efficiently increased in the presence of Zn2+ species. In this study, we developed a novel strategy to design highly active catalysts for cyclohexane oxidation.

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Acknowledgements

This work was supported by National Natural Science Foundation of China (Grant No. 22178294), Science and Technology Innovation Program of Hunan Province (Grant No. 2022RC1117), Project of Hunan Provincial Education Department (Grant No. 22A0125), Hunan Provincial Natural Science Foundation of China (Grant No. 2021JJ30663), Postgraduates Scientific Research Innovation Project of Xiangtan University (Grant No. QL20220146), Collaborative Innovation Center of New Chemical Technologies for Environmental Benignity and Efficient Resource Utilization, and Environment-friendly Chemical Process Integration Technology Hunan Province Key laboratory. In addition, we would like to thank KetengEdit for its linguistic assistance during the preparation of this manuscript.

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  1. College of Chemical Engineering, National & Local United Engineering Research Centre for Chemical Process Simulation and Intensification, Xiangtan University, Xiangtan, 411105, China

    Lei Chen, Yuan Sun, Jinshan Chi, Wei Xiong, Pingle Liu & Fang Hao

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  1. Lei Chen
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  2. Yuan Sun
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Correspondence to Wei Xiong or Fang Hao.

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Cobalt-nitrogen co-doped porous carbon sphere as highly efficient catalyst for liquid-phase cyclohexane oxidation with molecular oxygen and the active sites investigation

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Chen, L., Sun, Y., Chi, J. et al. Cobalt-nitrogen co-doped porous carbon sphere as highly efficient catalyst for liquid-phase cyclohexane oxidation with molecular oxygen and the active sites investigation. Front. Chem. Sci. Eng. 18, 33 (2024). https://doi.org/10.1007/s11705-024-2395-3

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