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Cobalt single atom site catalysts with ultrahigh metal loading for enhanced aerobic oxidation of ethylbenzene

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Abstract

The oxidation of hydrocarbons to produce high value-added compounds (ketones or alcohols) using oxygen in air as the only oxidant is an efficient synthetic strategy from both environmental and economic views. Herein, we successfully synthesized cobalt single atom site catalysts (Co SACs) with high metal loading of 23.58 wt.% supported on carbon nitride (CN), which showed excellent catalytic properties for oxidation of ethylbenzene in air. Moreover, Co SACs show a much higher turn-over frequency (19.6 h−1) than other reported non-noble catalysts under the same condition. Comparatively, the as-obtained nanosized or homogenous Co catalysts are inert to this reaction. Co SACs also exhibit high selectivity (97%) and stability (unchanged after five runs) in this reaction. DFT calculations reveal that Co SACs show a low energy barrier in the first elementary step and a high resistance to water, which result in the robust catalytic performance for this reaction.

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Acknowledgements

This work was supported by the National Key R&D Program of China (Nos. 2018YFA0702003 and 2016YFA0202801), the National Natural Science Foundation of China (Nos. 21890383, 21671117, 21871159, and 21901135), Science and Technology Key Project of Guangdong Province of China (No. 2020B010188002), Beijing Municipal Science & Technology Commission (No. Z191100007219003) and China Postdoctoral Science Foundation (No. 2018M640114). We thank the BL11B station in Shanghai Synchrotron Radiation Facility (SSRF) for XAFS measurement. We appreciate the BL12B station of National Synchrotron Radiation Laboratory (NRSL) for NEXAFS measurement.

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  1. Yu Xiong, Wenming Sun, and Yunhu Han contributed equally to this work.

Authors and Affiliations

  1. Department of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, China

    Yu Xiong

  2. Department of Chemistry, Tsinghua University, Beijing, 100084, China

    Yu Xiong, Pingyu Xin, Jian Zhang, Dingsheng Wang & Yadong Li

  3. China College of Science, China Agricultural University, Beijing, 100193, China

    Wenming Sun

  4. Institute of Flexible Electronics, Northwestern Polytechnical University, Xi’an, 710072, China

    Yunhu Han

  5. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029, China

    Xusheng Zheng & Wensheng Yan

  6. Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100084, China

    Juncai Dong

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Xiong, Y., Sun, W., Han, Y. et al. Cobalt single atom site catalysts with ultrahigh metal loading for enhanced aerobic oxidation of ethylbenzene. Nano Res. 14, 2418–2423 (2021). https://doi.org/10.1007/s12274-020-3244-4

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