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Nano Research 2021, 14(7): 2418-2423 https://doi.org/10.1007/s12274-020-3244-4
Research Article | Issue | Published: 05 July 2021

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

Show Author's Information Yu Xiong1,2,§,  Wenming Sun3,§,  Yunhu Han4,§,  Pingyu Xin2,  Xusheng Zheng5,  Wensheng Yan5,  Juncai Dong6,  Jian Zhang2,  Dingsheng Wang2( ),  Yadong Li2
Department of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China
Department of Chemistry, Tsinghua University, Beijing 100084, China
China College of Science, China Agricultural University, Beijing 100193, China
Institute of Flexible Electronics, Northwestern Polytechnical University, Xi’an 710072, China
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, China
Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100084, China

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

Keywords:
heterogeneous catalysts, single atom site, high-loading catalysts, ethylbenzene oxidation
Topics:
Carbon nitrideCatalytic oxidation NanocatalystsOxidation
Cite this article:
Xiong Y, Sun W, Han Y, et al. Cobalt single atom site catalysts with ultrahigh metal loading for enhanced aerobic oxidation of ethylbenzene. Nano Research, 2021, 14(7): 2418-2423. https://doi.org/10.1007/s12274-020-3244-4
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Abstract Full text Electronic supplementary material About this article

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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Electronic supplementary material
About this article

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

Show Author's information Yu Xiong1,2,§, Wenming Sun3,§, Yunhu Han4,§, Pingyu Xin2, Xusheng Zheng5, Wensheng Yan5, Juncai Dong6, Jian Zhang2, Dingsheng Wang2( ), Yadong Li2
Department of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China
Department of Chemistry, Tsinghua University, Beijing 100084, China
China College of Science, China Agricultural University, Beijing 100193, China
Institute of Flexible Electronics, Northwestern Polytechnical University, Xi’an 710072, China
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, China
Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100084, China

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

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.

Keywords: heterogeneous catalysts, single atom site, high-loading catalysts, ethylbenzene oxidation

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Publication history
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Acknowledgements

Publication history

Received: 04 October 2020
Revised: 10 November 2020
Accepted: 13 November 2020
Published: 05 July 2021
Issue date: July 2021

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2020

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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