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Research Article

Shedding light on the reversible deactivation of carbon-supported single-atom catalysts in hydrogenation reaction

Runze Chen1,2Xiaoying Wang1Jianfei Dang2Songjie Yun3Liqiang Wang1,2( )Fangong Kong1( )You-Nian Liu4
State Key Laboratory of Biobased Material and Green Papermaking, Qilu University of Technology, Jinan 250353, China
School of Material Science and Engineering, Zhengzhou University, Zhengzhou 450001, China
School of Chemical Engineering, Zhengzhou University, Zhengzhou 450001, China
Hunan Provincial Key Laboratory of Micro & Nano Materials Interface Science, College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China
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Graphical Abstract

A comprehensive examination and analysis of the reversible deactivation mechanism of metal single-atom catalysts supported on heteroatom-doped carbon (M1/HC) during the hydrogenation reaction were undertaken. The findings reveal that the primary cause of deactivation is pore blockage of the carbon support by substrate molecules, and the deactivated catalysts can be restored through thermal treatment, during which, the substrate molecules in the pore channels are removed.

Abstract

Carbon-supported single-atom catalysts were found to suffer reversible deactivation in catalytic hydrogenation, but the mechanism is still unclear. Herein, nitro compounds hydrogenation catalyzed by N-doped carbon-supported Co single atom (Co1/NC) was taken as a model to uncover the mechanism of the reversible deactivation phenomenon. Co1/NC exhibited moderate adsorption towards the substrate molecules (i.e., nitro compounds or related intermediates), which could be strengthened by the confinement effect from the porous structure. Consequently, substrate molecules tend to accumulate within the pore channel, especially micropores that host Co1, making it difficult for the reactants to access the active sites and finally leading to their deactivation. The situation could be even worse when the substrate molecules possess a large size. Nevertheless, the catalytic activity of Co1/NC could be restored via a simple thermal treatment, which could remove the adsorbates within the pore channel, hence releasing active sites that were originally inaccessible to reactants.

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Nano Research
Pages 4807-4814
Cite this article:
Chen R, Wang X, Dang J, et al. Shedding light on the reversible deactivation of carbon-supported single-atom catalysts in hydrogenation reaction. Nano Research, 2024, 17(6): 4807-4814. https://doi.org/10.1007/s12274-024-6449-0
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Received: 19 October 2023
Revised: 06 December 2023
Accepted: 25 December 2023
Published: 25 January 2024
© Tsinghua University Press 2024
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