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Research Article

Potassium-promoted single-atom Co-N-C catalyst for direct dehydrogenation of ethylbenzene

Jiajia Shi1,2,§, Yao Wei2,4,5,§, Leilei Zhang1, Dan Zhou1, Zhounan Yu1,2, Shengxin Zhang1,2, Xiaofeng Yang1, Ji Yang1, Yang Su1, Zheng Jiang4,5( ), Aiqin Wang1,3( )
CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
University of Chinese Academy of Sciences, Beijing 100049, China
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China
Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201204, China

§ Jiajia Shi and Yao Wei contributed equally to this work.

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Graphical Abstract

Potassium was introduced to the Co-N-C single-atom catalyst, yielding an outstanding Co-O-K moiety for ethylbenzene dehydrogenation with 9.7 mmolEB·gcat−1·h−1 of steady-state reaction rate.

Abstract

Alkali metals have been widely used as promoters of metal catalysts in various applications, yet the atomic understanding of the promotional mechanism remains elusive. In this work, we for the first time report the significant promotional effect of potassium to the Co-N-C single-atom catalyst for the direct dehydrogenation of ethylbenzene. K cation was introduced by impregnation of Co-N-C with KCl followed by calcination at 600 °C, which resulted in the bonding of K to the Co-O moiety of the Co-N-C catalyst as revealed by X-ray absorption spectroscopy in combination with theoretical calculations. The formation of Co-O-K moiety led to the increase of electron density at the O atom due to electron transfer of K to O, and consequently facilitated the heterolytic cleavage of the C–H bond of ethylbenzene across the Co-O moiety. The promotional effect of K was found to be a volcano-function with the K/Co ratio and became the greatest at the K/Co ratio of 1.36, which resulted in the highest steady-state reaction rate of 9.7 mmolEB·gcat−1·h−1 reported thus far. Moreover, the catalyst exhibited excellent stability during 100 h time on stream.

Keywords

alkali metalpotassiumpromoteralkane dehydrogenationsingle-atom catalystCo-N-C

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Nano Research
Volume 16 Issue 3,
March 2023
Pages 3687-3694
DOI: 10.1007/s12274-022-4828-y
Cite this article:
Shi J, Wei Y, Zhang L, et al. Potassium-promoted single-atom Co-N-C catalyst for direct dehydrogenation of ethylbenzene. Nano Research, 2023, 16(3): 3687-3694. https://doi.org/10.1007/s12274-022-4828-y
Topics:
CarbonCatalyst activityCatalysts
Part of a topical collection:
Women’s Special Issue: Nanomaterials: Preparation, Applications, and Challenges

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Received: 22 June 2022
Revised: 26 July 2022
Accepted: 27 July 2022
Published: 19 August 2022
© Tsinghua University Press 2022
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