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Research Article | Open Access

Regulation of cobalt active sites by antimony to match adsorption configuration for propyne semihydrogenation

Xiaohu Ge1, Ziyue Kou1, Nina Fei1, Yueqiang Cao1 ( ), Hao Jiang2, Xinggui Zhou1, Xuezhi Duan1 ( )
State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, China
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Graphical Abstract

Catalytic hydrogenation pathways, exemplified by propyne semihydrogenation, are regulated by constructing a CoSb intermetallic catalyst. The Co active sites, tailored by high-electronegativity Sb sites, suppress strong σadsorption and facilitate weak π-adsorption of propylene, thereby enhancing propyne semihydrogenation.

Abstract

Designing and fabricating atomically uniform active sites toward favorable adsorption configuration of essential species to match specific reaction pathways is of great importance in catalytic semihydrogenations, yet it remains challenging. In this research, we present a straightforward method for synthesizing a CoSb intermetallic catalyst through the structural conversion of layered double hydroxide precursors, optimizing Co sites for configuration matching in propyne semihydrogenation. Characterizations using X-ray diffraction, high resolution transmission electron microscopy, and X-ray absorption spectroscopy demonstrate the formation of P63/mmc CoSb intermetallic phase. The CoSb intermetallic catalyst, with its well-organized atomic surface and optimized electronic structure, achieves 97.0% propylene selectivity with nearly complete propyne conversion. Temperature-programmed surface reaction and desorption measurements, along with theoretical calculations, unravel that this exceptional selectivity arises from the kinetically preferred desorption of propylene over its further hydrogenation to undesired propane byproduct on the finely regulated Co sites of the CoSb intermetallic catalyst.

Keywords

Propyne semihydrogenationCo–Sb intermetallicadsorption behaviorsite isolationpropylene selectivity

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Carbon Future
Volume 1 Issue 3,
September 2024
Article number: 9200020
DOI: 10.26599/CF.2024.9200020
Cite this article:
Ge X, Kou Z, Fei N, et al. Regulation of cobalt active sites by antimony to match adsorption configuration for propyne semihydrogenation. Carbon Future, 2024, 1(3): 9200020. https://doi.org/10.26599/CF.2024.9200020

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Received: 06 August 2024
Revised: 20 September 2024
Accepted: 25 September 2024
Published: 29 September 2024
© The Author(s) 2024.

Open Access This article is licensed under a Creative Commons Attribution 4.0 International License (CC BY 4.0), which permits reusers to distribute, remix, adapt, and build upon the material in any medium or format, so long as attribution is given to the original author(s) and the source, provide a link to the license, and indicate if changes were made. See https://creativecommons.org/licenses/by/4.0/.
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