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Propane Dehydrogenation on Co-N-C/SiO2 Catalyst: The Role of Single-Atom Active Sites Full article

Journal Catalysts
ISSN: 2073-4344
Output data Year: 2022, Volume: 12, Number: 10, Article number : 1262, Pages count : 15 DOI: 10.3390/catal12101262
Tags propylene; propane dehydrogenation; cobalt–nitrogen–carbon catalyst; mechanistic aspects
Authors Chernov Aleksey N. 1 , Sobolev Vladimir I. 1 , Gerasimov Evgeny Yu. 1 , Koltunov Konstantin Yu. 1
Affiliations
1 Boreskov Institute of Catalysis, Russian Academy of Sciences, Pr. Akademika Lavrentieva, 5, 630090 Novosibirsk, Russia

Funding (1)

1 Ministry of Science and Higher Education of the Russian Federation 0239-2021-0009

Abstract: Recently, significant attention has been drawn to carbon materials containing cobalt coordinated to nitrogen, as the promising inexpensive catalysts of a wide range of applications. Given that non-oxidative propane dehydrogenation to propylene (PDH) is also becoming increasingly important, we present the results on PDH over Co-N-C/SiO2 composites. The latter were prepared by pyrolysis of silicone gel enriched with Co(II) salt and triethanolamine. According to XRD, HRTEM and XPS characterizations, the resulting materials consist of metallic cobalt nanoparticles of about 5 to 10 nm size and subnano-sized cobalt species (cobalt single atom sites coordinated to nitrogen/carbon), which are uniformly distributed in mesoporous silica of high specific surface area (up to 500 m2 g−1). The composites demonstrated significant catalytic activity in PDH, which was examined under typical reaction conditions (600 °C, 1 atm) using a fixed bed flow reactor. The subnano-sized Co centers proved to be the real active catalytic sites responsible for the target reaction, while carbon deposition induced by Co nanoparticles provided the catalyst deactivation. It is shown that the catalyst can be reactivated by the treatment with oxygen, which, in addition, notably increases selectivity to propylene (up to 98%) and enhances the catalyst stability in the next operation cycle. This remarkable change in catalytic behavior is shown to be due to the dramatic structural modification of the catalyst upon high-temperature oxidation
Cite: Chernov A.N. , Sobolev V.I. , Gerasimov E.Y. , Koltunov K.Y.
Propane Dehydrogenation on Co-N-C/SiO2 Catalyst: The Role of Single-Atom Active Sites
Catalysts. 2022. V.12. N10. 1262 :1-15. DOI: 10.3390/catal12101262 WOS Scopus РИНЦ AN OpenAlex
Dates:
Submitted: Sep 15, 2022
Accepted: Oct 13, 2022
Published print: Oct 17, 2022
Published online: Oct 17, 2022
Identifiers:
Web of science: WOS:000872592900001
Scopus: 2-s2.0-85140824628
Elibrary: 53213430
Chemical Abstracts: 2022:2754245
OpenAlex: W4306652923
Citing:
DB Citing
Scopus 8
Web of science 8
Elibrary 7
OpenAlex 11
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