Parahydrogen-Induced Polarization in Gas-Phase Heterogeneous Hydrogenation of Epoxides | Sciact - CRIS-system of Boreskov Institute of Catalysis

Parahydrogen-Induced Polarization in Gas-Phase Heterogeneous Hydrogenation of Epoxides Full article

Journal

The Journal of Physical Chemistry C
ISSN: 1932-7447 , E-ISSN: 1932-7455

Output data

Year: 2023, Volume: 127, Number: 49, Pages: 23634–23644 Pages count : 11 DOI: 10.1021/acs.jpcc.3c05059

Authors

Salnikov Oleg G. ¹ , Pokochueva Ekaterina V. ^1,3 , Burueva Dudari B. ¹ , Kovtunova Larisa M. ^2,1 , Kovtunov Kirill V. ¹ , Koptyug Igor V. ¹

Affiliations

1	International Tomography Center SB RAS, 3A Institutskaya St., 630090 Novosibirsk, Russia
2	Boreskov Institute of Catalysis SB RAS, 5 Acad. Lavrentiev Pr., 630090 Novosibirsk, Russia
3	Universite Claude Bernard Lyon 1, CRMN UMR-5082, CNRS, ENS Lyon, Villeurbanne 69100, France

Funding (3)

1	Council for Grants of the President of the Russian Federation	МК-2826.2022.1.3
2	Russian Science Foundation	23-23-00394
3	Russian Science Foundation	19-13-00172-П

Hydrogenation of epoxides is a reaction of both fundamental and practical importance. Herein, gas-phase heterogeneous hydrogenation of saturated and unsaturated epoxides over titania-supported Pt, Pd, and Rh catalysts was investigated using the parahydrogen-induced polarization (PHIP) technique. Hydrogenation of saturated epoxides (ethylene oxide and propylene oxide) yielded alcohols, carbonyl compounds, alkenes, and alkanes. While all three catalysts under study isomerized epoxides to carbonyl compounds in the presence of H2, only Pd/TiO2 showed catalytic activity under inert atmosphere, implying that on Pt and Rh catalysts, the epoxide C–O bond can be cleaved only simultaneously with H atom addition to form alkoxy species. PHIP effects were detected for propane and propylene but not for alcohols. Hydrogenation of bifunctional epoxide 3,4-epoxy-1-butene yielded 11 reaction products. Adsorption of the reactant via its C═C bond is followed by hydrogen addition, resulting in the formation of 1,2-epoxybutane, which does not react further. Alternatively, the reactant can be adsorbed via both its C═C bond and the oxygen atom, leading to the formation of crotonaldehyde, butanal, crotyl alcohol, 1-butanol, methyl 1-propenyl ether, methyl propyl ether, 1,3-butadiene, 1-butene, 2-butene, and butane. Based on the PHIP effects observation, the mechanisms of the corresponding processes were proposed.

Salnikov O.G. , Pokochueva E.V. , Burueva D.B. , Kovtunova L.M. , Kovtunov K.V. , Koptyug I.V.
Parahydrogen-Induced Polarization in Gas-Phase Heterogeneous Hydrogenation of Epoxides
The Journal of Physical Chemistry C. 2023. V.127. N49. P.23634–23644. DOI: 10.1021/acs.jpcc.3c05059 WOS Scopus РИНЦ ANCAN OpenAlex

Submitted:	Jul 27, 2023
Accepted:	Nov 21, 2023
Published online:	Dec 6, 2023
Published print:	Dec 14, 2023

Web of science:	WOS:001125232200001
Scopus:	2-s2.0-85180113180
Elibrary:	56738123
Chemical Abstracts:	2023:2513605
Chemical Abstracts (print):	185:90503
OpenAlex:	W4389388387

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OpenAlex	2
Scopus	2
Web of science	2
Elibrary	1