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13C MAS NMR Mechanistic Study of Propene Transformation on Silver-Modified ZSM-5 Zeolite in the Presence of Molecular Oxygen

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Abstract

Silver-modified zeolites have demonstrated promising properties for hydrocarbon feedstock valorization and the oxidation of organic compounds. Within the frame of the scientific interest for selective oxidation of light alkenes on metal-modified zeolites, the transformation of propene on Ag/H-ZSM-5 zeolite in the presence of molecular oxygen has been monitored by 13C (CP) MAS NMR spectroscopy at 296–773 K. Silver-allyl intermediate species have been detected by 13C CP/MAS NMR, indicating that Ag+ sites are involved in propene transformation. It is assumed that oxygen and propene compete for the Ag+ adsorption sites, thus prompting propene adsorption on zeolite Brønsted acid sites (BAS) and its further transformation by oligomerization and conjunct polymerization. Among the products of propene oxidation by molecular oxygen, only carbon dioxide has been detected by 13C MAS NMR, implying high activity of Ag/H-ZSM-5 in alkene total oxidation. It is thus inferred that silver-modified zeolite is not a promising catalyst for propene selective oxidation to propene oxide and carbonyl group containing organics.

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Acknowledgements

This work was supported by Russian Science Foundation (grant no. 21-73-10013). The maintenance of solid-state NMR and FTIR facilities was supported by the Ministry of Science and Higher Education of the Russian Federation within the governmental assignment for Boreskov Institute of Catalysis (project FWUR-2024-0032).

Funding

Russian Science Foundation (grant no. 21-73-10013). Ministry of Science and Higher Education of the Russian Federation within the governmental assignment for Boreskov Institute of Catalysis (project FWUR-2024-0032).

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Authors and Affiliations

  1. Boreskov Institute of Catalysis, Siberian Branch of the Russian Academy of Sciences, Prospekt Akademika Lavrentieva 5, Novosibirsk, 630090, Russia

    Zoya N. Lashchinskaya, Anton A. Gabrienko, Alexander V. Toktarev & Alexander G. Stepanov

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  1. Zoya N. Lashchinskaya
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  2. Anton A. Gabrienko
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  3. Alexander V. Toktarev
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Contributions

All authors contributed to the study conception and design. Material preparation was performed by Alexander V. Toktarev. Sample preparation and MAS NMR and FTIR measurements were performed by Zoya N. Lashchinskaya and Anton A. Gabrienko. Data analysis and writing of the manuscript were performed by Zoya N. Lashchinskaya, Anton A. Gabrienko, and Alexander G. Stepanov. All authors read and approved the final manuscript.

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Correspondence to Anton A. Gabrienko.

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Lashchinskaya, Z.N., Gabrienko, A.A., Toktarev, A.V. et al. 13C MAS NMR Mechanistic Study of Propene Transformation on Silver-Modified ZSM-5 Zeolite in the Presence of Molecular Oxygen. Appl Magn Reson (2024). https://doi.org/10.1007/s00723-024-01652-0

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