Combining computational and experimental studies to gain mechanistic insights for n-butane isomerisation with a model microporous catalyst

Matthew E. Potter; Lucas Spiske; Philipp N. Plessow; Evangeline B. McShane; Marina Carravetta; Alice E. Oakley; Takudzwa Bere; James H. Carter; Bart D. Vandegehuchte; Kamila M. Kaźmierczak; Felix Studt; Robert Raja

doi:10.1039/d4cy01035c

Combining computational and experimental studies to gain mechanistic insights for n-butane isomerisation with a model microporous catalyst

Matthew E. Potter, Lucas Spiske, Philipp N. Plessow, Evangeline B. McShane, Marina Carravetta, Alice E. Oakley, Takudzwa Bere, James H. Carter, Bart D. Vandegehuchte, Kamila M. Kaźmierczak, Felix Studt, Robert Raja

Research output: Contribution to journal › Article › peer-review

Abstract

Microporous solid acid catalysts are widely used in industrial hydrocarbon transformations in both the fuels and petrochemical industries. The specific choice of microporous framework often dictates the acidic properties of the system, such as acid site strength and concentration. In this work we have explored the influence of acid site concentration on butane isomerisation activity and the mechanistic pathway by controlling the quantity of magnesium doped into an aluminophosphate, keeping the acid site strength and framework topology constant. By combining experimental kinetic studies, and theoretical mechanistic studies, we conclude that isobutane formation, from n-butane, predominantly proceeds through a bimolecular pathway. Specifically, the activity of the system is strongly linked to the presence of alkenes, and herein the precise mechanistic roles of the alkenes are explored.

Original language	English
Journal	Catalysis Science and Technology
Early online date	30 Oct 2024
DOIs	https://doi.org/10.1039/d4cy01035c
Publication status	E-pub ahead of print - 30 Oct 2024

Acknowledgements

This study was conducted as part of the Consortium of Metal Nanocatalysis funded by TotalEnergies OneTech Belgium. The authors acknowledge support by the KIT-Publication Fund of the Karlsruhe Institute of Technology. Support from TotalEnergies through Houston HPC computational resources is greatly acknowledged. Prof. Graham Hutchings is thanked for kind access to his groups DRIFTS equipment at Cardiff University.

ASJC Scopus subject areas

Catalysis

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Potter, M. E., Spiske, L., Plessow, P. N., McShane, E. B., Carravetta, M., Oakley, A. E., Bere, T., Carter, J. H., Vandegehuchte, B. D., Kaźmierczak, K. M., Studt, F., & Raja, R. (2024). Combining computational and experimental studies to gain mechanistic insights for n-butane isomerisation with a model microporous catalyst. Catalysis Science and Technology. Advance online publication. https://doi.org/10.1039/d4cy01035c

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AU - Spiske, Lucas

AU - Plessow, Philipp N.

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AU - Carravetta, Marina

AU - Oakley, Alice E.

AU - Bere, Takudzwa

AU - Carter, James H.

AU - Vandegehuchte, Bart D.

AU - Kaźmierczak, Kamila M.

AU - Studt, Felix

AU - Raja, Robert

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Combining computational and experimental studies to gain mechanistic insights for n-butane isomerisation with a model microporous catalyst

Abstract

Acknowledgements

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