Combining computational and experimental studies to gain mechanistic insights for n-butane isomerisation with a model microporous catalyst
Combining computational and experimental studies to gain mechanistic insights for n-butane isomerisation with a model microporous catalyst
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.
Potter, Matthew E.
34dee7dc-2f62-4022-bb65-fc7b7fb526d2
Spiske, Lucas
982dac5a-a3e7-4157-be33-fd223447462c
Plessow, Philipp N.
2d1b0099-9a39-49a7-a97c-80439881c0d6
McShane, Evangeline Bridget
520cad09-cd84-4861-ae29-16414d7dc4c2
Carravetta, Marina
1b12fa96-4a6a-4689-ab3b-ccc68f1d7691
Oakley, Alice Elizabeth
78ad819d-33bb-4c77-af90-9dcc96ed52e0
Bere, Takudzwa
b0182278-9244-420f-ab74-bb752bba0f8b
Carter, James H.
2d28942f-c8d2-4f01-a6af-abc28bcd97b9
Vandegehuchte, Bart D.
c102634f-27ac-4ab6-be84-25fa8c14f7fd
Kaźmierczakf, Kamila M.
3e42f612-0c4b-49bb-99c6-df595d552fc3
Studt, Felix
960c61b7-4d49-4f73-8483-a61c1e4c4fa2
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b
30 October 2024
Potter, Matthew E.
34dee7dc-2f62-4022-bb65-fc7b7fb526d2
Spiske, Lucas
982dac5a-a3e7-4157-be33-fd223447462c
Plessow, Philipp N.
2d1b0099-9a39-49a7-a97c-80439881c0d6
McShane, Evangeline Bridget
520cad09-cd84-4861-ae29-16414d7dc4c2
Carravetta, Marina
1b12fa96-4a6a-4689-ab3b-ccc68f1d7691
Oakley, Alice Elizabeth
78ad819d-33bb-4c77-af90-9dcc96ed52e0
Bere, Takudzwa
b0182278-9244-420f-ab74-bb752bba0f8b
Carter, James H.
2d28942f-c8d2-4f01-a6af-abc28bcd97b9
Vandegehuchte, Bart D.
c102634f-27ac-4ab6-be84-25fa8c14f7fd
Kaźmierczakf, Kamila M.
3e42f612-0c4b-49bb-99c6-df595d552fc3
Studt, Felix
960c61b7-4d49-4f73-8483-a61c1e4c4fa2
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b
Potter, Matthew E., Spiske, Lucas, Plessow, Philipp N., McShane, Evangeline Bridget, Carravetta, Marina, Oakley, Alice Elizabeth, Bere, Takudzwa, Carter, James H., Vandegehuchte, Bart D., Kaźmierczakf, Kamila M., Studt, Felix and Raja, Robert
(2024)
Combining computational and experimental studies to gain mechanistic insights for n-butane isomerisation with a model microporous catalyst.
Catalysis Science & Technology, 14 (24).
(doi:10.1039/D4CY01035C).
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.
Text
d4cy01035c
- Version of Record
More information
Accepted/In Press date: 25 October 2024
Published date: 30 October 2024
Identifiers
Local EPrints ID: 496262
URI: http://eprints.soton.ac.uk/id/eprint/496262
ISSN: 2044-4753
PURE UUID: 14b5a331-1e38-4dfe-b2bd-e560d1c33721
Catalogue record
Date deposited: 10 Dec 2024 17:44
Last modified: 11 Dec 2024 02:44
Export record
Altmetrics
Contributors
Author:
Lucas Spiske
Author:
Philipp N. Plessow
Author:
Evangeline Bridget McShane
Author:
Alice Elizabeth Oakley
Author:
Takudzwa Bere
Author:
James H. Carter
Author:
Bart D. Vandegehuchte
Author:
Kamila M. Kaźmierczakf
Author:
Felix Studt
Download statistics
Downloads from ePrints over the past year. Other digital versions may also be available to download e.g. from the publisher's website.
View more statistics