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Designing bimetallic active centres in microporus architectures for synergistic catalysis’

Designing bimetallic active centres in microporus architectures for synergistic catalysis’
Designing bimetallic active centres in microporus architectures for synergistic catalysis’
The introduction of two distinct dopants in a microporous zeotype framework can lead to the formation of isolated, or complementary catalytically active sites. Careful selection of dopants and framework topology can facilitate synergistic enhancements in catalysts efficiency in a range of reaction pathways, leading to the use of sustainable precursors (bioethanol) for plastic production. In this work we describe our unique synthetic design procedure for creating a bimetallic solid-acid catalyst (MgSiAPO-34), designed to improve and contrast with the performance of SiAPO-34 (monometallic analogue), for the dehydration of ethanol to ethylene. We employ a range of in situ characterisation techniques to explore the influence of magnesium substitution, with specific attention to the acidity of the framework. Through a combined catalysis, kinetic analysis and computational fluid dynamics (CFD) study we explore the reaction pathway of the system, with emphasis on the improvements facilitated by the bimetallic MgSiAPO-34 species. The experimental data supports the validation of the CFD results across a range of operating conditions; both of which supports our hypothesis that the presence of the bimetallic solid acid centres enhances the catalytic performance. Furthermore, the development of a robust computational model, capable of exploring chemical catalytic flows within a reactor system, affords further avenues for enhancing reactor engineering and process optimisation, towards improved ethylene yields, under mild conditions.
2296-2646
Potter, Matthew
34dee7dc-2f62-4022-bb65-fc7b7fb526d2
Armstrong, Lindsay-Marie
97effe7b-3d9f-42ab-bbcc-878a4d027ca7
Carravetta, Marina
1b12fa96-4a6a-4689-ab3b-ccc68f1d7691
Mezza, Thomas M.
a77c484c-a79f-4283-90c3-b049b63bdb1c
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b
Potter, Matthew
34dee7dc-2f62-4022-bb65-fc7b7fb526d2
Armstrong, Lindsay-Marie
97effe7b-3d9f-42ab-bbcc-878a4d027ca7
Carravetta, Marina
1b12fa96-4a6a-4689-ab3b-ccc68f1d7691
Mezza, Thomas M.
a77c484c-a79f-4283-90c3-b049b63bdb1c
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b

Potter, Matthew, Armstrong, Lindsay-Marie, Carravetta, Marina, Mezza, Thomas M. and Raja, Robert (2020) Designing bimetallic active centres in microporus architectures for synergistic catalysis’. Frontiers in Chemistry. (doi:10.3389/fchem.2020.00171). (In Press)

Record type: Article

Abstract

The introduction of two distinct dopants in a microporous zeotype framework can lead to the formation of isolated, or complementary catalytically active sites. Careful selection of dopants and framework topology can facilitate synergistic enhancements in catalysts efficiency in a range of reaction pathways, leading to the use of sustainable precursors (bioethanol) for plastic production. In this work we describe our unique synthetic design procedure for creating a bimetallic solid-acid catalyst (MgSiAPO-34), designed to improve and contrast with the performance of SiAPO-34 (monometallic analogue), for the dehydration of ethanol to ethylene. We employ a range of in situ characterisation techniques to explore the influence of magnesium substitution, with specific attention to the acidity of the framework. Through a combined catalysis, kinetic analysis and computational fluid dynamics (CFD) study we explore the reaction pathway of the system, with emphasis on the improvements facilitated by the bimetallic MgSiAPO-34 species. The experimental data supports the validation of the CFD results across a range of operating conditions; both of which supports our hypothesis that the presence of the bimetallic solid acid centres enhances the catalytic performance. Furthermore, the development of a robust computational model, capable of exploring chemical catalytic flows within a reactor system, affords further avenues for enhancing reactor engineering and process optimisation, towards improved ethylene yields, under mild conditions.

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Accepted/In Press date: 25 February 2020

Identifiers

Local EPrints ID: 446672
URI: http://eprints.soton.ac.uk/id/eprint/446672
ISSN: 2296-2646
PURE UUID: c0f27de3-65ee-47d0-b527-b6cd79c24c72
ORCID for Matthew Potter: ORCID iD orcid.org/0000-0001-9849-3306
ORCID for Marina Carravetta: ORCID iD orcid.org/0000-0002-6296-2104
ORCID for Robert Raja: ORCID iD orcid.org/0000-0002-4161-7053

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Date deposited: 17 Feb 2021 17:33
Last modified: 13 Dec 2021 03:05

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Contributors

Author: Matthew Potter ORCID iD
Author: Lindsay-Marie Armstrong
Author: Thomas M. Mezza
Author: Robert Raja ORCID iD

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