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.
Potter, Matthew
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Armstrong, Lindsay-Marie
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Carravetta, Marina
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Mezza, Thomas M.
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Raja, Robert
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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)
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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fchem-08-00171
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Accepted/In Press date: 25 February 2020
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Local EPrints ID: 446672
URI: http://eprints.soton.ac.uk/id/eprint/446672
ISSN: 2296-2646
PURE UUID: c0f27de3-65ee-47d0-b527-b6cd79c24c72
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Date deposited: 17 Feb 2021 17:33
Last modified: 13 Dec 2021 03:05
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Author:
Lindsay-Marie Armstrong
Author:
Thomas M. Mezza
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