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Designing multi-dopant species in microporous architectures to probe reaction pathways in solid-acid catalysis

Designing multi-dopant species in microporous architectures to probe reaction pathways in solid-acid catalysis
Designing multi-dopant species in microporous architectures to probe reaction pathways in solid-acid 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 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 multi-dopant solid-acid catalyst (MgSiAPO-34), designed to improve and contrast with the performance of SiAPO-34 (mono-dopant analogue), for the dehydration of ethanol to ethylene. We employ a range of 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 multi-dopant 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 multi-dopant 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.
Catalysis, Zeotypes, solid-acid catalysts, Ethanol, CFD
2296-2646
1-13
Potter, Matthew
34dee7dc-2f62-4022-bb65-fc7b7fb526d2
Armstrong, Lindsay-Marie
db493663-2457-4f84-9646-15538c653998
Carravetta, Marina
1b12fa96-4a6a-4689-ab3b-ccc68f1d7691
Mezza, Thomas
c81e4984-d885-4a18-a1b5-64c5d5ca275e
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b
Potter, Matthew
34dee7dc-2f62-4022-bb65-fc7b7fb526d2
Armstrong, Lindsay-Marie
db493663-2457-4f84-9646-15538c653998
Carravetta, Marina
1b12fa96-4a6a-4689-ab3b-ccc68f1d7691
Mezza, Thomas
c81e4984-d885-4a18-a1b5-64c5d5ca275e
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b

Potter, Matthew, Armstrong, Lindsay-Marie, Carravetta, Marina, Mezza, Thomas and Raja, Robert (2020) Designing multi-dopant species in microporous architectures to probe reaction pathways in solid-acid catalysis. Frontiers in Chemistry, 8, 1-13, [171]. (doi:10.3389/fchem.2020.00171).

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 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 multi-dopant solid-acid catalyst (MgSiAPO-34), designed to improve and contrast with the performance of SiAPO-34 (mono-dopant analogue), for the dehydration of ethanol to ethylene. We employ a range of 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 multi-dopant 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 multi-dopant 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
Published date: 17 March 2020
Keywords: Catalysis, Zeotypes, solid-acid catalysts, Ethanol, CFD

Identifiers

Local EPrints ID: 438444
URI: http://eprints.soton.ac.uk/id/eprint/438444
ISSN: 2296-2646
PURE UUID: 06f00527-951d-427d-953d-a620f9691c97
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: 10 Mar 2020 17:31
Last modified: 18 Feb 2021 17:16

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