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Probing the design rationale of a high-performing faujasitic zeotype engineered with hierarchical porosity and moderated acidity

Probing the design rationale of a high-performing faujasitic zeotype engineered with hierarchical porosity and moderated acidity
Probing the design rationale of a high-performing faujasitic zeotype engineered with hierarchical porosity and moderated acidity

Porosity and acidity are influential properties in the rational design of solid-acid catalysts. Probing the physicochemical characteristics of an acidic zeotype framework at the molecular level can provide valuable insights in understanding intrinsic reaction pathways, for affording structure–activity relationships. Herein, we employ a variety of probe-based techniques (including positron annihilation lifetime spectroscopy (PALS), FTIR and solid-state NMR spectroscopy) to demonstrate how a hierarchical design strategy for a faujasitic (FAU) zeotype (synthesized for the first time, via a soft-templating approach, with high phase-purity) can be used to simultaneously modify the porosity and modulate the acidity for an industrially significant catalytic process (Beckmann rearrangement). Detailed characterization of hierarchically porous (HP) SAPO-37 reveals enhanced mass-transport characteristics and moderated acidity, which leads to superior catalytic performance and increased resistance to deactivation by coking, compared to its microporous counterpart, further vindicating the interplay between porosity and moderated acidity.

acid catalysis, heterogeneous catalysis, hierarchical porosity, materials characterization, probe-based techniques, structure-activity relationships, structure–activity relationships
1433-7851
19561-19569
Chapman, Stephanie
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Carravetta, Marina
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Miletto, Ivana
9a3fe0ee-6afd-4e72-abff-8e83a9114ae9
Doherty, Cara
de812571-3f1f-48d6-8fbc-db6092703ae9
Dixon, Hannah
ad0ab533-1b81-4d15-9b15-cc1221127fd2
Taylor, James
6b2c3c09-54ed-4494-8222-cb14aad8ca31
Gianotti, Enrica
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Yu, Jihong
08b7cf53-d539-4636-b851-9390a3128d92
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b
Chapman, Stephanie
02fa6ac4-c0e7-4cd3-8ffb-bf1c88cbfd45
Carravetta, Marina
1b12fa96-4a6a-4689-ab3b-ccc68f1d7691
Miletto, Ivana
9a3fe0ee-6afd-4e72-abff-8e83a9114ae9
Doherty, Cara
de812571-3f1f-48d6-8fbc-db6092703ae9
Dixon, Hannah
ad0ab533-1b81-4d15-9b15-cc1221127fd2
Taylor, James
6b2c3c09-54ed-4494-8222-cb14aad8ca31
Gianotti, Enrica
2496d8d3-780f-4fe0-a43e-147e68331078
Yu, Jihong
08b7cf53-d539-4636-b851-9390a3128d92
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b

Chapman, Stephanie, Carravetta, Marina, Miletto, Ivana, Doherty, Cara, Dixon, Hannah, Taylor, James, Gianotti, Enrica, Yu, Jihong and Raja, Robert (2020) Probing the design rationale of a high-performing faujasitic zeotype engineered with hierarchical porosity and moderated acidity. Angewandte Chemie International Edition, 59 (44), 19561-19569. (doi:10.1002/anie.202005108).

Record type: Article

Abstract

Porosity and acidity are influential properties in the rational design of solid-acid catalysts. Probing the physicochemical characteristics of an acidic zeotype framework at the molecular level can provide valuable insights in understanding intrinsic reaction pathways, for affording structure–activity relationships. Herein, we employ a variety of probe-based techniques (including positron annihilation lifetime spectroscopy (PALS), FTIR and solid-state NMR spectroscopy) to demonstrate how a hierarchical design strategy for a faujasitic (FAU) zeotype (synthesized for the first time, via a soft-templating approach, with high phase-purity) can be used to simultaneously modify the porosity and modulate the acidity for an industrially significant catalytic process (Beckmann rearrangement). Detailed characterization of hierarchically porous (HP) SAPO-37 reveals enhanced mass-transport characteristics and moderated acidity, which leads to superior catalytic performance and increased resistance to deactivation by coking, compared to its microporous counterpart, further vindicating the interplay between porosity and moderated acidity.

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Accepted/In Press date: 9 June 2020
e-pub ahead of print date: 25 August 2020
Published date: 26 October 2020
Keywords: acid catalysis, heterogeneous catalysis, hierarchical porosity, materials characterization, probe-based techniques, structure-activity relationships, structure–activity relationships

Identifiers

Local EPrints ID: 442665
URI: http://eprints.soton.ac.uk/id/eprint/442665
ISSN: 1433-7851
PURE UUID: f8c1980f-1018-4ec9-b971-ea85105cc0d1
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: 22 Jul 2020 17:02
Last modified: 20 Feb 2021 02:40

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Contributors

Author: Stephanie Chapman
Author: Ivana Miletto
Author: Cara Doherty
Author: Hannah Dixon
Author: James Taylor
Author: Enrica Gianotti
Author: Jihong Yu
Author: Robert Raja ORCID iD

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