Contrasting structure-property relationships in amorphous, hierarchical and microporous aluminophosphate catalysts for Claisen-Schmidt condensation reactions
Contrasting structure-property relationships in amorphous, hierarchical and microporous aluminophosphate catalysts for Claisen-Schmidt condensation reactions
Amorphous aluminophosphates are industrial catalysts that are active in aldol-type condensations, dehydration and alkylation. The intrinsic nature of the active sites present in these materials is poorly understood. Herein we report a comparative investigation of the catalytic active sites in amorphous and crystalline aluminophosphates (AFI topology) and their corresponding iron-containing analogues, employing Claisen-Schmidt condensation of acetophenone and benzaldehyde as the test reaction. Secondary porosity generated via the soft-templating approach in hierarchically-porous HP FeAlPO-5, and the presence of large mesopores in amorphous Am FeAlPO resulted in improved mass-transport and high conversion of carbonyls. The nature and concentration of the active acidic sites within these materials were characterized by pyridine-DRIFTS and propylamine-TPD studies and was shown to play a crucial role in the activation of carbonyl groups and better catalytic performance. Am FeAlPO(5) nearly outperformed HP FeAlPO-5, thus providing a promising alternative for expanding scope in industrial and pharmaceutical applications.
Aluminophosphate, Amorphous and crystalline catalysts, Chalcones, Claisen-Schmidt condensation, Hierarchically porous
Annath, Hamza
cee58991-da81-412f-b374-998ad604f63d
Manayil, Jinesh C.
c510d2ac-ffb8-4d91-b284-477d655a0841
Thompson, Jillian
3658d182-0d09-41ba-9231-817a9c9e4a50
Marr, Andrew C.
de50d3e6-48ab-46aa-90ca-0278b30c4137
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b
25 October 2021
Annath, Hamza
cee58991-da81-412f-b374-998ad604f63d
Manayil, Jinesh C.
c510d2ac-ffb8-4d91-b284-477d655a0841
Thompson, Jillian
3658d182-0d09-41ba-9231-817a9c9e4a50
Marr, Andrew C.
de50d3e6-48ab-46aa-90ca-0278b30c4137
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b
Annath, Hamza, Manayil, Jinesh C., Thompson, Jillian, Marr, Andrew C. and Raja, Robert
(2021)
Contrasting structure-property relationships in amorphous, hierarchical and microporous aluminophosphate catalysts for Claisen-Schmidt condensation reactions.
Applied Catalysis A: General, 627, [118376].
(doi:10.1016/j.apcata.2021.118376).
Abstract
Amorphous aluminophosphates are industrial catalysts that are active in aldol-type condensations, dehydration and alkylation. The intrinsic nature of the active sites present in these materials is poorly understood. Herein we report a comparative investigation of the catalytic active sites in amorphous and crystalline aluminophosphates (AFI topology) and their corresponding iron-containing analogues, employing Claisen-Schmidt condensation of acetophenone and benzaldehyde as the test reaction. Secondary porosity generated via the soft-templating approach in hierarchically-porous HP FeAlPO-5, and the presence of large mesopores in amorphous Am FeAlPO resulted in improved mass-transport and high conversion of carbonyls. The nature and concentration of the active acidic sites within these materials were characterized by pyridine-DRIFTS and propylamine-TPD studies and was shown to play a crucial role in the activation of carbonyl groups and better catalytic performance. Am FeAlPO(5) nearly outperformed HP FeAlPO-5, thus providing a promising alternative for expanding scope in industrial and pharmaceutical applications.
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Accepted FeAlPO manuscript HA-JM-JT-AM-RR Sept21
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Accepted/In Press date: 20 September 2021
e-pub ahead of print date: 22 September 2021
Published date: 25 October 2021
Additional Information:
Funding Information:
This work was supported by the EPSRC U.K. Catalysis Hub through Grant EP/K014714/1 ; they are kindly thanked for the resources and support provided via our membership of the U.K. Catalysis Hub Consortium . JCM thanks BBSRC GCRF Grant ( BB/P022685/1 ) for financial support.
Publisher Copyright:
© 2021 Elsevier B.V.
Copyright:
Copyright 2021 Elsevier B.V., All rights reserved.
Keywords:
Aluminophosphate, Amorphous and crystalline catalysts, Chalcones, Claisen-Schmidt condensation, Hierarchically porous
Identifiers
Local EPrints ID: 453533
URI: http://eprints.soton.ac.uk/id/eprint/453533
ISSN: 0926-860X
PURE UUID: e5a621c3-8f7d-4772-ac87-dca5b0eafa2c
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Date deposited: 19 Jan 2022 17:37
Last modified: 18 Mar 2024 05:28
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Contributors
Author:
Hamza Annath
Author:
Jinesh C. Manayil
Author:
Jillian Thompson
Author:
Andrew C. Marr
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