Contrasting Structure-Property Relationships in Amorphous, Hierarchical and Microporous Aluminophosphate Catalysts for Claisen-Schmidt Condensation Reactions

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.

Publication DOI: https://doi.org/10.1016/j.apcata.2021.118376
Divisions: College of Engineering & Physical Sciences > Energy and Bioproducts Research Institute (EBRI)
College of Engineering & Physical Sciences
Additional Information: © 2021, Elsevier. Licensed under the Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International http://creativecommons.org/licenses/by-nc-nd/4.0/ Funding: 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.
Uncontrolled Keywords: Aluminophosphate,Amorphous and crystalline catalysts,Chalcones,Claisen-Schmidt condensation,Hierarchically porous,Catalysis,Process Chemistry and Technology
Publication ISSN: 1873-3875
Full Text Link:
Related URLs: https://linking ... 926860X21003902 (Publisher URL)
http://www.scop ... tnerID=8YFLogxK (Scopus URL)
PURE Output Type: Article
Published Date: 2021-10-25
Published Online Date: 2021-09-22
Accepted Date: 2021-09-20
Authors: Annath, Hamza
Manayil, Jinesh C. (ORCID Profile 0000-0002-9864-3332)
Thompson, Jillian
Marr, Andrew C.
Raja, Robert

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Version: Accepted Version

Access Restriction: Restricted to Repository staff only until 22 September 2022.

License: Creative Commons Attribution Non-commercial No Derivatives


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