Staff View: Soft-templating synthesis of hierarchical mordenite as high-performance catalyst for cyclic acetals production via acetylation of glycerol and benzaldehyde

Soft-templating synthesis of hierarchical mordenite as high-performance catalyst for cyclic acetals production via acetylation of glycerol and benzaldehyde

Highly active hierarchical mordenite zeolite with micro/mesoporosity (TM-n) for selective synthesis of cyclic acetals via acetylation reaction is reported. The hierarchical zeolite is synthesized using soft-templating approach with variations in octadecyltrimethoxysilane (OTMS/Al2O3 ratio, n = 0.2,...

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Main Authors:	Gong, Jiang-Tian, Alomar, Taghrid S., Almasoud, Najla, Pace, Ludovica, Vicente, Aurelie, Maireles-Torres, Pedro, Juan, Joon Ching, El-Bahy, Zeinhom M., Mintova, Svetlana, Ng, Eng-Poh
Format:	Article
Published:	Elsevier 2024
Subjects:	Q Science (General) QD Chemistry
Online Access:	http://eprints.um.edu.my/45231/ https://doi.org/https://doi.org/10.1016/j.micromeso.2024.113111
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spelling	my.um.eprints.452312024-09-30T02:46:00Z http://eprints.um.edu.my/45231/ Soft-templating synthesis of hierarchical mordenite as high-performance catalyst for cyclic acetals production via acetylation of glycerol and benzaldehyde Gong, Jiang-Tian Alomar, Taghrid S. Almasoud, Najla Pace, Ludovica Vicente, Aurelie Maireles-Torres, Pedro Juan, Joon Ching El-Bahy, Zeinhom M. Mintova, Svetlana Ng, Eng-Poh Q Science (General) QD Chemistry Highly active hierarchical mordenite zeolite with micro/mesoporosity (TM-n) for selective synthesis of cyclic acetals via acetylation reaction is reported. The hierarchical zeolite is synthesized using soft-templating approach with variations in octadecyltrimethoxysilane (OTMS/Al2O3 ratio, n = 0.2, 0.3 and 0.4) in precursor hydrogels. The results reveal that OTMS not only creates secondary mesoporosity in zeolite framework (larger mesopore volume, external surface area, average pore diameter), but also influences the crystallization process, altering the crystal morphology, crystallinity and Si/Al ratios. Among TM-n zeolites prepared, TM-0.3 hierarchical mordenite has the optimum OTMS amount incorporated while further increasing the OTMS amount leads to the formation of ANA/GIS intergrowth. Thanks to the accessible hierarchical porosity, reduced acidity and morphological effects, the TM-0.3 hierarchical mordenite exhibits excellent catalytic performance (84.1% conversion, TOF = 0.087 s-1, 61.5% dioxolane selectivity) in acetylation of glycerol and benzaldehyde (160 degrees C, 20 min) better than pristine mordenite. The catalyst is reusable for five runs with minimal loss of activity (TOF = 0.087 -> 0.084 s-1), making it a promising catalyst for chemical productions involving bulky molecules. In addition, comparative catalytic tests with classical homogeneous and heterogeneous catalysts, including H2SO4, HCl, CH3COOH, H-Y, H-LTL, Na-X, Na-A, were performed. Elsevier 2024-05 Article PeerReviewed Gong, Jiang-Tian and Alomar, Taghrid S. and Almasoud, Najla and Pace, Ludovica and Vicente, Aurelie and Maireles-Torres, Pedro and Juan, Joon Ching and El-Bahy, Zeinhom M. and Mintova, Svetlana and Ng, Eng-Poh (2024) Soft-templating synthesis of hierarchical mordenite as high-performance catalyst for cyclic acetals production via acetylation of glycerol and benzaldehyde. Microporous and Mesoporous Materials, 372. p. 113111. ISSN 1387-1811, DOI https://doi.org/10.1016/j.micromeso.2024.113111 <https://doi.org/10.1016/j.micromeso.2024.113111>. https://doi.org/https://doi.org/10.1016/j.micromeso.2024.113111 10.1016/j.micromeso.2024.113111
institution	Universiti Malaya
building	UM Library
collection	Institutional Repository
continent	Asia
country	Malaysia
content_provider	Universiti Malaya
content_source	UM Research Repository
url_provider	http://eprints.um.edu.my/
topic	Q Science (General) QD Chemistry
spellingShingle	Q Science (General) QD Chemistry Gong, Jiang-Tian Alomar, Taghrid S. Almasoud, Najla Pace, Ludovica Vicente, Aurelie Maireles-Torres, Pedro Juan, Joon Ching El-Bahy, Zeinhom M. Mintova, Svetlana Ng, Eng-Poh Soft-templating synthesis of hierarchical mordenite as high-performance catalyst for cyclic acetals production via acetylation of glycerol and benzaldehyde
description	Highly active hierarchical mordenite zeolite with micro/mesoporosity (TM-n) for selective synthesis of cyclic acetals via acetylation reaction is reported. The hierarchical zeolite is synthesized using soft-templating approach with variations in octadecyltrimethoxysilane (OTMS/Al2O3 ratio, n = 0.2, 0.3 and 0.4) in precursor hydrogels. The results reveal that OTMS not only creates secondary mesoporosity in zeolite framework (larger mesopore volume, external surface area, average pore diameter), but also influences the crystallization process, altering the crystal morphology, crystallinity and Si/Al ratios. Among TM-n zeolites prepared, TM-0.3 hierarchical mordenite has the optimum OTMS amount incorporated while further increasing the OTMS amount leads to the formation of ANA/GIS intergrowth. Thanks to the accessible hierarchical porosity, reduced acidity and morphological effects, the TM-0.3 hierarchical mordenite exhibits excellent catalytic performance (84.1% conversion, TOF = 0.087 s-1, 61.5% dioxolane selectivity) in acetylation of glycerol and benzaldehyde (160 degrees C, 20 min) better than pristine mordenite. The catalyst is reusable for five runs with minimal loss of activity (TOF = 0.087 -> 0.084 s-1), making it a promising catalyst for chemical productions involving bulky molecules. In addition, comparative catalytic tests with classical homogeneous and heterogeneous catalysts, including H2SO4, HCl, CH3COOH, H-Y, H-LTL, Na-X, Na-A, were performed.
format	Article
author	Gong, Jiang-Tian Alomar, Taghrid S. Almasoud, Najla Pace, Ludovica Vicente, Aurelie Maireles-Torres, Pedro Juan, Joon Ching El-Bahy, Zeinhom M. Mintova, Svetlana Ng, Eng-Poh
author_facet	Gong, Jiang-Tian Alomar, Taghrid S. Almasoud, Najla Pace, Ludovica Vicente, Aurelie Maireles-Torres, Pedro Juan, Joon Ching El-Bahy, Zeinhom M. Mintova, Svetlana Ng, Eng-Poh
author_sort	Gong, Jiang-Tian
title	Soft-templating synthesis of hierarchical mordenite as high-performance catalyst for cyclic acetals production via acetylation of glycerol and benzaldehyde
title_short	Soft-templating synthesis of hierarchical mordenite as high-performance catalyst for cyclic acetals production via acetylation of glycerol and benzaldehyde
title_full	Soft-templating synthesis of hierarchical mordenite as high-performance catalyst for cyclic acetals production via acetylation of glycerol and benzaldehyde
title_fullStr	Soft-templating synthesis of hierarchical mordenite as high-performance catalyst for cyclic acetals production via acetylation of glycerol and benzaldehyde
title_full_unstemmed	Soft-templating synthesis of hierarchical mordenite as high-performance catalyst for cyclic acetals production via acetylation of glycerol and benzaldehyde
title_sort	soft-templating synthesis of hierarchical mordenite as high-performance catalyst for cyclic acetals production via acetylation of glycerol and benzaldehyde
publisher	Elsevier
publishDate	2024
url	http://eprints.um.edu.my/45231/ https://doi.org/https://doi.org/10.1016/j.micromeso.2024.113111
_version_	1811682106141573120
score	13.211869

Soft-templating synthesis of hierarchical mordenite as high-performance catalyst for cyclic acetals production via acetylation of glycerol and benzaldehyde

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