Inter-connected and open pore hierarchical TS-1 with controlled framework titanium for catalytic cyclohexene epoxidation

Jiao, Yilai, Adedigba, Abdul-Lateef, He, Qian ORCID: https://orcid.org/0000-0003-4891-3581, Miedziak, Peter J., Brett, Gemma Louise, Dummer, Nicholas F. ORCID: https://orcid.org/0000-0002-0946-6304, Perdjon, Michal ORCID: https://orcid.org/0000-0002-0224-1647, Liu, Jinmin and Hutchings, Graham John ORCID: https://orcid.org/0000-0001-8885-1560 2018. Inter-connected and open pore hierarchical TS-1 with controlled framework titanium for catalytic cyclohexene epoxidation. Catalysis Science and Technology 8 , pp. 2211-2217. 10.1039/C7CY02571H

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Abstract

A post-synthesis method was developed to reduce the extra-framework titanium (Ti) in TS-1 zeolites (Si/Ti ratio = 50), in which tetrapropylamonium hydroxide (TPAOH) aqueous solution was used to promote the dissolution, redistribution and recrystallization processes, and hence to convert amorphous Ti species into zeolitic phases. It was found that TPAOH could effectively convert the extra-framework Ti into framework Ti, and the TPAOH concentration influenced the pore structure significantly. Under lower TPAOH concentration (i.e. 0.05–0.4 M), only closed meso-/macropores (grooves and hollow cavities) can be created in the TS-1 crystals. At an optimum concentration of 0.5 M TPAOH, open and connected hierarchical mesopores and macropores were created in the resulting TS-1 zeolites. Compared with the parent TS-1, the amount of extra-framework titanium was reduced significantly from 14.4% to 0.3% and the meso-/macropore volume was increased from 0.014 to 0.168 cm3 g−1 accordingly upon TPAOH post treatment. Along with the parent TS-1 zeolite, the developed hierarchical TS-1 zeolites were assessed in the catalytic epoxidation of cyclohexene. It was confirmed that the amount of framework titanium and hierarchical pore structure influenced the catalytic activity considerably. Closed porosity slightly improved the cyclohexene conversion, whereas the open-pore sample shows the optimum catalytic activity in cyclohexene conversion.

Item Type:	Article
Date Type:	Published Online
Status:	Published
Schools:	Chemistry Cardiff Catalysis Institute (CCI)
Publisher:	Royal Society of Chemistry
ISSN:	2044-4753
Date of First Compliant Deposit:	10 April 2018
Date of Acceptance:	28 March 2018
Last Modified:	06 Nov 2024 07:15
URI:	https://orca.cardiff.ac.uk/id/eprint/110610

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