Seed- and solvent-free synthesis of ZSM-5 with tuneable Si/Al ratios for biomass hydrogenation

Zhang, Bin, Douthwaite, Mark, Liu, Qiang, Zhang, Chao, Wu, Qifan, Shi, Ruhui, Wu, Peixuan, Liu, Ke, Wang, Zhuangqing, Lin, Weiwei, Cheng, Haiyang, Ma, Ding, Zhao, Fengyu and Hutchings, Graham J. ORCID: https://orcid.org/0000-0001-8885-1560 2020. Seed- and solvent-free synthesis of ZSM-5 with tuneable Si/Al ratios for biomass hydrogenation. Green Chemistry 22 (5) , pp. 1630-1638. 10.1039/C9GC03622A

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Abstract

A novel method for the synthesis of MFI zeolites has been developed, which does not require any crystal seeds or solvent. The adaptability of this method was also evidenced; a series of ZSM-5 zeolites with differing Si/Al ratios (18∼∞) were synthesized, which to date, has been a challenge in the field of solvent-free synthesis. The materials were probed by in situ DRIFTS and 2D 27Al–19F HETCOR NMR spectroscopy, the results from which indicated that fluorine-containing species play a crucial role in the crystallization of ZSM-5. During the crystallization process F− anions coordinate with Al3+ cations, resulting in the formation of 6-coordinated “F–Al–O–Si” species. It is these intermediate species which drive the formation of tetrahedral [AlO4]− units in the zeolitic framework. The effectiveness of these materials as catalyst supports was subsequently assessed in the hydrogenation of levulinic acid and glucose, which exhibited a comparable performance to commercial ZSM-5. The simple, efficient and low-cost method presented herein provides an alternative approach for the green scaled-up synthesis of zeolites.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry Cardiff Catalysis Institute (CCI)
Publisher:	Royal Society of Chemistry
ISSN:	1463-9262
Date of First Compliant Deposit:	12 March 2020
Date of Acceptance:	5 February 2020
Last Modified:	15 Nov 2024 12:00
URI:	https://orca.cardiff.ac.uk/id/eprint/130376

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