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

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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.

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

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Supplementary files

Article information


Submitted
21 Oct 2019
Accepted
05 Feb 2020
First published
06 Feb 2020

Green Chem., 2020, Advance Article
Article type
Paper

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

B. Zhang, M. Douthwaite, Q. Liu, C. Zhang, Q. Wu, R. Shi, P. Wu, K. Liu, Z. Wang, W. Lin, H. Cheng, D. Ma, F. Zhao and G. J. Hutchings, Green Chem., 2020, Advance Article , DOI: 10.1039/C9GC03622A

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