An, S., Wang, Z., Zhang, H., Miras, H. N. and Song, Y.-F. (2019) Self‐organization of ionic liquid‐modified organosilica hollow nanospheres and heteropolyacids: efficient preparation of 5‐HMF under mild conditions. ChemCatChem, 11(10), pp. 2526-2536. (doi: 10.1002/cctc.201900285)
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184938.pdf - Accepted Version 4MB |
Abstract
As a biomass‐derived platform molecule, 5‐hydroxymethylfurfural (5‐HMF) is a highly desirable feedstock for manufacturing of high value‐added chemicals ranging from starting materials for polyesters to biofuels. In this work, we reported the fabrication of a series of multicomponent solid acid catalysts based on heteropolyacids immobilized ILs‐modified organosilica hollow nanospheres (denoted as PW12‐ILs‐Cn‐HNS), in which PW12 (PW12=H3PW12O40 ⋅ xH2O) provides Brønsted acid site, ILs show strong electrostatic interactions with PW12, Cn (Cn=alkyl chain) is attached for hydrophobicity and HNS represents organosilica hollow nanospheres. When applied for catalytic dehydration of fructose to 5‐HMF, the PW12‐ILs‐C4‐HNS catalyst with 15.2 % PW12 loading exhibited the best dehydration activity to 5‐HMF with 93.7 % yield in DMSO at 100 °C in 2 h. Compared with 2D hexagonal and 3D interconnected structures, the excellent porosity properties of hollow nanospherical structure can provide a high population of the PW12 sites and enough confined nanospace for the dehydration of fructose. Moreover, the PW12‐ILs‐Cn‐HNS catalyst showed excellent stability over six catalytic cycles without obvious loss of activity. Most importantly, careful identification of the observed intermediates revealed crucial information for the dehydration process of fructose to 5‐HMF. As such, the proposed heterogeneous catalysts show great potential in biomass conversion processes.
| Item Type: | Articles |
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| Additional Information: | This research was supported by the National Nature Science Foundation of China (21625101, 21808011, 21521005), the National Key Research and Development Program of China (2017YFB0307303), the Fundamental Research Funds for the Central Universities (XK1802‐6, XK1902, 12060093063), Beijing Natural Science Foundation (2182047), Postdoctoral Science Foundation of China (2018M631313). H. N. M would like to thank the University of Glasgow for supporting this work. |
| Status: | Published |
| Refereed: | Yes |
| Glasgow Author(s) Enlighten ID: | Moiras, Professor Haralampos |
| Authors: | An, S., Wang, Z., Zhang, H., Miras, H. N., and Song, Y.-F. |
| College/School: | College of Science and Engineering > School of Chemistry |
| Journal Name: | ChemCatChem |
| Publisher: | Wiley |
| ISSN: | 1867-3899 |
| ISSN (Online): | 1867-3899 |
| Published Online: | 02 April 2019 |
| Copyright Holders: | Copyright © 2019 Wiley-VCH Verlag GmbH & Co. KGaA |
| First Published: | First published in ChemCatChem 11(10)2526-2536 |
| Publisher Policy: | Reproduced in accordance with the publisher copyright policy |
University Staff: Request a correction | Enlighten Editors: Update this record
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