Journal of Catalysis, Vol.385, 10-20, 2020
Unprecedented activity and stability on zirconium phosphates grafted mesoporous silicas for renewable aromatics production from furans
The selective production of aromatic chemicals such as benzene, toluene and xylenes from biomass-derived furans are quite challenging since zeolites and other supported heterogeneous catalysts are easily deactivated by trapping oligomeric species over their pores. Herein, a series of zirconium phosphates (ZrP) grafted on ordered mesoporous architectures of silicas was prepared by nonhydrolytic sol-gel method, and evaluated for the selective production of valuable para-xylene (pX) by catalytic reaction of 2,5-dimethylfuran (DMF) with gaseous ethylene through tandem Diels-Alder cycloaddition and dehydration reactions. The surface properties such as P/Zr ratio, Bronsted (B) to Lewis (L) acid sites and grafting layer thickness of the ZrP grafted silica catalysts were largely altered by changing P/Zr ratios and parent mesoporous silica surfaces. The amounts and strengths of acidic sites including B and L sites from the active (Zr-O)(2)-PO(OH) and (Zr-O)(3)-PO species were crucial factors for the differences in pX production rate on the ZrP grafted KIT-6, SBA-15 and fumed SiO2. (C) 2020 Elsevier Inc. All rights reserved.
Keywords:Aromatics;Biomass;Optimal Bronsted/Lewis acid sites;Ordered mesoporous silicas;Zirconium phosphate species