期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 10, 期 31, 页码 10157-10168出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.2c01394
关键词
5-hydroxymethylfurfural; glucose; titanium phosphate; SBA-15; solid acid
资金
- University of Groningen
- China Scholarship Council [201606740069]
The study presented a mesoporous Lewis-Brensted bifunctional solid acid catalyst prepared by grafting titania on SBA-15 followed by phosphation, achieving selective tandem catalysis for glucose conversion via fructose to HMF with enhanced catalytic performance and stability.
The grafting of titania on SBA-15 followed by its phosphation was presented to prepare a mesoporous Lewis-Brensted bifunctional solid acid catalyst for the tandem conversion of glucose via fructose to 5-hydroxymethylfurfural (HMF). Titania was dispersed on SBA-15 as an amorphous surface layer containing abundant coordinatively unsaturated tetrahedral Ti ions, which was reactive and readily transformed upon phosphation into a new titanium phosphate phase with the chemical formula identified as Ti2O3(H2PO4)(2)center dot 2H(2)O. The ordered mesoporous structure was well maintained after three modification cycles, affording a desirable surface area of over 300 m(2)/g. The SBA-15 supported titanium phosphate layer affords higher overall acidity and Brensted to Lewis acid ratio, compared with the conventional post-phosphated bulk anatase titania. The tetrahedral Ti ions and the adjacent protonated phosphate groups on the titanium phosphate layer could form Lewis-Brensted acid pairs at molecular level proximity, which largely enhanced the selective tandem catalysis for glucose conversion via fructose to HMF. An optimized HMF yield of 71% was achieved at 160 degrees C in a water-methyltetrahydrofuran biphasic system over the SBA-15-supported titanium phosphate catalyst. The catalyst exhibited good hydrothermal stability with a rather limited silicon and phosphate leaching, and no distinct pore collapse or performance loss over three sequential reaction runs.
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