期刊
ACS CATALYSIS
卷 6, 期 11, 页码 7722-7727出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.6b02431
关键词
biofuels; hydrogen transfer; heterogeneous catalysis; acid base catalyst; mesoporous materials
资金
- International S&T Cooperation Program of China [2010DFB60840]
- National Natural Science Foundation of China [21576059, 21666008]
- Department of Biotechnology (Government of India)
- Key Technologies R&D Program of China [2014BAD23B01]
Catalytic transfer hydrogenation (CTH) reactions are efficient transformation routes to upgrade biobased chemicals. Herein, we report a facile and template-free route to synthesize a series of heterogeneous nitrogen-containing alkyltriphosphonate-metal hybrids with enhancive Lewis acid and base sites, and their catalytic activity in converting biomass-derived carbonyl compounds to corresponding alcohols in 2-propanol. Particularly, a quantitative yield of furfuryl alcohol (FFA) was obtained from furfural (FUR) over organotriphosphate-zirconium hybrid (ZrPN) under mild conditions. The presence of Lewis basic sites adjacent to acid sites with an appropriate base/acid site ratio (1:0.7) in ZrPN significantly improved the yield of FFA. Mechanistic studies for the transformation of FUR to FFA with ZrPN in 2-propanol-d(8) evidently indicate CTH reaction proceeding via a direct intermolecular hydrogen transfer route. It was also found that ZrPN could catalyze isomerization of C-3-C-6 aldoses to ketoses involving intramolecular hydrogen transfer in water.
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