期刊
GREEN CHEMISTRY
卷 19, 期 9, 页码 2101-2106出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c7gc00580f
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资金
- National Natural Science Foundation of China [21576059, 21666008]
- Key Technologies R&D Program of China [2014BAD23B01]
- Postdoctoral Science Foundation of China [2016 M600422]
- Jiangsu Postdoctoral Research Funding Plan [1601029A]
An in situ domino process has been developed to be highly efficient for direct and mild conversion of various hexose sugars to the biofuel 2,5-dimethylfuran in almost quantitative yields, without separation of unstable intermediates at 120 degrees C in n-butanol, by using polymethylhydrosiloxane and hydrophobic Pd/C as a H-donor and a bifunctional catalyst, respectively. Among the cascade reactions, the hydrosilylation process was confirmed by deuterium-labeling and kinetic studies to be favorable for sugar dehydration and exclusively acts on deoxygenation of in situ formed intermediates including furanic alcohols and aldehydes to DMF via a hydride transfer process that was facilitated by an alcoholic solvent. The catalytic system is more selective than the H-2- participated counterpart, and could be scaled up with only 0.04 mol% catalyst loading, giving DMF in a comparable yield of 85%. Moreover, Pd(0) was demonstrated to be the active species for deoxygenation, and the heterogeneous catalyst exhibited good recyclability with little elemental leaching.
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