In-situ approach to porous nitrogen-doped carbon nanosheets functionalized by Br?nsted acidic ionic liquids for microwave-assisted upgrading fructose to 5-hydroxymethylfurfural

FUEL(2024)

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摘要
In the search for robust and recoverable supported Br & oslash;nsted acidic ionic liquids (BAILs) catalysts for efficient upgrading bio-sugars to value-added chemicals, an in-situ strategy of supramolecular preorganization-thermal polycondensation is designed to fabricate porous ultrathin nitrogen-doped carbon nanosheets (NCNSs), and then BAILs-functionalized NCNSs catalysts are prepared via successive quaternary ammonization by sultones and anion exchange with Br & oslash;nsted acids. By adjusting the molar composition of the starting monomers, the textural properties of NCNSs supports are tuned; and by functionalization with different sultones (1,3-propanesultone and 1,4-butanesultone) and organic (trifluoromethanesulfonic acid and p-toluenesulfonic acid) or inorganic (H2SO4 and H3PO4) acids, the surface hydrophobicity and Br & oslash;nsted acid strength of the catalysts are regulated. The catalysts are applied in microwave-assisted upgrading fructose to 5-hydroxymethylfurfural, and influences of Br & oslash;nsted acid nature, surface hydrophobicity and textural properties on the catalytic performance are explored. For the most active [C4SO3HN][OTf]-NCNSs-MA-3 catalyst with the advantages of superstrong Br & oslash;nsted acidity, higher surface hydrophobicity and perfect porous ultrathin sheet-like nanostructure, the conversion of fructose and the yield of 5-hydroxymethylfurfural of 100% and 87.7% are achieved after microwave irradiation for 15 min, outperforming Amberlyst-15 resin and HY zeolite. The catalysts also demonstrate the robust catalytic reusability, and after five consecutive catalytic runs, the obvious activity loss hardly occurs, along with little acid sites leaching.
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关键词
Br & oslash,nsted acidic ionic liquids,Solid acid,Nitrogen -doped carbon,Bio-sugar,5-hydroxymethylfurfural
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