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Solid Lewis acidity of boehmite gamma-AlO(OH) and its catalytic activity for transformation of sugars in water

机译:勃姆石γ-AlO(OH)的固体路易斯酸度及其对水中糖转化的催化活性

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摘要

Aqueous-phase transformation of C3- and C6-sugars toward valuable intermediates such as lactic acid and 5-hydroxymethylfurfural (HMF) using boehmite, an abundant, inexpensive and simple aluminium oxide hydroxide gamma-AlO(OH) was demonstrated. Pyridine-adsorbed Fourier transform infrared (FTIR) spectroscopy and trimethylphosphine oxide-adsorbed P-31 magic angle spinning (MAS) nuclear magic resonance (NMR) revealed that boehmite had no Bronsted acid sites and a small amount of weak Lewis acid sites. The amount of Lewis acid sites and the initial reaction rate for lactic acid synthesis from dihydroxyacetone increased with increase of calcination temperature of boehmite whereas the selectivity for lactic acid remained unchanged and turnover frequency decreased. Boehmite afforded lactic acid selectively from aqueous C3-sugars solution with the yields of 32% and 42% from dihydroxyacetone and glyceraldehyde, respectively, which were higher than those of hydrotalcite, titanium oxide, tin oxide and tungsten oxide. Moreover, boehmite gave both lactic acid and HMF simultaneously from aqueous glucose solution as well as fructose. The total yields of lactic acid and HMF from aqueous glucose solution reached 40%. Boehmite was found to catalyse a variety of reactions including isomerization, retro-aldol condensation, dehydration and hydration in water.
机译:证明了使用勃姆石将C3-和C6-糖水相转化为有价值的中间体(如乳酸和5-羟甲基糠醛(HMF))的方法,可以得到大量,廉价且简单的氧化铝氢氧化物γ-AlO(OH)。吡啶吸附的傅立叶变换红外光谱(FTIR)和三甲基氧化膦吸附的P-31魔角旋转(MAS)核魔术共振(NMR)表明,勃姆石没有布朗斯台德酸位点,而有少量弱路易斯酸位点。随着勃姆石煅烧温度的升高,路易斯酸位点的数量和由二羟基丙酮合成乳酸的初始反应速率增加,而乳酸的选择性保持不变,周转频率降低。勃姆石从C3糖水溶液中选择性地提供了乳酸,二羟基丙酮和甘油醛的收率分别为32%和42%,高于水滑石,氧化钛,氧化锡和氧化钨。此外,勃姆石同时从葡萄糖水溶液和果糖中产生乳酸和HMF。从葡萄糖水溶液中乳酸和HMF的总产率达到40%。发现勃姆石可催化多种反应,包括异构化,逆醛醇缩合,脱水和在水中水合。

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