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Dicationic ionic liquids as sustainable approach for direct conversion of cellulose to levulinic acid

机译:阳离子阳离子液体是将纤维素直接转化为乙酰丙酸的可持续方法

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The conversion of cellulose to platform chemicals and renewable energies is the most promising and sustainable route to solve the crisis of fossil fuel resources. With this aim, the one-pot conversion of cellulose to industrial important levulinic acid (LA) using dicationic ionic liquids as a catalyst has been investigated. In the present research work, dicationic ionic liquids, containing 1,1-bis(3-methylimidazolium-1-y1) butylene ([C-4(Mim)(2)]) cation with counter anions hydrogensulfate, dihydrogensulfate, methanesulfonate, and trifluoromethanesulfonate has been synthesized and applied for one-pot conversion of cellulose to LA. The structures, thermal stability, and acidity of ILs were determined by H-1 NMR, CHNS values, thermogravimetric analyzer (TGA) and Hammet acidity function, respectively. Among the synthesized ionic liquids, [C-4(Mim)(2)]K2HSO4)(H2SO4)(2)] showed higher catalytic activity for conversion of cellulose to LA (55%) without using any additional catalyst or solvent at 100 degrees C for 3 h, which is the best result compared to previous reports. A mechanism to explain the reaction route toward LA formation is proposed. Moreover, the recycling of IL was easily achieved without structural changes or any impurities. This one-pot production of levulinic acid from untreated cellulose will open new opportunity for the conversion of sustainable biomass resources into valuable chemicals. (C) 2017 Elsevier Ltd. All rights reserved.
机译:纤维素向平台化学品和可再生能源的转化是解决化石燃料资源危机的最有希望和可持续的途径。为了这个目的,已经研究了使用阳离子型离子液体作为催化剂将纤维素一锅转化为工业上重要的乙酰丙酸(LA)。在当前的研究工作中,含有1,1-双(3-甲基咪唑-1-y1)丁烯([C-4(Mim)(2)])阳离子以及抗衡阴离子硫酸氢根,二氢硫酸根,甲磺酸根和已经合成了三氟甲磺酸酯,并将其用于将纤维素一锅法转化为LA。 IL的结构,热稳定性和酸度分别通过H-1 NMR,CHNS值,热重分析仪(TGA)和Hammet酸度函数确定。在合成的离子液体中,[C-4(Mim)(2)] K2HSO4)(H2SO4)(2)在不使用任何其他催化剂或溶剂的情况下,在100度下表现出较高的催化活性,可将纤维素转化为LA(55%) C进行3小时,与以前的报告相比,这是最好的结果。提出了解释向LA形成的反应途径的机制。此外,IL的回收很容易实现,而没有结构变化或任何杂质。从未经处理的纤维素一锅生产乙酰丙酸将为将可持续的生物质资源转化为有价值的化学品提供新的机会。 (C)2017 Elsevier Ltd.保留所有权利。

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