Acid–base bi-functionalized, large-pored mesoporous silica nanoparticles for cooperative catalysis of one-pot cellulose-to-HMF conversion
Acid–base bi-functionalized, large-pored mesoporous silica nanoparticles for cooperative catalysis of one-pot cellulose-to-HMF conversion
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DOI：
10.1039/c2jm35391a
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发表时间：
2012-10
影响因子：
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通讯作者：
Wu Peng;Yin-Ying Lee;Connie Wu;K. Wu
中科院分区：
文献类型：
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作者：
Wu Peng;Yin-Ying Lee;Connie Wu;K. Wu
合成了孔径约为30 nm的介孔二氧化硅纳米颗粒（MSNs），并采用酸（SO3H）、碱（NH2）和酸碱（SO3H和NH2）官能团（分别为LPMSN-SO3H、LPMSN-NH2和LPMSN-both）进行了官能团化。然后将这些功能化的LPMSN纳米材料用作非均相固体催化剂，在离子液体（即[EMIM]Cl）体系中将纤维素一锅转化为5-羟甲基糠醛（HMF）。一般来说，纤维素转化包括三个主要反应：(1)纤维素-葡萄糖解聚，(2)葡萄糖-果糖异构化，(3)果糖-羟甲基糠醛脱水，每个反应分别需要酸、碱和催化剂。因此，为了了解催化剂在每个步骤中的作用，我们将合成的LPMSN-SO3H、LPMSN-NH2和lpmsn -两种催化剂分别应用于以纤维素、纤维素二糖、葡萄糖和果糖为起始原料的反应中。结果表明，LPMSN-SO3H和LPMSN-NH2分别可以提高需要酸和碱催化剂的反应的HMF收率。此外，LPMSN-SO3H和lpmsn -两种催化剂都有助于一锅纤维素到HMF的转化，并提高了HMF的收率。
Mesoporous silica nanoparticles (MSNs) with large pore size around 30 nm were synthesized and functionalized with acid (SO3H), base (NH2) and both acid–base (SO3H and NH2) functional groups (namely, LPMSN-SO3H, LPMSN-NH2 and LPMSN-both, respectively). These functionalized LPMSN nanomaterials were then used as heterogeneous solid catalysts for one-pot conversion of cellulose to 5-hydroxymethylfurfural (HMF) in an ionic liquid (i.e., [EMIM]Cl) system. In general, cellulosic conversion involves three main reactions: (1) cellobiose-to-glucose depolymerization, (2) glucose-to-fructose isomerization, and (3) fructose-to-HMF dehydration, and each reaction needs an acid, base, and catalyst, respectively. Therefore, in order to understand the role of catalysts in each step, we applied the synthesized LPMSN-SO3H, LPMSN-NH2 and LPMSN-both catalysts in the reactions using cellulose, cellobiose, glucose and fructose as starting materials. Results show that LPMSN-SO3H and LPMSN-NH2 could increase the yield of HMF converted from the reactions that need acid and base catalysts, respectively. In addition, LPMSN-SO3H and LPMSN-both catalysts are found to be useful for one-pot cellulose-to-HMF conversion with an enhanced HMF yield.