水合氯化锌和硫酸根离子协同促进二氧化钛催化剂将纤维素解聚为高价值化学品。
Depolymerization of cellulose into high-value chemicals by using synergy of zinc chloride hydrate and sulfate ion promoted titania catalyst.
机构信息
State Key Laboratory of Pulp and Paper Engineering, South China University of Technology, Guangzhou 510640, China.
State Key Laboratory of Pulp and Paper Engineering, South China University of Technology, Guangzhou 510640, China.
出版信息
Bioresour Technol. 2017 Oct;241:760-766. doi: 10.1016/j.biortech.2017.06.004.
Experiments for cellulose depolymerization by synergy of zinc chloride hydrate (ZnCl·RHO) and sulfated titania catalyst (SO/TiO) were investigated in this study. The results showed the introduction of sulfate into the TiO significantly enhanced the catalyst acid amount, especially for Brønsted acid site, which is beneficial for subsequent cellulose depolymerization. ZnCl·RHO hydrate, only a narrow composition range of water, specifically 3.0≤R≤4.0, can dissolve cellulose, which finally resulted the cellulose with low crystallinity and weak intrachain and interchain hydrogen bond network. Coupling of ZnCl·RHO hydrate and SO/TiO catalyst as a mixed reaction system promoted cellulose depolymerization, and the products can be adjusted by the control of reaction conditions, the low temperature (80-100°C) seemed beneficial for glucose formation (maximal yield 50.5%), and the high temperature (120-140°C) favored to produce levulinic acid (maximal yield 43.1%). Besides, the addition of organic co-solvent making HMF as the main product (maximal yield 38.3%).
本研究考察了水合氯化锌（ZnCl·RHO）和硫酸化二氧化钛催化剂（SO/TiO）协同作用对纤维素解聚的实验。结果表明，硫酸盐的引入显著提高了 TiO 的催化剂酸量，特别是对 Brønsted 酸位，这有利于后续的纤维素解聚。ZnCl·RHO 水合物只有在特定的水含量范围 3.0≤R≤4.0 内才能溶解纤维素，这最终导致纤维素结晶度降低，并且其链内和链间氢键网络减弱。ZnCl·RHO 水合物和 SO/TiO 催化剂的耦合作为一个混合反应体系促进了纤维素的解聚，并且可以通过控制反应条件来调节产物，低温（80-100°C）有利于葡萄糖的生成（最大产率为 50.5%），高温（120-140°C）有利于生成乙酰丙酸（最大产率为 43.1%）。此外，添加有机溶剂可以使 HMF 成为主要产物（最大产率为 38.3%）。
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