多级孔Brønsted/Lewis酸硅基催化剂选择性催化转化纤维素制备5-羟甲基糠醛

5-羟甲基糠醛（HMF）是一种关键的生物质基平台化合物，在生产呋喃型化合物、聚合物以及烷烃等方面具有重要的应用价值。然而，化学催化法制HMF选择性低，易发生分解、再水合、缩聚等副反应，导致目前的HMF制备技术经济性较差，难以支撑HMF的商业化应用。本项目从HMF催化制备过程的产物控制规律这一关键科学问题出发，拟以纤维素及其衍生单糖为起始原料，在多级孔Brønsted/Lewis酸硅基催化剂设计、合成和活性评价的基础上，揭示催化剂表面化学性质和结构性质调控及催化剂-溶剂协同对HMF制备反应路径调控的影响机制及催化剂失活机制，构建高效稳定的硅基催化剂；在反应过程参数优化、化学动力学、原位实验和理论计算研究的基础上，揭示催化剂-溶剂的协同作用机制及纤维素→葡萄糖→HMF转化的反应机理。研究工作将为生物质高效转化制HMF提供理论依据和技术支撑，进而推动HMF在高附加值化学品合成领域的规模化应用。

5-Hydroxymethylfurfural (HMF) is a crucial bio-based platform compound, having important application values for producing furan-based chemicals, polymers, and alkanes. However, recent chemical catalytic production of HMF has tough problem of low product selectivity, which was caused by the easy occurrence of many side reactions, including fragmentation, rehydration, and condensation. As a result, the current HMF preparation technologies are not economically viable to support its commercial application. In the present research, in order to interpret the product control law in the catalytic production of HMF, cellulose and its derived monosaccharides are selected as the starting material, the design, synthesis and activity evaluation of the silica-based catalyst with hierarchical pore and Brønsted/Lewis acidity will be carried out. The influence mechanisms of chemical and structural properties of silica-based catalysts and catalyst-solvent synergy on the conversion of cellulose→glucose→HMF, and catalyst deactivation mechanism will be discussed, and the synthesis method of efficient and long-term durable silica based catalyst will be established. Furthermore, the optimization of reaction process parameters, chemical kinetics study, in-situ HMF production experiments and theoretical calculations will be deeply performed to allow a better understanding of the catalyst-solvent synergistic mechanism and the catalytic mechanism of the cellulose→glucose→HMF conversion process. This study will provide theoretical basis and technical support for the highly efficient conversion of biomass to HMF, and strongly push forward the large-scale application of HMF in the synthesis of high value-added chemicals.