中文摘要
木质素是来源丰富的生物质资源,实现木质素的高值利用对于缓解化石资源短缺危机具有重要意义;本项目针对当前木质素催化裂解过程所用液体强酸、微孔分子筛和介孔分子筛等催化剂的固有缺陷,拟在酸功能离子液体存在的离子热条件下,通过酸功能离子液体、环氧乙烷环氧丙烷嵌段共聚物模板剂、能产生强酸中心的水溶性金属盐及不同硅源之间的自组装作用,创制孔壁具有微孔分子筛晶态结构特征,而孔径为介孔尺寸的新一类杂化材料—高稳强酸介-微孔分子筛,使微孔分子筛与介孔分子筛的优点融为一体;通过对比研究,阐明离子热条件创制的介-微孔分子筛在酸强度和稳定性上显著优于水热条件的本质原因;将高稳强酸介-微孔分子筛用于催化木质素裂解反应过程,依据介-微孔分子筛的酸性和孔结构能有效调控的特性,高选择性制备出芳香基产物;明确介-微孔分子筛的结构与催化性能的相关性,以及新催化反应的动力学规律和反应机制,为木质素的高效转化利用提供理论依据。
英文摘要
Lignin is an abundant biomass, so it is an important significance of efficient utilization of lignin in view of the shortage of fossil resource. Due to the inherent defects of the traditional catalysts, such as liquid strong acid, microporous molecular sieve and mesoporous molecular sieve, used in the lignin catalytic pyrolysis process, this project will prepare a novel meso-microporous molecular sieve with the good stability and high acid strength by the ionthermal synthesis on the supramolecular self-assembly effect of acidic functional ionic liquid, template of block copolymer from ethylene oxide and propylene oxide, soluble metal salts with the strong acid center, and different silica sources, which would make it have the advantages of both microporous and mesoporous zeolites. Through comparative study, it will be clarified that the essential reason why the acid strength and stability of meso-microporous molecular sieve by the ionthermal synthesis is significantly superior to that of the hydrothermal synthesis. Then the meso-microporous molecular sieve will be used in the catalytic pyrolysis of lignin, and base on the characteristic of the effective regulation in the pore structure and acidity of meso-microporous molecular sieve, the aromatic products will be formed with high selectivity. The relationship of the structure and catalytic property will be revealed, and the kinetics and reaction mechanism will be clarified. This study will provide the theoretical basis for the high value utilization of lignin.
