松香基季铵盐引导合成有序超微孔材料及其结构导向作用机制研究

Ordered supermicroporous material is a kind of porous material with pores on the border between the micropore and mesopore regions. Much attention has been paid to this material because of its broad application prospect in the shape selective catalysis and drug controlled release fields. Due to the lack of suitable template agents, the fabrication of an ordered structure is difficult. Rosin-based quaternary ammonium salt possesses a unique skeleton. Its strong self-assembling ability guarantees the construction of an ordered structure, while its smaller molecular size ensures the material with pores in the supermicropore region..In the early stage of the research, highly ordered supermicroporous silica material has been synthesized with rosin-based quaternary ammonium salt. The results were published in journal of RSC Advances from Royal Society of Chemistry. Based on the previous work, a series of rosin-based quaternary ammonium salts will be designed and synthesized, and their self-assembly behavior will be investigated. The ordered supermicroporous silicas will be synthesized guided by the formation rules of self-assembling structures. The cooperative-assembling behavior between rosin-based quaternary ammonium salts and silicon sources in the synthesis process will also be studied to explore the structure directing mechanism of the rosin-based quaternary ammonium salts. Water-insoluble drug ibuprofen will be selected as a probe, and the water-insoluble drug solubilization and release properties of the ordered supermicroporous materials with different structures will be evaluated. This project can provide the theoretical basis for the design, synthesis and application researches of the ordered supermicroporous materials, and open up a new way toward the highly value-added utilization of rosin resources.

有序超微孔材料是一类孔径介于微介孔临界区间的特殊多孔材料，因其在择形催化、药物控释等领域的广阔应用前景而倍受关注，但因适宜模板剂的匮乏，其有序结构的构筑十分困难。松香基季铵盐具有独特的骨架结构，其较强的自组装能力可为有序结构的获得提供必要保障，而其较小的分子尺寸则确保材料孔径处于超微孔界限内。.在前期探索中，申请者以松香基季铵盐合成出高度有序的超微孔材料，结果发表于英国皇家化学学会的RSC Advances期刊。在此基础上，本项目拟设计合成系列松香基季铵盐，研究其自组装行为；以自组装结构形成规律指导有序超微孔二氧化硅的合成，考察合成过程中松香基季铵盐与硅源的协同自组装行为，揭示松香基季铵盐的结构导向作用机制；以难溶药物布洛芬为探针，评价不同结构有序超微孔材料的难溶药物增溶与缓释性能。本研究可为新型有序超微孔材料的设计、合成与应用研究提供理论依据，并为松香资源的高附加值利用开辟新途径。

项目以我国丰富的松香资源为原料，开展系列松香基季铵盐的合成，并以此为模板剂开展有序超微孔材料的制备研究，获得多种具有不同介观孔结构及宏观形貌的有序超微孔材料。实现立方相（Ia3d）有序超微孔及手性超微孔材料的首次合成，系统开展了有序超微孔材料宏观形貌调变研究，总结出材料形貌调变机制。对所得材料进行了难溶性药物布洛芬及挥发性精油成分柠檬醛的负载缓释性能研究，相对于经典介孔材料SBA-15与MCM-41，所合成有序超微孔材料有着更为优良的缓释性能。拓展了松香基季铵盐及其复合前驱体的抑菌活性研究，以及非硅基有序超微孔材料的合成研究，取得良好结果。发表SCI 收录期刊论文2 篇，中科院分区1区1篇，3区1篇；申请国家发明专利6 项，其中获得授权1 项；相关成果获得江西省科技进步奖一等奖1 项；所发表相关论文获得梁希青年论文奖三等奖1项。