基于模板剂超分子相互作用介导合成大孔和超大孔分子筛

Zeolites with extra-large pores have attracted great attention because of their important applications such as in hydrocracking, catalysis of large molecules, diagnostic treatments and controlled drug delivery. However, there are still very rare so far among the known zeolite frameworks, which severely limited the development of zeolite and related subjects. Based on the result of the previous research about a set of semi-rigid benzyl imidaolium structure-directing agents (SDAs), we proposed a rational strategy for SDA design in order to synthesize large and extra-large zeolite through utilizing the supramolecular interaction of the SDAs. This research topic is the extension of the earlier work, by changing the aromatic core and the cation portion of the SDAs, we can roughly regulate its state of aggregation and the special molecular characterization, while by forming into stable host-guest complexes between macrocyclic compound and corresponding SDAs, we also can precisely control its aggregation. Following this way, we intend to synthesize kinds of characteristic SDAs which can be applied into zeolite crystallization, to systematically investigate the influences of their special characteristics and state of aggregation on the zeolite crystallization, in order to find out several large and extra-large pore zeolites with novel structures and yield general rules of their formation.

具有交叉大孔、超大孔等特殊孔道结构的分子筛在石油加工（催化裂解）、大分子催化、医学诊断和药物分子传输等领域具有重要的应用价值，其合成研究一直是多孔材料化学及其相关领域最为人们关注的方向之一。然而，迄今为止，其数量仍非常有限，严重限制了分子筛及其相关学科的发展。基于对一类半刚性含芳环的咪唑盐模板剂的研究结果，我们提出了一个利用模板剂超分子自组装作用高效导向合成大孔和超大孔分子筛的新策略。本课题基于此策略，通过对模板剂分子中心芳环和阳离子中心的调变，实现对其团聚状态的粗略定性调控和特定分子特性的调节；通过大环化合物与特定模板剂分子形成稳定的主-客体配合物，实现对模板剂分子团聚状态的精确调控。拟设计合成一批性能各异的新型模板剂，并将其应用于分子筛的合成研究，综合考察模板剂特定分子特性及团聚状态对分子筛晶化结果的影响，以期合成出若干具有新颖结构的大孔和超大孔分子筛材料，并归纳出其生成的一般规律。

具有交叉大孔、超大孔等特殊孔道结构的分子筛在石油加工（催化裂解）、大分子催化、医学诊断和药物分子传输等领域具有重要的应用价值，其合成研究一直是多孔材料化学及其相关领域最为人们关注的方向之一。然而，迄今为止，其数量仍非常有限，严重限制了分子筛及其相关学科的发展。本项目提出了一个基于模板剂超分子相互作用介导合成大孔和超大孔分子筛是一个的新策略。项目执行过程中，合成了若干已知大孔和超大孔分子筛晶相，同时获得了两例分子筛新相和一个新型的ITH二维分子筛纳米片。本项目归纳了了模板剂超分子相互作用在诱导分子筛晶化过程中的一般性规律，明确了超分子自组装体在大孔和超大孔生成上至关重要的作用，为今后模板剂的设计合成提供了指导性的设计策略。本项目的研究成果，对新型大孔和超大孔分子筛的探索合成以及新型二维分子筛纳米片的合成都具有非常重要的借鉴意义。