生物质转化多功能层状分子筛催化剂的可控构筑

构筑多功能分子筛催化剂用以提高生物质转化级联反应的效率具有重要意义。近些年来，人们在此方面进行了诸多有益的探索，但是仍存在以下问题限制其高效利用及新反应的开发：1.已开发的分子筛结构类型有待丰富；2.可整合的功能中心类型存在瓶颈，尤其是低尺度贵金属封装于Lewis酸分子筛实施困难；3.活性中心的可控式引入仍待探索。结合以上问题，申请人拟以MWW层状分子筛为基础材料，利用其“三明治”的结构特点，即片层和夹心统一又独立，可灵活变换、分级调控，采用“多步走”的策略，在结构变换的过程中逐级可控的引入多种活性中心。该路线可操作性强，对层状材料具有普遍适用性，拓展了多功能分子筛催化剂的范畴；可引入的活性中心类型丰富、便于调节，有利于实现多种协同作用，提高反应效率；并且为开发更多新型反应提供了契机。目前，初步的研究结果证明了该项目的可行性。

The past decade has witnessed a surge of research on rational design of multi-functional catalysts for cascade biomass conversion reactions. However, the following problems still exist that hinders its efficient use and exploring of new reactions: 1.The thorough-investigated zeolite types are still limited; 2.It remains big challenge to fulfill the integration of certain functional centers, especially confining subnanometric noble metal into Lewis acid zeolites; 3.Controllable tailoring of the active centers requires more research effort. To address the above problems, in this project, based on lamellar MWW zeolite which is a "sandwich " like easy-convertible structure, we demonstrate a "step-by-step" strategy for controllable introducing active centers during each structure conversion procedure. The layers and inner part of the "sandwich " are independent and related, which means it is possible to flexibly control each part and plant in multiple active centers. This approach has excellent maneuverability ensuring its universal applicability to layered zeolite materials which extends the scope of multi-functional zeolite catalysts. The diversified assembly of synergistic functional centers may offer an answer and shed light on improving reaction efficiency and developing new reactions. Our preliminary research results have proved the feasibility of the project.