多孔载体引入同源金属氧化物层诱导形成高稳定金属有机骨架分离膜的设计制备与成膜机理

项目名称： 多孔载体引入同源金属氧化物层诱导形成高稳定金属有机骨架分离膜的设计制备与成膜机理

项目编号： No.21476039

项目类型： 面上项目

立项/批准年度： 2015

项目学科： 数理科学和化学

项目作者： 张雄福

作者单位： 大连理工大学

项目金额： 88万元

中文摘要： 针对当今MOF膜稳定性及其相应制膜方法存在的局限性问题，本项目拟提出在多孔载体表面引入具有诱导成核生长点、连接膜层与载体的连接点和修饰载体表面等多功能作用的同源金属氧化物层，诱导合成相应高稳定性MOF分离膜。以ZIF-8膜为典型代表，研究载体表面引入不同结构形式的氧化锌涂层（粒子层和纳米棒层），对诱导合成ZIF-8膜的完整性和稳定性的影响规律及成膜机制；通过设计调控氧化锌棒层微结构形式，构筑合成具有不同结构的'柱支式'和'框架式'高性能ZIF-8膜；以含锌ZIF系列膜(如ZIF-7, 71和78)为代表，研究氧化锌涂层诱导合成相应ZIF系列膜的性能和规律; 以含铁MIL-53和MIL-101膜为代表，研究载体表面引入氧化铁涂层诱导合成相应MOF分离膜的性能和规律。通过研究优化制备条件与成膜性能的关系，揭示同源氧化物诱导成膜机理，开辟一条制备高稳定MOF膜的有效方法和膜分离技术。

中文关键词： 分子筛膜；无机膜；膜制备；膜材料；气体分离

英文摘要： Nowadays, there still exist some drawbacks for the stability of a MOF membrane and its preparation methods. Thus, in this proposal, a new preparation strategy is designed and used to study the preparation and formation mechanism of a highly stable MOF membrane. The strategy is based on the principle that when the metal oxide layer is made of the same metal as the MOF membrane to be grown, it can produce active sites to induce a uniform nucleation of ZIF nuclei on their surface to initiate and guide the growth of a defect-free ZIF-8 membrane, and also act as an inorganic linker between the porous ceramic substrate and the thin polycrystalline MOF membrane and a modification layer for the porous substrate. Thus, this preparation strategy favors growing a stable and defect-free MOF membrane. It includes a two-step process, that is, first the introduction of a layer of metal oxide on a porous substrate and then the growth of a stable and defect-free MOF membrane which is made of the same metal as the introduced metal oxide layer. The layer of the metal oxide introduced on the substrate plays multifunctional roles such as induction sites, linker and modification in the synthesis of the MOF membrane. With ZIF-8 membrane as typical research representive, the effects of the ZnO layers of different forms including nanoparticles and nanorods on ZIF-8 membrane properties (stability and permeation) and the mechanism of the membrane formation will be investigated. The ZIF-8 membranes with different structures supported on ZnO nanorods grown on the substrates will be designed and prepared by adjusting the morphologies of ZnO nanorods. The formation of other containing zinc ZIF membranes on the ZnO layer as induction introduced on a porous substrate will be also studied. By taking both containing Fe MIL-53 and MIL-101 membranes as the research representives, the induction formation of the membranes on the ferric oxide layers introduced on the substrate will be carried out. The membrane properties will be optimized by adjusting the preparation conditions. It is expected that the mechanism on membrane formation can be clarified. A feasible preparation route for stable MOF membranes and membrane technology can be developed.

英文关键词： molecular sieve membrane;inorganic membrane;membrane preparation;membrane material;gas separation