脱氧金属有机骨架材料(MOFs)的构建及水敏性失活机理研究

可燃气体中氧气的存在无疑使其净化和应用都非常危险，利用可逆吸氧剂能够实现安全高效脱氧。金属有机骨架（MOFs）材料是一种微多孔功能材料，且由亚稳态的金属 Cr和Fe配位的MOFs系列材料（Cr3(BTC)2和Fe2(dobdc)）具有可逆吸氧性能，但存在严重的水敏性失活问题，痕量水分子既可以严重破坏材料的可逆吸氧性。首先采用远离水的方式，受人体血液血红蛋白中由Fe2+配位的卟啉具有憎水与载氧双功能性能启发，运用仿生学原理先期选择带有憎水性基团的配体合成与后期憎水性基团加入两种手段研究构建并制备新型憎水性可逆吸氧MOFs材料；其次从不惧怕水的角度考虑，基于Mn和V具有比传统吸氧金属配合物Cr和Fe系列更稳定的价态，研究制备可以脱水的可逆吸氧MOFs材料。关联材料的金属类型、配位与构建方式及水氧的竞争性吸附性能，为寻找抗痕量水分子失活的可逆吸氧MOFs材料提供理论支撑，拓展其工业应用奠定基础。

Oxygen present in the combustible gases is undoubtedly very dangerous especially in its purification and application, and a reversible oxygen-absorbing agent is capable of achieving a safe and efficient deoxidation. Metal-organic frameworks (MOFs) material is a micro-porous functional materials, and materials by the metastable metallic Cr and Fe ligand MOFs series (Cr3 (BTC) 2 and Fe2 (dobdc)) with the reversible oxygen performance, but it is extremely sensitive to water molecules. The traces of water molecules contained in the air may be severely damaged reversible oxygen-absorbing material, so that it is completely inactivated. First of all away from the water. Inspired by the human blood hemoglobin by Fe2 + porphyrin ligand with hydrophobic and oxygen-carrying dual-function performance, preparation of the novel hydrophobic reversible oxygen of MOFs with two approaches based the bionics principle: preliminary ligand synthesis with a hydrophobic group, or make it is joined lately.And then, in the perspective of not afraid of water. Based on Mn and V with more stable valence states than Cr and Fe series, the study can be prepared by dehydration of Reversible oxygen MOFs. Associated materials of metal type, the competitive coordination mode and water oxygen adsorption performance, provide the theoretical support of anti-trace water molecules inactivation the reversible oxygen MOFs materials, and expand its industrial application basis.