氨功能化与碱金属掺杂对MOF膜CO2吸附分离性能的协同机制

This project mainly focuses on metal-organic frameworks involving high hydrothermal stability and CO2 capture and separation capability, we first obtain continuous inorganic supported MOF membrane, while post-modification by alkylamines and alkali metal doping are carried on for preparing MOF composite membranes. MOF membrane with different thickness and surface structure are prepared by adjusting the inorganic supporter modification methods and membrane synthesis conditions, clarifying the influence of interaction between MOF and inorganic supporter on the hydrothermal stability. Through effective use of alkylamines and alkali metal to identify the factors of CO2 capture and separation capability. Revealing the relationship of composite structures, channel properties and other features, and CO2 adsorption separation thermodynamic and kinetic properties, proposing adsorption mechanism through theoretical analysis and data fitting. This project will provide a theoretical basis and practical guidance for high stability, high performance MOFs based CO2 gas separation membrane device, plays an important role in understanding the coordination mechanism of MOFs composites.

本项目以提高MOF材料水热稳定性和CO2吸附分离性能为目标，拟在无机载体上构筑稳定、连续致密的MOF薄膜，通过后合成功能化引入能与CO2发生可逆相互作用的伯胺基、仲胺基、叔胺基等，再向MOF孔道中掺杂碱金属离子，进一步增加薄膜的CO2吸附分离性能。通过MOFs结构、载体修饰方式、薄膜合成方法及合成条件的调节，得到具有不同厚度及表面结构的复合薄膜，阐明MOFs与无机载体相互作用力对水热稳定性的影响规律；通过氨基的有效利用和碱金属离子的有效掺杂，查明二者对复合膜的CO2吸附分离的影响因素及协同机制；揭示复合薄膜结构、孔道等特性与CO2吸附分离热力学和动力学性质的关系，通过理论分析与数据拟合提出吸附作用机理。本项目将为高稳定、高性能MOFs基CO2气体吸附分离膜的器件化提供理论基础与实际指导，对深入认识MOFs基复合材料的协同机制及CO2吸附机理具有普遍指导意义。

金属有机骨架材料因比表面积高和孔道结构丰富等特点，被认为具有较好的CO2吸附分离性能实际应用前景，研究如何进一步提高其低压条件下的CO2吸附能力十分必要。本项目以提高MOFs材料水热稳定性和CO2吸附分离性能为目标，在无机载体上构筑稳定连续的MOFs薄膜，探讨了碱金属掺杂的MOFs复合材料的结构特点和CO2吸附行为之间的关系。通过MOFs结构、载体修饰方式、薄膜合成方法及合成条件的调节，查明影响MOFs与无机载体相互作用力的影响因素；通过氨基引入和碱金属掺杂方式的调整，阐明双功能化对复合材料物相结构、孔道特性等与CO2吸附性能的关系，提出吸附作用机理。本项目成果对认识掺杂改性MOFs复合材料的协同机制及CO2吸附机理具有普遍指导意义。