基于氟介质共晶调控合成CO2高效分离分子筛膜的机制研究

To solve the low perm-selectivity and instability of CO2 separation membrane material under high temperature and high pressure conditions. Zeolite T membrane layer was composited by intergrowth of erioffite and offretite crytal, and attracting many concerns due to its high chemical stability, acid resistance and suitable pore size for CO2 selectivity. in this project, Zeolite T membrane will be synthesized via novel fluoride medium to reduce the pore size and membrane thickness, by using the method of gel modification, seed size and morphology control to prepare high perm-selectivity membranes. Depending on nature gas and fuel gas as research model to study the constant correlation between separation ability and erioffite content in the membrane layer; Molecular simulation combined with experimental method will be applied to set up the kinetics model of crystal growth process and gas adsorption/desorption to study the formation and separation machanism of zeolite membranes . Expected CO2 permeance will be improved by an order of magnitude and keeping high selectivity and stability, A combined of theory and experiment to provide scientific basic for applicaion of zeolite membranes in natural gas and fuel gas decarbonization.

用于CO2分离的分子筛膜材料普遍存在渗透及选择性偏低以及高温高压条件下不稳定的问题。T型分子筛膜层由毛沸石和菱钾沸石共晶而成，因其强的化学稳定性、耐酸性和合适的CO2分离孔道而受到关注。本项目拟在新颖的氟介质中，通过共晶调控合成高毛沸石含量的T型分子筛膜，以减小分子筛孔道和降低膜层厚度，结合“晶种调控”、“形貌调控”和“溶胶调控”等手段制备具有高CO2选择性和高渗透速率的T型分子筛膜；以天然气和高炉气脱碳为研究模型，探究膜层毛沸石含量与膜分离性能的定量关系；采用分子模拟与实验表征相结合的方法，建立晶体生长过程和气体吸附-分离动力学模型,研究成膜和分离机理。预期分子筛膜渗透速率在现有基础上提高一个数量级，并保持高选择性和稳定性，为分子筛膜应用于天然气、高炉气脱碳提供实验依据。

用于CO2分离的分子筛膜材料普遍存在渗透及选择性低以及膜材料不稳定等问题。T型分子筛膜层由毛沸石和菱钾沸石共晶而成，因其强的化学稳定性、耐酸性和合适的CO2分离孔道而受到关注。本项目通过在氟介质中共晶调控合成高毛沸石含量的T型分子筛膜，以减小分子筛孔道和降低膜层厚度，结合“晶种调控”、“形貌调控”和“溶胶调控”等手段合成了T型分子筛膜；探究膜层毛沸石含量对膜分离性能的影响，高毛沸石含量的T型分子筛对CO2具有较好的选择性。采用实验与模拟手段研究了成膜和分离机理。同时，我们也研究了合成后修饰对膜性能的影响，采用APTES修饰膜层后，膜层的缺陷明显减少，实现孔径的精准调控，膜的选择性有很大提高。针对CO2的选择性分离膜，我们也研究了申请书中未涉及的膜材料，如SSZ-13型分子筛膜和ZIF-8膜等。为高通量分子筛膜材料的制备提供了科学依据。