薄片状MFI晶体无凝胶蒸汽辅助晶化制备b轴取向沸石膜  

Gel-less steam-assisted crystallization of platelike MFI crystals for the fabrication of b-oriented zeolite membranes

作　　者：马宇康 陈姣 李毅 杨玉婷 张豪益 卢春山[2] 武光军 肖强 MA Yu-Kang;CHEN Jiao;LI Yi;YANG Yu-Ting;ZHANG Hao-Yi;LU Chun-Shan;WU Guang-Jun;XIAO Qiang(Key Laboratory of the Ministry of Education for Advanced Catalysis Materials,Institute of Advanced Fluorine Containing Materials,Zhejiang Normal University,Jinhua,Zhejiang 321004,China;State Key Laboratory of Green Chemistry Synthesis Technology,Zhejiang University of Technology,Hangzhou 310032,China;School of Materials Science and Engineering&National Institute for Advanced Materials,Nankai University,Tianjin 300350,China)

机构地区：[1]浙江师范大学,含氟新材料研究所,先进催化材料教育部重点实验室,金华321004 [2]浙江工业大学,省部共建绿色化学合成技术国家重点实验室(筹),杭州310032 [3]南开大学材料科学与工程学院,天津300350

出　　处：《无机化学学报》2023年第2期245-254,共10页Chinese Journal of Inorganic Chemistry

基　　金：国家自然科学基金(No.22075253);省部共建绿色化学合成技术国家重点实验室开放课题(No.GCST-20200005)资助。

摘　　要：采用新型薄片状MFI沸石晶体作为晶种,通过无凝胶蒸汽辅助晶化法(gel-less steam-assisted crystallization,GLSAC)在烧结氧化硅多孔载体上制备了致密平整、b轴取向的MFI沸石膜。考察了GLSAC中模板剂浓度、釜底水量、生长温度及时间对MFI沸石膜的影响。扫描电子显微镜和X射线衍射结果显示,适量的模板剂和釡底水量能抑制晶种的面外生长。成功制备了厚度750 nm、致密平整的MFI沸石膜。制备的对丁烷异构体气体分离测试表明,25℃时,等物质的量的丁烷异构体的分离因子(SF_(A/B))可达36,对正丁烷的渗透速率为1.5×10^(-7)mol·m^(-2)·s^(-1)·Pa^(-1)。Novel platelike MFI zeolite crystals were used as seeds to fabricate dense and flat MFI zeolite membranes with b-axis orientation on porous sintered quartz wool discs through a gel-free steam-assisted crystallization(GLSAC)method.Firstly,the platelike MFI crystals were coated on the porous support by a filtration method.Then the seeded support was dipped in a tetrapropylammonium hydroxide(TPAOH)aqueous solution followed by a drying step.Subsequently,the dried discs were heated in an autoclave with a small amount of water at the bottom to grow into continuous membranes.Influences of the TPAOH concentration,water at the autoclave bottom,temperature,and time on the MFI zeolite membranes were investigated.The results of the scanning electron microscope and X-ray diffraction show that the out-plane growth of the platelike MFI seeds was suppressed at an optimized TPAOH concentration and water content.A dense and flat MFI zeolite membrane with a thickness of about 750 nm was successfully prepared.Binary butane isomers separation tests revealed that a separation factor(SF_(A/B))of 36 at a permeation rate of 1.5×10^(-7)mol·m^(-2)·s^(-1)·Pa^(-1)for n-butane was achieved.

关 键 词：MFI沸石膜 无凝胶蒸汽辅助晶化法 薄片状MFI沸石晶种 丁烷异构体分离 

分 类 号：TB34[一般工业技术—材料科学与工程] O647.313[理学—物理化学] P619.217[理学—化学]