以开孔的二维MFI纳米片为构筑单元制备沸石片膜
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摘要
以食人鱼溶液(体积比为3∶1的95%～98%(w/w)H_2SO_4和30%(w/w)H_2O_2混合液)处理多层MFI(ML-MFI)除去有机结构导向剂(OSDA),经超声剥离和沉降纯化后得到了开孔的MFI沸石纳米片。采用X射线衍射(XRD)、扫描电镜(SEM)、透射电镜(TEM)、N_2吸附-脱附、傅立叶变换红外光谱(FT-IR)和热重分析(TGA)等手段对得到的MFI沸石纳米片进行表征,发现食人鱼溶液处理可移除ML-MFI中的OSDA,再经超声剥离得到可分散、开孔的MFI沸石纳米片。将MFI沸石纳米片用简单抽滤的方式沉积到自制Al_2O_3载体上,不经二次生长得到了连续的沸石纳米片膜。单组分气体渗透性能测试结果表明,制备的MFI沸石纳米片膜对正/异丁烷的理想选择性为4.1～5.8,正丁烷的渗透速率为2.2×10~(-7)～4.1×10~(-7) mol·m~(-2)·s~(-1)·Pa~(-1)。
Open-pore MFI zeolite nanosheets were prepared by removal of organic structure-directing agents(OSDA) from a multilamellar MFI zeolite(ML-MFI) using a mixture of 95%～98%(w/w)H_2SO_4 and 30%(w/w)H_2O_2 with V_(H_2SO_4)∶V_(H_2O_2)=3∶1(known as piranha solution), followed by ultrasonication for exfoliation and sedimentation for purification. The exfoliated MFI zeolite nanosheets were characterized by various techniques, such as X-ray diffraction(XRD), scanning electron microscope(SEM), transmittance electron microscope(TEM), N_2 adsorptiondesorption, Fourier transform infrared spectrometer(FT-IR) and thermal gravimetric analyzer(TGA), etc.,indicating that OSDA was removed after the piranha solution treatment and dispersed, open-pore MFI nanosheets were obtained followed by exfoliation through ultrasonication. Continuous MFI nanosheet membranes were prepared by depositing the open-pore MFI nanosheets on home-made alumina disc supports by a simple vacuumassisted filtration method. Single gas permeance tests on the MFI zeolite nanosheet membranes indicated that ideal selectivities for n-butane over i-butane of 4.1～5.8 with a permeance of n-butane of 2.2×10~(-7)～4.1×10~(-7)mol·m~(-2)·s~(-1)·Pa~(-1)were achieved.
Open-pore MFI zeolite nanosheets were prepared by removal of organic structure-directing agents(OSDA) from a multilamellar MFI zeolite(ML-MFI) using a mixture of 95%～98%(w/w)H_2SO_4 and 30%(w/w)H_2O_2 with V_(H_2SO_4)∶V_(H_2O_2)=3∶1(known as piranha solution), followed by ultrasonication for exfoliation and sedimentation for purification. The exfoliated MFI zeolite nanosheets were characterized by various techniques, such as X-ray diffraction(XRD), scanning electron microscope(SEM), transmittance electron microscope(TEM), N_2 adsorptiondesorption, Fourier transform infrared spectrometer(FT-IR) and thermal gravimetric analyzer(TGA), etc.,indicating that OSDA was removed after the piranha solution treatment and dispersed, open-pore MFI nanosheets were obtained followed by exfoliation through ultrasonication. Continuous MFI nanosheet membranes were prepared by depositing the open-pore MFI nanosheets on home-made alumina disc supports by a simple vacuumassisted filtration method. Single gas permeance tests on the MFI zeolite nanosheet membranes indicated that ideal selectivities for n-butane over i-butane of 4.1～5.8 with a permeance of n-butane of 2.2×10~(-7)～4.1×10~(-7)mol·m~(-2)·s~(-1)·Pa~(-1)were achieved.
引文
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[3]Zhuang X D, Mai Y Y, Wu D Q, et al. Adv. Mater., 2015,27(3):403-427
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[6]Li H, Song Z N, Zhang X J, et al. Science, 2013,342(6154):95-98
[7]Han Y, Xu Z, Gao C, et al. Adv. Funct. Mater., 2013,23(29):3693-3700
[8]Shen H P, Wang N X, Ma K, et al. J. Membr. Sci., 2017,527:43-50
[9]Chen L, Shi G S, Shen J, et al. Nature, 2017,550:380-383
[10]Peng Y, Li Y S, Ban Y J, et al. Science, 2014,346(6215):1356-1359
[11]Peng Y, Li Y S, Ban Y J, et al. Angew. Chem. Int. Ed.,2017,56(33):9757-9761
[12]Zhong Z X, Yao J F, Chen R Z, et al. J. Mater. Chem. A,2015,3(30):15715-15722
[13]Ying Y P, Liu D H, Ma J, et al. J. Mater. Chem. A, 2016,4(35):13444-13449
[14]Morigami Y, Kondo M, Abe J, et al. Sep. Purif. Technol.,2001,25(1/2/3):251-260
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[17]LIU Xiu-Feng(刘秀凤), LIU Wei(柳伟), ZHENG Meng-Yao(郑孟瑶), et al. Chinese J. Inorg. Chem.(无机化学学报),2014,30(12):2706-2712
[18]ZHANG Fei(张飞), ZHENG Yi-Hong(郑艺鸿), GUI Tian(桂田), et al. Chinese J. Inorg. Chem.(无机化学学报), 2014,30(8):1845-1854
[19]LUO Yi-Wei(罗益韦), PAN En-Ze(潘恩泽), CHU Jing-Jing(褚晶晶), et al. Chinese J. Inorg. Chem.(无机化学学报),2018,34(7):1351-1364
[20]Agrawal K V, Zhang X, Elyassi B, et al. Science, 2011,334(6052):72-75
[21]Zhang H, Xiao Q, Guo X H, et al. Angew. Chem. Int. Ed.,2016,559(25):7184-7187
[22]WANG Ya-Dan(王亚丹), XIAO Qiang(肖强), ZHONG YiJun(钟依均), et al. Acta Phys.-Chim. Sin.(物理化学学报),2017,33(10):2058-2063
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[25]Agrawal K V, Topuz B, Phan T C T, et al. Adv. Mater.,2015,27(21):3243-3249