渗透汽化异丙醇脱水ZSM-5沸石膜的制备与表征
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摘要
采用二次生长法在无有机模板剂条件下水热晶化制备高质量纯相ZSM-5沸石膜。考察了Na2O/SiO_2摩尔比和Na F/SiO_2摩尔比对制备ZSM-5沸石膜及其结构、形貌与渗透汽化异丙醇脱水分离性能的影响。结果表明,在较低Na2O/SiO_2摩尔比或Na F/SiO_2摩尔比下制备的沸石膜膜层结晶度低;而在较高Na2O/SiO_2摩尔比或Na F/SiO_2摩尔比时,易转晶生成mordenite沸石晶体;仅在Na2O/SiO_2摩尔比为0.17、Na F/SiO_2摩尔比为0.9时,制备出高质量纯相ZSM-5沸石膜,其膜层平整、连续、致密且结晶度高,该膜在渗透汽化异丙醇脱水中具有最佳的分离性能,其渗透通量为3.88 kg/(m2·h),水对异丙醇的分离系数达10 000以上。
High-quality pure phase ZSM-5 zeolite membranes are prepared through hydrothermal crystallization and secondary growth methods under situation of organo-template-free. The influences of the molar ratios of Na2 O/SiO_2 and Na F/SiO_2 on the preparation,structure,morphology and pervaporation performances of ZSM-5 zeolite membranes are investigated.The results show that ZSM-5 zeolite membranes prepared at lower molar ratio of Na2 O/SiO_2 or Na F/SiO_2 has a lower crystallinity in membrane layer,and mordenite crystals are easy to form at higher molar ratio of Na2 O/SiO_2 or Na F/SiO_2.Only when the molar ratios of Na2 O/SiO_2 and Na F/SiO_2 are 0. 17 and 0. 9,respectively,high-quality pure phase ZSM-5 zeolite membrane can be synthesized,with smooth,continuous,dense and high crystallinity. Such a ZSM-5 zeolite membrane shows high pervaporation performance in dehydration of isopropanol,with a flux of 3. 88 kg·m-2·h-1 and a separation factor of higher than 10 000 for dehydration of isopropanol.
High-quality pure phase ZSM-5 zeolite membranes are prepared through hydrothermal crystallization and secondary growth methods under situation of organo-template-free. The influences of the molar ratios of Na2 O/SiO_2 and Na F/SiO_2 on the preparation,structure,morphology and pervaporation performances of ZSM-5 zeolite membranes are investigated.The results show that ZSM-5 zeolite membranes prepared at lower molar ratio of Na2 O/SiO_2 or Na F/SiO_2 has a lower crystallinity in membrane layer,and mordenite crystals are easy to form at higher molar ratio of Na2 O/SiO_2 or Na F/SiO_2.Only when the molar ratios of Na2 O/SiO_2 and Na F/SiO_2 are 0. 17 and 0. 9,respectively,high-quality pure phase ZSM-5 zeolite membrane can be synthesized,with smooth,continuous,dense and high crystallinity. Such a ZSM-5 zeolite membrane shows high pervaporation performance in dehydration of isopropanol,with a flux of 3. 88 kg·m-2·h-1 and a separation factor of higher than 10 000 for dehydration of isopropanol.
引文
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[4]Budd P M,Elabas E S,Ghanem B S,et al.Solution-processed,organophilic membrane derived from a polymer of intrinsic microporosity[J].Adv Mater,2004,16(5):456-459.
[5]Wee S L,Tye C T,Bhatia S.Membrane separation process pervaporation through zeolite membrane[J].Sep Purif Technol,2008,63(3):500-516.
[6]Feng X,Huang R Y M.Liquid separation by membrane pervaporation:A review[J].Ind Eng Chem Res,1997,36(4):1048-1066.
[7]Shao P,Huang R Y M.Polymeric membrane pervaporation[J].J Membr Sci,2007,287(2):162-179.
[8]Li Y,Yang W.Microwave synthesis of zeolite membranes:A review[J].J Membr Sci,2008,316(1-2):3-17.
[9]Caro J,Noack M,K9lsch P,et al.Zeolite membranes-state of their development and perspective[J].Micropor Mesopor Mater,2000,38(1):3-24.
[10]Tavolaro A,Drioli E.Zeolite membranes[J].Adv Mater,1999,11(12):975-996.
[11]Morigami Y,Kondo M,Abe J,et al.The first large-scale pervaporation plant using tubular-type module with zeolite Na A membrane[J].Sep Purif Technol,2001,25(1-3):251-260.
[12]Li L,Yang J,Li J,et al.Synthesis of high performance mordenite membranes from fluoride-containing dilute solution under microwave-assisted heating[J].J Membr Sci,2016,512:83-92.
[13]Kondo M,Kita H.Permeation mechanism through zeolite Na A and T-type membranes for practical dehydration of organic solvents[J].J Membr Sci,2010,361(1-2):223-231.
[14]Li L,Yang J,Li J,et al.High performance ZSM-5 membranes on coarse macroporousα-Al2O3supports for dehydration of alcohols[J].AICh E J,2016,62(8):2813-2824.
[15]Bakker W J W,Van Den Broeke L J P,Kapteijn F,et al.Temperature dependence of one-component permeation through a silicalite-1membrane[J].AICh E J,1997,43(9):2203-2214.
[16]Lai Z,Tsapatsis M,Nicolich J P.Siliceous ZSM-5 membranes by secondary growth of b-oriented seed layers[J].Adv Funct Mater,2004,14(7):716-729.
[17]Gao X,Zou X,Zhang F,et al.Eco-friendly fabrication of hydrophilic ZSM-5 membranes for alcohol upgrading[J].Chem Commun,2013,49(78):8839-8841.
[18]Korelskiy D,Leppjrvi T,Zhou H,et al.High flux MFI membranes for pervaporation[J].J Membr Sci,2013,427:381-389.
[19]Coronas J,Falconer J L,Noble R D.Characterization and permeation properties of ZSM-5 tubular membranes[J].AICh E J,1997,43(7):1797-1812.
[20]Schoeman B J.ZSM-5 films prepared from template free precursors[J].J Mater Chem,1998,8(10):2217-2221.
[21]Li G,Kikuchi E,Matsukata M.A study on the pervaporation of water-acetic acid mixtures through ZSM-5 zeolite membranes[J].J Membr Sci,2003,218(1-2):185-194.
[22]Kim S D,Noh S H,Seong K H,et al.Compositional and kinetic study on the rapid crystallization of ZSM-5 in the absence of organic template under stirring[J].Micropor Mesopor Mater,2004,72(1-3):185-192.