CHA分子筛膜用于DMF渗透汽化脱水研究
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摘要
将氧化钇稳定型氧化锆(YSZ)中空纤维载体上制备的CHA分子筛膜用于二甲基甲酰胺(DMF)渗透汽化脱水,系统考察了进料水含量和操作温度对膜分离性能的影响,并研究了CHA分子筛膜渗透汽化的长期稳定性。结果表明:膜的渗透水通量随进料水含量和操作温度的升高而增加;对于质量分数为10.0%水/DMF溶液,当操作温度为75℃时,CHA分子筛膜的初始渗透水通量和分离因子分别为5.7 kg/(m~2·h)和1 180;DMF分子在CHA分子筛膜表面和孔道内的吸附阻碍了水的渗透,膜的渗透水通量逐渐下降并在24 h后稳定在1.0 kg/(m~2·h)左右,渗透侧水质量分数稳定在99.0%以上。
A CHA zeolite membrane supported on external surface of yttria-stabilized zirconia( YSZ)hollow fiber was used for pervaporation( PV) dehydration of dimethylformamide( DMF). Effects of feed water content and operating temperature on separation performance of the membrane were investigated.The long-term PV stability of CHA zeolite membrane was also studied. Results showed that water fluxes increased with the increasing water content and operation temperature in the water/DMF mixture. The membrane exhibited a high water permeation flux of 5. 7 kg/(m~2·h) together with a separation factor of 1 180 at 75 ℃ in dehydration of 10. 0% water/DMF mixture.Due to the adsorption of DMF on membrane surface and in pores,the water permeation flux initially decreased and then stabilized at about 1. 0 kg/(m~2·h) after 24 h stabilization period and the water content in permeate stabilized at above 99. 0%.
A CHA zeolite membrane supported on external surface of yttria-stabilized zirconia( YSZ)hollow fiber was used for pervaporation( PV) dehydration of dimethylformamide( DMF). Effects of feed water content and operating temperature on separation performance of the membrane were investigated.The long-term PV stability of CHA zeolite membrane was also studied. Results showed that water fluxes increased with the increasing water content and operation temperature in the water/DMF mixture. The membrane exhibited a high water permeation flux of 5. 7 kg/(m~2·h) together with a separation factor of 1 180 at 75 ℃ in dehydration of 10. 0% water/DMF mixture.Due to the adsorption of DMF on membrane surface and in pores,the water permeation flux initially decreased and then stabilized at about 1. 0 kg/(m~2·h) after 24 h stabilization period and the water content in permeate stabilized at above 99. 0%.
引文
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[16]HU N,LI Y Q,ZHONG S L,et al.Fluoride-mediated synthesis of high-flux chabazite membranes for pervaporation of ethanol using reusable macroporous stainless steel tubes[J].Journal of membrane science,2016,510:91.
[17]HASEGAWA Y,HOTTA H,SATO K,et al.Preparation of novel chabazite(CHA)-type zeolite layer on porous alpha-Al2O3tube using template-free solution[J].Journal of membrane science,2010,347:193.
[18]JIANG J,WANG X R,ZHANG Y T,et al.Fabrication of purephase CHA zeolite membranes with ball-milled seeds at low K+concentration[J].Microporous and mesoporous materials,2015,215:98.
[19]PERA-TITUS M,BAUSACH M,LLORENS J,et al.Preparation of inner-side tubular zeolite Na A membranes in a continuous flow system[J].Seperation and purification technology,2008,59:141.
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[2]DEVI D A,SMITHA B,SRIDHAR S,et al.Pervaporation separation of dimethylformamide/water mixtures through poly(vinyl alcohol)/poly(acrylic acid)blend membranes[J].Seperation and purification technology,2006,51:104.
[3]何勇,王学瑞,陈园园,等.真空抽吸晶种涂覆法制备中空纤维Na A分子筛膜[J].南京工业大学学报(自然科学版),2013,35(5):24.
[4]ZHU M H,KUMAKIRI I,TANAKA K,et al.Dehydration of acetic acid and esterification product by acid-stable ZSM-5 membrane[J].Microporous and mesoporous materials,2013,15:47.
[5]姜华,张玉亭,魏潇,等.中空纤维Na Y分子筛膜的制备与表征[J].南京工业大学学报(自然科学版),2015,37(5):27.
[6]WANG X R,CHEN Y Y,ZHANG C,et al.Preparation and characterization of high-flux T-type zeolite membranes supported on YSZ hollow fibers[J].Journal of membrane science,2014,455:294.
[7]RANGNEKAR N,MITTAL N,ELYASSI B,et al.Zeolite membranes:a review and comparison with MOFs[J].Chemical society reviews,2015,44(20):7128.
[8]KITA H,HORII K,OHTOSHI Y,et al.Synthesis of a zeolite Na A membrane for pervaporation of water/organic liquid mixtures[J].Journal of materials science letters,1995,14(3):206.
[9]SHAH D,KISSICK K,GHORPADE A,et al.Pervaporation of alcohol-water and dimethylformamide-water mixtures using hydrophilic zeolite Na A membranes:mechanisms and experimental results[J].Journal of membrane science,2000,179(1/2):185.
[10]LI Y S,ZHOU H,ZHU G Q,et al.Hydrothermal stability of LTA zeolite membranes in pervaporation[J].Journal of membrane science,2007,297:10.
[11]YAMANAKA N,ITAKURA M,KIYOZUMI Y,et al.Acid stability evaluation of CHA-type zeolites synthesized by interzeolite conversion of FAU-type zeolite and their membrane application for dehydration of acetic acid aqueous solution[J].Microporous and mesoporous materials,2012,158:141.
[12]SATO K,SUGIMOTO K,SHIMOTSUMA N,et al.Development of practically available up-scaled high-silica CHA-type zeolite membranes for industrial purpose in dehydration of Nmethylpyrrolidone solution[J].Journal of membrane science,2012,409:82.
[13]HASEGAWA Y,HOTTA H,SATO K,et al.Preparation of novel chabazite(CHA)-type zeolite layer on porous alpha-Al2O3tube using template-free solution[J].Journal of membrane science,2010,347:193.
[14]ITOH N,TOKUNAGA T,SATO K,et al.Two-step enhanced dehydration of IPA-water vapor mixture using water-selective CHA zeolite membrane in continuously recycling system[J].Kagaku Kogaku ronbunshu(in Japanese),2016,42(1):8.
[15]HU N,LI Y Q,ZHONG S L,et al.Microwave synthesis of zeolite CHA(chabazite)membranes with high pervaporation performance in absence of organic structure directingagents[J].Microporous and mesoporous materials,2016,228:22.
[16]HU N,LI Y Q,ZHONG S L,et al.Fluoride-mediated synthesis of high-flux chabazite membranes for pervaporation of ethanol using reusable macroporous stainless steel tubes[J].Journal of membrane science,2016,510:91.
[17]HASEGAWA Y,HOTTA H,SATO K,et al.Preparation of novel chabazite(CHA)-type zeolite layer on porous alpha-Al2O3tube using template-free solution[J].Journal of membrane science,2010,347:193.
[18]JIANG J,WANG X R,ZHANG Y T,et al.Fabrication of purephase CHA zeolite membranes with ball-milled seeds at low K+concentration[J].Microporous and mesoporous materials,2015,215:98.
[19]PERA-TITUS M,BAUSACH M,LLORENS J,et al.Preparation of inner-side tubular zeolite Na A membranes in a continuous flow system[J].Seperation and purification technology,2008,59:141.
[20]PERA-TITUS M,LLORENS J,TEJERO J,et al.Description of the pervaporation dehydration performance of A-type zeolite membranes:a modeling apporach based on the Maxwell-Stefan theory[J].Catalysis today,2006,118:73.
[21]杨占照,刘艳梅,顾学红,等.管式支撑体内表面Na A分子筛膜的合成与表征[J].化工学报,2011,62(3):840.