在石油工业、生物制药以及有机合成等领域中,化工产品的生产、分离与提纯需要使用大量有机溶剂,因此有机溶剂的回收显得至关重要。渗透汽化作为一种新兴的膜分离技术引起了人们的广泛关注。以1,2-双(三乙氧基硅基)乙烷(BTESE)、1,6-双(三甲氧基硅基)己烷(BTMSH)、1,8-双(三乙氧基硅基)辛烷(BTESO)为有机硅前驱体,采用溶胶-凝胶法制备有机硅膜,并将其用于有机溶剂混合物(甲醇/甲苯、甲醇/碳酸二甲酯)的渗透汽化分离。考察了前驱体烷基链的长短、原料液甲醇浓度、渗透汽化温度等因素对膜性能的影响。结果表明:在相同的实验条件下,随着烷基链的增加,膜的渗透通量增大,分离因子减小。对于同一种膜,随着原料液甲醇含量的增加,其渗透通量逐渐增加,分离因子减小。
The synthesis,separation and purification of chemical products require the use of a large amount of organic solvents in fields such as the petroleum industry,biopharmaceutical industry,and organic synthesis.Therefore,the recovery of organic solvents was of crucial importance.As a relatively new separation technology,pervaporation has attracted widespread attention.In this study,organosilica membranes were prepared via the sol-gel method by using 1,2-bis(triethoxysilyl)ethane (BTESE),1,6-bis(trimethoxysilyl)hexane (BTMSH),and 1,8-bis(triethoxysilyl)octane (BTESO) as organosilica precursors.The fabricated membranes were used for the pervaporation separation of organic solvent mixtures (methanol/toluene,methanol/dimethyl carbonate).The effects of the length of alkyl chain of the precursor,the methanol concentration of feed solution,and the pervaporation temperature on the membrane performance were investigated.The experimental results showed that the permeation flux of the membrane increased and the separation factor decreased as the alkyl chain increased under the same experimental conditions.For the same membrane,as the methanol content of the feed solution increased,the permeation flux gradually increased while the separation factor decreased.
[1] Wang W,Xu L,Wang X,et al.Measurement and correlation of vapor-liquid equilibrium data of the toluene,o-chlorotoluene,and p-chlorotoluene system at 101.3kPa[J].Journal of Chemical & Engineering Data,2022,67(11):3426-3434.
[2] Číhal P,Vopička O,Durd'áková T M,et al.Pervaporation and vapour permeation of methanol-dimethyl carbonate mixtures through PIM-1 membranes[J].Separation and Purification Technology,2019,217:206-214.
[3] Raza W,Wang J,Yang J,et al.Progress in pervaporation membranes for dehydration of acetic acid[J].Separation and Purification Technology,2021,262:118338.
[4] Ong Y K,Shi G M,Le N L,et al.Recent membrane development for pervaporation processes[J].Progress in Polymer Science,2016,57:1-31.
[5] Park H C,Meertens R M,Mulder M H V,et al.Pervaporation of alcohol-toluene mixtures through polymer blend membranes of poly(acrylic acid) and poly(vinyl alcohol)[J].Journal of Membrane Science,1994,90(3):265-274.
[6] Chen X,Zhu M,Xiang S,et al.Growth process and short chain alcohol separation performance of fluoride-containing NaY zeolite membrane[J].Chinese Journal of Chemical Engineering,2021,29:154-159.
[7] Nian P,Ma C,Liu H,et al.High-performance Co-based ZIF-67 tubular membrane achieved by ZnO-induced synthesis for highly efficient pervaporation separation of methanol/methyl tert-butyl ether mixture[J].Industrial & Engineering Chemistry,2019,58(33):15297-15306.
[8] Dong G,Nagasawa H,Yu L,et al.Pervaporation removal of methanol from methanol/organic azeotropes using organosilica membranes:experimental and modeling[J].Journal of Membrane Science,2020,610:118284.
[9] Anggarini U,Yu L,Nagasawa H,et al.Microporous Nickel-coordinated aminosilica membranes for improved pervaporation performance of methanol/toluene separation[J].ACS Applied Materials & Interfaces,2021,13(19):23247-23259.
[10] Yu X,Nagasawa H,Kanezashi M,et al.Improved thermal and oxidation stability of bis(triethoxysilyl)ethane (BTESE)-derived membranes,and their gas-permeation properties[J].Journal of Materials Chemistry A,2018,6(46):23378-23387.
[11] Yang J,Yoshioka T,Tsuru T,et al.Pervaporation characteristics of aqueous-organic solutions with microporous SiO2-ZrO2 membranes:experimental study on separation mechanism[J].Journal of Membrane Science,2006,284(1):205-213.
[12] Dong G,Nagasawa H,Yu L,et al.Energy-efficient separation of organic liquids using organosilica membranes via a reverse osmosis route[J].Journal of Membrane Science,2020,597:117758.
[13] Cheng L,Guo M,Zhong J,et al.Network engineering of organosilica membranes for efficient pervaporation dehydration[J].Separation and Purification Technology,2024,344:127105.
[14] Polotskaya G,Tian N,Faykov I,et al.Novel design of Co-poly(hydrazide imide) and its complex with Cu(Ⅰ) for membrane separation of methanol/dimethyl carbonate mixture[J].Membranes,2023,13(2):160.
[15] Van der Bruggen B,Schaep J,Wilms D,et al.Influence of molecular size,polarity and charge on the retention of organic molecules by nanofiltration[J].Journal of Membrane Science,1999,156(1):29-41.
[16] Pyo S H,Park J H,Chang T S,et al.Dimethyl carbonate as a green chemical[J].Current Opinion in Green and Sustainable Chemistry,2017,5:61-66.
[17] Yu X,Meng L,Niimi T,et al.Network engineering of a BTESE membrane for improved gas performance via a novel pH-swing method[J].Journal of Membrane Science,2016,511:219-227.
[18] Ngamou P H T,Overbeek J P,Kreiter R,et al.Plasma-deposited hybrid silica membranes with a controlled retention of organic bridges[J].Journal of Materials Chemistry A,2013,1(18):5567-5576.
[19] Kaneko K,Ishii C,Ruike M,et al.Origin of superhigh surface area and microcrystalline graphitic structures of activated carbons[J].Carbon,1992,30(7):1075-1088.
[20] Kanezashi M,Yoneda Y,Nagasawa H,et al.Gas permeation properties for organosilica membranes with different Si/C ratios and evaluation of microporous structures[J].AlChE Journal,2017,63(10):4491-4498.
[21] Svang-Ariyaskul A,Huang R Y M,Douglas P L,et al.Blended chitosan and polyvinyl alcohol membranes for the pervaporation dehydration of isopropanol[J].Journal of Membrane Science,2006,280(1):815-823.
[22] Niimi T,Nagasawa H,Kanezashi M,et al.Preparation of BTESE-derived organosilica membranes for catalytic membrane reactors of methylcyclohexane dehydrogenation[J].Journal of Membrane Science,2014,455:375-383.
[23] Wang Q,Yu L,Nagasawa H,et al.High-performance molecular-separation ceramic membranes derived from oxidative cross-linked polytitanocarbosilane[J].Journal of the American Ceramic Society,2020,103(8):4473-4488.
[24] Garg P,Singh R P,Choudhary V.Pervaporation separation of organic azeotrope using poly(dimethyl siloxane)/clay nanocomposite membranes[J].Separation and Purification Technology,2011,80(3):435-444.
[25] Huang R Y M,Moon G Y,Pal R.N-acetylated chitosan membranes for the pervaporation separation of alcohol/toluene mixtures[J].Journal of Membrane Science,2000,176(2):223-231.
[26] Moriyama N,Nagasawa H,Kanezashi M,et al.Pervaporation dehydration of aqueous solutions of various types of molecules via organosilica membranes:effect of membrane pore sizes and molecular sizes[J].Separation and Purification Technology,2018,207:108-115.
[27] Wang L,Li J,Lin Y,et al.Separation of dimethyl carbonate/methanol mixtures by pervaporation with poly(acrylic acid)/poly(vinyl alcohol) blend membranes[J].Journal of Membrane Science,2007,305(1-2):238-246.
[28] Chen J H,Dong X F,He Y S.Investigation into glutaraldehyde crosslinked chitosan/cardo-poly-etherketone composite membrane for pervaporation separation of methanol and dimethyl carbonate mixtures[J].RSC Advances,2016,6(65):60765-60772.
[29] Won W,Feng X,Lawless D.Pervaporation with chitosan membranes:separation of dimethyl carbonate/methanol/water mixtures[J].Journal of Membrane Science,2002,209(2):493-508.
[30] Chen J H,Liu Q L,Zhu A M,et al.Pervaporation separation of MeOH/DMC mixtures using STA/CS hybrid membranes[J].Journal of Membrane Science,2008,315(1):74-81.
[31] Sun Q,Ma H,Wu L,et al.Molecular simulation for guiding the design and optimization of mixed matrix membranes (MMMs) in the pervaporation process[J].Langmuir,2023,39(14):5199-5210.
基金资助
江苏省研究生科研与实践创新计划项目(SJCX24＿1613)
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