| 13 | 0 | 21 |
| 下载次数 | 被引频次 | 阅读次数 |
聚砜-聚酰胺复合膜(TFC膜)的聚酰胺选择层是水盐分离核心，但其20～200nm的超薄结构使传输行为难以量化，制约了膜的发展。主流交联芳香聚酰胺反渗透膜中，均苯三甲酰氯(TMC)水解引入的羧基官能团对分离性能影响显著。本研究从聚酰胺结构出发，以低温溶液缩聚法制备不同羧基含量的线性芳香聚酰胺，基于溶解-扩散理论，探究羧基含量对其均质膜盐传输性能的影响。研究结果表明：随着聚合物中羧基单体含量的增加，聚合物玻璃化转变温度(Tg)增加，聚合物膜水吸收(Kw)变化不显著，可看成等水含量的聚合物膜；羧基单体含量的增加有助于提高聚合物膜表面荷负电性，降低聚合物膜中自由水含量以及自由体积；盐吸收(KS)、盐扩散(DS)与盐渗透(PS)随聚合物膜中羧基含量增加显著降低。
Abstract：The polyamide selective layer in the polysulfone-polyamide thin film composite(TFC)membranes is crucial for the separation of water and salt.However,its ultra-thin structure(20～200 nm)makes it challenging to quantify transport behavior,limiting membrane development.In mainstream crosslinked aromatic polyamide reverse osmosis membranes,carboxyl groups introduced by hydrolysis of trimesoyl chloride(TMC)significantly affect separation performance.Therefore,based on the structure of polyamide,this study prepared linear aromatic polyamide polymers with different carboxyl group contents by low-temperature solution polycondensation.Based on the solution-diffusion theory,the effect of carboxyl group content on salt transport performance was investigated.The results showed that with the increase of carboxyl monomer content in the polymer,the glass transition temperature(Tg)of the polymer increased.The water sorption(Kw)of the polymer membranes had no significant change,indicating membranes with equivalent water content.The increase of carboxyl monomer content enhanced the surface charge of the polymer membranes,decreasing the free water content and the free volume of polyamides.The salt sorption(KS),salt diffusivity(DS)and salt permeability(PS)decreased significantly with the increase of carboxyl group content in polymer membranes.
[1]龙海彧．价值链视角下中国省级水资源利用动态变迁及其影响因素研究[D]．长沙：湖南大学，2023.
[2] LIU Weifan,LIVINGSTON J L,WANG Li,et al.Pressure-driven membrane desalination[J].Nature Reviews Methods Primers,2024,4:10.DOI:10.1038/s43586-023-00287-y.
[3] SARKAR P,WU Chenyue,YANG Zhe,et al.Empowering ultrathin polyamide membranes at the water-energy nexus:strategies,limitations,and future perspectives[J].Chemical Society Reviews,2024,53(9):4374-4399.
[4] HU Mingguang,ZHANG Chenchen,YOU Meng,et al.Water/salt transport properties of polyamide reverse osmosis membranes using quartz crystal microbalance[J].ACS Applied Polymer Materials,2023,5(9):7252-7262.
[5] XU Jian,YAN Hao,ZHANG Yang,et al.The morphology of fully-aromatic polyamide separation layer and its relationship with separation performance of TFC membranes[J].Journal of Membrane Science,2017,541:174-188.
[6] FRASER A C,CHEW N G P,HEGDE M,et al.Linear versus nonlinear aromatic polyamides:the role of backbone geometry in thin film salt exclusion membranes[J].ACS Applied Materials&Interfaces,2022,14(31):36143-36156.
[7] AHMED F E,HASHAIKEH R,DIABAT A,et al.Mathematical and optimization modelling in desalination:state-ofthe-art and future direction[J].Desalination,2019,469:114092.DOI:10.1016/j.desal.2019.114092.
[8] WANG Fei,YANG Zhe,TANG Chunyang.Modeling water transport in interlayered thin-film nanocomposite membranes:gutter effect vs funnel effect[J].ACS ES&T Engineering,2022,2(11):2023-2033.
[9] GEISE G M,LEE H S,MILLER D J,et al.Water purification by membranes:the role of polymer science[J].Journal of Polymer Science Part B-Polymer Physics,2010,48(15):1685-1718.
[10]FROMMER M A,MURDAY J S,MESSALEM R M.Solubility and diffusivity of water and of salts in an aromatic polyamide film[J].European Polymer Journal,1973,9(4):367-373.
[11]JIN Ying,SU Zhaohui.Effects of polymerization conditions on hydrophilic groups in aromatic polyamide thin films[J].Journal of Membrane Science,2009,330(1/2):175-179.
[12]LUO Hongxi,CHANG K,BAHATI K,et al.Functional group configuration influences salt transport in desalination membrane materials[J].Journal of Membrane Science,2019,590:117295.DOI:10.1016/j.memsci.2019.117295.
[13]GEISE G M,PAUL D R,FREEMAN B D.Fundamental water and salt transport properties of polymeric materials[J].Progress in Polymer Science,2014,39(1):1-42.
[14]SHABBIR S,ZULFIQAR S,SARWAR M I.Amine-terminated aromatic and semi-aromatic hyperbranched polyamides:synthesis and characterization[J].Journal of Polymer Research,2011,18:1919-1929.
[15]TAMBOLI A B,MALDAR N N.Soluble aromatic polyamides containing pendant pentadecyl substituted methoxy phenyl unit[J].Journal of Polymer Research,2019,26(6):139.DOI:10.1007/s10965-019-1799-0.
[16]SHABAAN A K E,HASSAN A E,SAADULLAH G A.Effects of protonation and deprotonation on the reactivity of quinolone:a theoretical study[J].Chinese Science Bulletin,2012,57(14):1665-1671.
基本信息:
DOI：10.16191/j.cnki.hbkx.2025.05.006
中图分类号:TQ051.893
引用信息:
[1]胡明广,白璐,陈孝起,等.羧基化芳香聚酰胺膜材料的盐传输行为研究[J].河北省科学院学报,2025,42(05):39-47.DOI:10.16191/j.cnki.hbkx.2025.05.006.
基金信息:
河北省科学院科技计划项目博士科研启动项目（25B701）
