• •
收稿日期:
2024-06-07
修回日期:
2024-07-07
出版日期:
2024-07-17
通讯作者:
金万勤
作者简介:
赵静(1989—),女,博士,教授, zhaojingmem@njtech.edu.cn
基金资助:
Jing ZHAO1(), Gongping LIU1, Wanqin JIN1(
), Nanping XU2
Received:
2024-06-07
Revised:
2024-07-07
Online:
2024-07-17
Contact:
Wanqin JIN
摘要:
限域传质分离膜面向分子/离子的亚纳米尺度高精度分离,是目前国内外膜领域研究的热点和难点。厘清膜内的限域传质效应,形成共性传质机制及调控方法,是突破trade-off效应,实现超常膜分离性能的关键途径。本文从限域传质通道构筑、限域传质机理及限域传质分离膜应用三个方面入手,对限域传质分离膜近年来的研究进展进行举例介绍与讨论,并对限域传质分离膜的未来发展方向进行了思考与展望,以期为高性能膜材料的设计与应用提供参考。
中图分类号:
赵静, 刘公平, 金万勤, 徐南平. 限域传质分离膜的精密构筑与应用[J]. 化工学报, DOI: 10.11949/0438-1157.20240639.
Jing ZHAO, Gongping LIU, Wanqin JIN, Nanping XU. Precise construction and application of separation membranes based on confined mass transfer mechanism[J]. CIESC Journal, DOI: 10.11949/0438-1157.20240639.
图1 (a)柱芳烃组装形成纳米管示意图[8],(b)柱芳烃纳米管镶嵌于双分子层结构示意图[8],(c)环肽分子与嵌段共聚物共组装形成纳米管结构示意图[17]
Fig.1 Schematic diagrams of (a) formation of nanotube through assembly of pillar[5]arene[8], (b) embedding of nanotubes in bilayers[8], (c) assembly of cyclic peptide with the assistance of block copolymer[17]
图2 (a)K+固定GO膜层间距实现离子截留示意图[29],(b)GO膜在纯水及不同盐溶液中层间距[29],(c)经KCl浸泡后GO膜在不同盐溶液中的层间距[29],(d)MXene膜内通道从“扩散主导型”变为“溶解主导型”示意图[20],(e)MXene膜改性前后溶解选择性与扩散选择性变化(MB:MXene+硼酸;MBP:Mxene+硼酸+聚乙烯亚胺)[20],(f)MXene/PSS复合膜内Li+快速传递亚纳米通道示意图[21],(g)MXene/PSS复合膜离子渗透速率及选择性随PSS含量变化[21]
Fig.2 (a) A schematic of how K+ ions fix the interlayer spacing of GO membrane such that other cations are rejected[29], (b) Interlayer spacings for GO membranes immersed in pure water or in various salt solutions[29], (c) Interlayer spacings of GO membranes that were soaked in KCl solution, followed by being immersed in various salt solutions[29], (d) schematic of the transformation of MXene channels from “diffusion-controlled” to“solution-controlled”[20], (e) change of sorption selectivity and diffusion selectivity after chemical tuning of MXene membrane (MB: MXene+borate; MBP: MXene+borate+PEI)[20], (f) schematic of the fast transport subnanochannels for Li+ in MXene/PSS composite membranes[21], (g) the PSS content dependent ion permeation rates and permselectivity of MXene/PSS composite membrane[21]
图3 (a)“固态溶剂法”制备超薄高填充MOFs混合基质膜示意图[53],(b)不同填充量下非取向片状分子筛在高分子基质中的分布示意图[54],(c)具有准连续分子筛相的混合基质膜及片状Na-SSZ-39分子筛三维通道中CO2渗透(绿色箭头)路径示意图[54],(d)通过UiO-66与PIM-1结合构建CO2高速传递路径示意图[43]
Fig.3 Schematic diagram of fabricating ultrathin and high-loading MOFs mixed matrix membranes via a solid-solvent processing strategy[53], (b) illustration of the nonaligned zeolite platelet distribution in the polymer matrix with different zeolite loadings[54], (c) illustration of the mixed matrix membrane with quasi-continuous zeolite phase and the unhindered CO2 permeation (indicated with green arrows) through the 3D-channel system of platelet-shaped Na-SSZ-39 filler[54], (d) schematic diagram of building CO2 transport freeways through interweaving UiO-66 and PIM-1[43]
图4 (a)不同溶剂分子在Ti3C2/graphene通道内的通量测定值与计算值[60],(b)石墨烯膜对不同水/醇体系(水/乙醇,水/正丁醇,水/异丙醇)分离选择性的实验值与计算值[61]
Fig.4 (a) The experimental fluxes (purple stars) and predicted fluxes (bars) of different solvents through Ti3C2/graphene channels [60], (b) the experimental and predicted selectivitiesof different water/alcohol systems (water/ethanol, water/n-butanol, and water/isopropanol) in graphene-based membranes[61]
图5 (a)UiO-66-(COOH)2亚纳米通道(MOFSNC)的离子筛分机理及(b)二元离子选择性(K+/Mg2+,Na+/Mg2+,Li+/Mg2+)[63],(c)磺酸共价三嗪框架膜内刚性离子通道示意图[65],(d)联苯共价三嗪框架(SCTF-BP)分子结构[65],(e)不同膜内及水溶液中Na+扩散系数[65]
Fig.5 (a) Ion sieving mechanism and (b) binary K+/Mg2+, Na+/Mg2+ and Li+/Mg2+ selectivities in the UiO-66-(COOH)2 subnanochannels (MOFSNC)[63], (c) schematic diagram of the rigid ion channels in sulfonated SCTF (SCTF) membrane[65], (d) molecular structure of SCTF- biphenyl (SCTF-BP)[65], (e) diffusion coefficients of Na+ in water and different membrane samples[65]
图6 (a)用于膜蒸馏的亲水梯度结构COF膜示意图[66],(b)孔径对水蒸发通量的影响(分子模拟)[66],(c)通过COF纳米片与纳米带结合形成的COF膜内通道结构与作用力示意图[67],(d)温度对COF膜渗透通量的影响[67],(e)Ti3C2/石墨烯复合膜结构示意图[60],(f)温度对不同组成Ti3C2/石墨烯复合膜水通量的影响[60]
Fig.6 (a) Schematic illustration of the COF membrane with hydrophilicity gradient for membrane distillation[66], (b) water evaporation flux as a function of pore diameter (molecular dynamics simulations)[66], (c) Schematic for the channel structures and interactions in the COF membranes formed through binding of COF nanosheets and nanoribbons[67], (d) temperature-dependent permeation flux of COF membrane[67], (e) schematic illustration of the Ti3C2-graphene membrane structure[60], (f) water flux of the Ti3C2-graphene hetero-channel membranes under different feed temperatures[60]
图7 (a)无晶格缺陷的MOF晶体膜制备过程示意图[71],(b)不同有机配体/金属团簇化学计量比倍增因子下Zr-MOF(富马酸)膜的缺陷浓度及H2/CO2选择性[71],(c)MOF-COF合金膜制备过程示意图[72],(d)MOF-COF合金膜的C3H6/C3H8混合气分离性能[72],(e)热处理前后RUB沸石膜内气体传递通道结构对比[36]
Fig.7 (a) Schematic diagram of the formation of MOF membranes with perfect lattices[71], (b) the defect concentration and H2/CO2 selectivity of Zr-MOF(fumarate) membranes prepared using various multiplicative factors of the ligand/SBU stoichiometric ratio[71], (c) schematic diagram of the construction of MOF–COF alloy membranes[72], (d) Mixed C3H6/C3H8 separation performance of the MOF-COF alloy membrane[72], (e) comparison of the gas transport channel strctures in RUB zeolite membranes before and after calcination[36]
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