限域传质分离膜的精密构筑与应用

doi:10.11949/0438-1157.20240639

摘要/Abstract

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。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。

关键词: 限域传质, 亚纳米通道, 膜, 分离, 传递

Abstract:

The sub-nanometer high-precision separation of molecules/ions by confined mass transfer separation membranes is a hot topic and difficulty in the current membrane research field. Clarifying the confined mass transfer effect within the membrane, forming a common mass transfer mechanism and manipulation methods, is a key way to break through the trade-off effect and achieve extraordinary membrane separation performance. This article reviews the research progresses of confined mass transfer separation membranes in recent years from three aspects: the construction of confined mass transfer channels, the confined mass transfer mechanism, and the application of confined mass transfer separation membranes. The future development direction of confined mass transfer separation membranes has also been proposed, which is expected to provide reference for the design and application of high-performance membrane materials.

Key words: confined mass transfer, sub-nanometer channels, membrane, separation, transport

中图分类号:

TQ 028.8

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, 2024, 75(11): 3857-3869.

Jing ZHAO, Gongping LIU, Wanqin JIN, Nanping XU. Precision construction and application of separation membranes based on confined mass transfer mechanism[J]. CIESC Journal, 2024, 75(11): 3857-3869.

图/表 7

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 formation of nanotube through assembly of pillar[5]arene[8] (a); embedding of nanotubes in bilayers[8] (b), assembly of cyclic peptide with the assistance of block copolymer[17](c)

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的层间距[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 selectivities of 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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