Reducing active layer thickness of polyamide composite membranes using a covalent organic framework interlayer in interfacial polymerization

doi:10.1016/j.cjche.2019.11.007

Abstract

Abstract: Polyamide (PA)-based thin-film composite membranes exhibit enormous potential in water purification, owing to their facile fabrication, decent performance and desirable stability. However, the thick PA active layer with high transport resistance from the conventional interfacial polymerization hampers their applications. The controllable fabrication of a thin PA active layer is essential for high separation efficiency but still challenging. Herein, a covalent organic framework TpPa-1 interlayer was firstly deposited on a polyethersulfone (PES) substrate to reduce the thickness of PA active layer in interfacial polymerization. The abundant pores of TpPa-1 increase the local concentration of amine monomers by adsorbing piperazine molecules, while hydrogen bonds between hydrophilic groups of TpPa-1 and piperazine molecules slow down their diffusion rate. Arising from those synergetic effects, the PA active layer is effectively reduced from 200 nm to 120 nm. By optimizing TpPa-1 interlayer and PA active layer, the water flux of resultant membranes can reach 171.35 L·m^-2·h^-1·MPa^-1, which increased by 125.4% compared with PA/PES membranes, while the rejection rates of sodium sulfate and dyes solution remained more than 90% and 99%, respectively. Our strategy may stimulate rational design of ultrathin PA-based nanofiltration membranes with high performances.

Key words: Thin film composite membranes, Interfacial polymerization, Covalent organic frameworks interlayer, Nanofiltration

摘要： Polyamide (PA)-based thin-film composite membranes exhibit enormous potential in water purification, owing to their facile fabrication, decent performance and desirable stability. However, the thick PA active layer with high transport resistance from the conventional interfacial polymerization hampers their applications. The controllable fabrication of a thin PA active layer is essential for high separation efficiency but still challenging. Herein, a covalent organic framework TpPa-1 interlayer was firstly deposited on a polyethersulfone (PES) substrate to reduce the thickness of PA active layer in interfacial polymerization. The abundant pores of TpPa-1 increase the local concentration of amine monomers by adsorbing piperazine molecules, while hydrogen bonds between hydrophilic groups of TpPa-1 and piperazine molecules slow down their diffusion rate. Arising from those synergetic effects, the PA active layer is effectively reduced from 200 nm to 120 nm. By optimizing TpPa-1 interlayer and PA active layer, the water flux of resultant membranes can reach 171.35 L·m^-2·h^-1·MPa^-1, which increased by 125.4% compared with PA/PES membranes, while the rejection rates of sodium sulfate and dyes solution remained more than 90% and 99%, respectively. Our strategy may stimulate rational design of ultrathin PA-based nanofiltration membranes with high performances.

关键词: Thin film composite membranes, Interfacial polymerization, Covalent organic frameworks interlayer, Nanofiltration

Meidi Wang, Weixiong Guo, Zhongyi Jiang, Fusheng Pan. Reducing active layer thickness of polyamide composite membranes using a covalent organic framework interlayer in interfacial polymerization[J]. Chinese Journal of Chemical Engineering, 2020, 28(4): 1039-1045.

References

[1] P. Marchetti, M.F. Jimenez Solomon, G. Szekely, A.G. Livingston, Molecular separation with organic solvent nanofiltration:a critical review, Chem. Rev. 114(2014) 10735-10806.
[2] R. Bi, R. Zhang, J. Shen, Y.N. Liu, M. He, X. You, Y. Su, Z. Jiang, Graphene quantum dots engineered nanofiltration membrane for ultrafast molecular separation, J. Membr. Sci. 572(2019) 504-511.
[3] J.R. Werber, C.O. Osuji, M. Elimelech, Materials for next-generation desalination and water purification membranes, Nat. Rev. Mater. 1(2016).
[4] Y.L. Ji, W.J. Qian, Y.W. Yu, Q.F. An, L.F. Liu, Y. Zhou, C.J. Gao, Recent developments in nanofiltration membranes based on nanomaterials, Chin. J. Chem. Eng. 25(2017) 1639-1652.
[5] Z. Zhang, X. Shi, R. Wang, A. Xiao, Y. Wang, Ultra-permeable polyamide membranes harvested by covalent organic framework nanofiber scaffolds:a two-in-one strategy, Chem. Sci. 10(2019) 9077-9083.
[6] Z.A. Yi, F.D. Wu, Y. Zhou, C.J. Gao, Novel nanofiltration membranes with tunable permselectivity by polymer mediated phase separation in polyamide selective layer, Chin. J. Chem. Eng. 24(2016) 1533-1540.
[7] V. Freger, Nanoscale heterogeneity of polyamide membranes formed by interfacial polymerization, Langmuir 19(2003) 4791-4797.
[8] V. Freger, S. Srebnik, Mathematical model of charge and density distributions in interfacial polymerization of thin films, J. Appl. Polym. Sci. 88(2010) 1162-1169.
[9] H. Wu, H. Sun, W. Hong, L. Mao, Y. Liu, Improvement of polyamide thin film Nanocomposite membrane assisted by tannic acid-Fe(Ⅲ) functionalized multiwall carbon nanotubes, ACS Appl. Mater. Interf. 9(2017) 32255-32263.
[10] Y.S. Guo, Y.F. Mi, F.Y. Zhao, Y.L. Ji, Q.F. An, C.J. Gao, Zwitterions functionalized multiwalled carbon nanotubes/polyamide hybrid nanofiltration membranes for monovalent/divalent salts separation, Sep. Purif. Technol. 206(2018) 59-68.
[11] Z. Tan, S. Chen, X. Peng, L. Zhang, C. Gao, Polyamide membranes with nanoscale Turing structures for water purification, Science 360(2018) 518-521.
[12] L. Fan, Q. Zhang, Z. Yang, R. Zhang, Y.N. Liu, M. He, Z. Jiang, Y. Su, Improving permeation and antifouling performance of polyamide nanofiltration membranes through the incorporation of arginine, ACS Appl. Mater. interf. 9(2017) 13577-13586.
[13] Q. Wang, G.S. Zhang, Z.S. Li, S. Deng, H. Chen, P. Wang, Preparation and properties of polyamide/titania composite nanofiltration membrane by interfacial polymerization, Desalination 352(2014) 38-44.
[14] C. Van Goethem, R. Verbeke, S. Hermans, R. Bernstein, I.F.J. Vankelecom, Controlled positioning of MOFs in interfacially polymerized thin-film nanocomposites, J. Mater. Chem. A 4(2016) 16368-16376.
[15] K. Santanu, J. Zhiwei, A.G. Livingston, MEMBRANE FILTRATION, Sub-10 nm polyamide nanofilms with ultrafast solvent transport for molecular separation, Science 348(2015) 1347.
[16] R.P. Bisbey, W.R. Dichtel, Covalent organic frameworks as a platform for multidimensional polymerization, ACS Cent. Sci. 3(2017) 533-543.
[17] S.Y. Ding, W. Wang, Covalent organic frameworks (COFs):from design to applications, Chem. Soc. Rev. 42(2013) 548-568.
[18] H. Wang, Z. Zeng, P. Xu, L. Li, G. Zeng, R. Xiao, Z. Tang, D. Huang, L. Tang, C. Lai, D. Jiang, Y. Liu, H. Yi, L. Qin, S. Ye, X. Ren, W. Tang, Recent progress in covalent organic framework thin films:fabrications, applications and perspectives, Chem. Soc. Rev. 48(2019) 488-516.
[19] H. Fan, A. Mundstock, A. Feldhoff, A. Knebel, J. Gu, H. Meng, J. Caro, Covalent organic framework-covalent organic framework bilayer membranes for highly selective gas separation, J. Am. Chem. Soc. 140(2018) 10094-10098.
[20] Y. Ying, D. Liu, J. Ma, M. Tong, W. Zhang, H. Huang, Q. Yang, C. Zhong, A GO-assisted method for the preparation of ultrathin covalent organic framework membranes for gas separation, J. Mater. Chem. A 4(2016) 13444-13449.
[21] M. Wang, F. Pan, H. Yang, Y. Cao, H. Wang, Y. Song, Z. Lu, M. Sun, H. Wu, Z. Jiang, Constructing channel-mediated facilitated transport membranes by incorporating covalent organic framework nanosheets with tunable microenvironments, J. Mater. Chem. A 7(2019) 9912-9923.
[22] H. Yang, H. Wu, Z. Yao, B. Shi, Z. Xu, X. Cheng, F. Pan, G. Liu, Z. Jiang, X. Cao, Functionally graded membranes from nanoporous covalent organic frameworks for highly selective water permeation, J. Mater. Chem. A 6(2018) 583-591.
[23] H. Fan, J. Gu, H. Meng, A. Knebel, J. Caro, High-flux membranes based on the covalent organic framework COF-LZU1 for selective dye separation by nanofiltration, Angew. Chem. Int. Ed. Engl. 57(2018) 4083-4087.
[24] J. Yuan, M. Wu, H. Wu, Y. Liu, X. You, R. Zhang, Y. Su, H. Yang, J. Shen, Z. Jiang, Covalent organic framework-modulated interfacial polymerization for ultrathin desalination membranes, J. Mater. Chem. A 7(2019) 25641-25649.
[25] S. Kandambeth, A. Mallick, B. Lukose, M.V. Mane, T. Heine, R. Banerjee, Construction of crystalline 2D covalent organic frameworks with remarkable chemical (acid/base) stability via a combined reversible and irreversible route, J. Am. Chem. Soc. 134(2012) 19524-19527.
[26] J.-J. Wang, H.-C. Yang, M.-B. Wu, X. Zhang, Z.-K. Xu, Nanofiltration membranes with cellulose nanocrystals as an interlayer for unprecedented performance, J. Mater. Chem. A 5(2017) 16289-16295.
[27] F. Pan, W. Guo, Y. Su, N.A. Khan, H. Yang, Z. Jiang, Direct growth of covalent organic framework nanofiltration membranes on modified porous substrates for dyes separation, Sep. Purif. Technol. 215(2019) 582-589.
[28] C. Wang, Z. Li, J. Chen, Z. Li, Y. Yin, L. Cao, Y. Zhong, H. Wu, Covalent organic framework modified polyamide nanofiltration membrane with enhanced performance for desalination, J. Membr. Sci. 523(2017) 273-281.
[29] H. Yang, H. Wu, Z. Xu, B. Mu, Z. Lin, X. Cheng, G. Liu, F. Pan, X. Cao, Z. Jiang, Hierarchical pore architectures from 2D covalent organic nanosheets for efficient water/alcohol separation, J. Membr. Sci. 561(2018) 79-88.