Dissipative Particle Dynamics Simulation of the Effect of Polymer Chain Rigidity on Membranes Formation by Nonsolvent Induced Phase Separation Process

doi:10.7503/cjcu20220169

Abstract

Abstract:

In this work， a new harmonic force field that was consistent with polyethersulfone（PES） structure was constructed by a mapping between the molecular dynamics（MD） simulation and the dissipative particle dynamics（DPD）， and the effect of polymer chain rigidity on the formation of PES membranes via the nonsolvent induced phase separation（NIPS） process with N-methyl-2-pyrrolidone（NMP） as the solvent and H₂O as the nonsolvent coagulant was investigated. The results showed that the rapid exchange of the solvent and nonsolvent at the interface between NMP/PES solution and H₂O caused the accumulation of PES at the interface， resulting in the formation of a thin but dense polymer layer near the interface. And in the interior region of the PES solution， the addition of the nonsolvent induced a spinodal decomposition of the PES solution， thus presenting asymmetric morphologies with a dense layer on the top surface and a porous sub-layer beneath the top surface. Also， the enhancement of PES chain rigidity can significantly improve the phase separation speed of the system and lead to the formation of the surface layer with a smaller pore size more quickly. Moreover， the effect of PES chain rigidity on membrane structure is obviously on the surface layer rather than the sub-layer. In addition， by comparing the influence of polymer concentration on the NIPS process in different force fields， it can be found that the enhancement of PES chain rigidity with different PES concentrations did not cause fundamental changes in the characteristics and evolution trend of the phase separation process. And the effect of the harmonic force field and classical spring force field on the NIPS process is similar. The simulation results reveal that the harmonic force field constructed in this study can obviously improve the rigidity of the PES chain， and thus can be helpful to simulate the membrane formation process of phase separation more realistically.

Key words: Dissipative particle dynamics, Non-solvent induced phase separation, Porous membrane, Polymer chain rigidity, Polyethersulfone

CLC Number:

O631.4

TrendMD:

TANG Yuanhui, LI Chunyu, LIN Yakai, ZHANG Chunhui, LIU Ze, YU Lixin, WANG Haihui, WANG Xiaolin. Dissipative Particle Dynamics Simulation of the Effect of Polymer Chain Rigidity on Membranes Formation by Nonsolvent Induced Phase Separation Process[J]. Chem. J. Chinese Universities, 2022, 43(10): 20220169.

Figures/Tables 19

Table 1 Mean and variance of bond lengths and angles in MD and DPD simulation

Method	Bond length		Bond angle
Method	Mean value/nm	Variance	Mean value/（°）	Variance
MD	0.945	1.35	116.28	53.59
DPD	0.939	3.43	116.69	59.23

Table 2 Molecular volume, molar mass, and the number of species per particle for PES, NMP and water

Species	Molecular volume/nm³	Molar mass	Number/ particle
PES repeat unit（P）	0.2	232.26	1
NMP molecule（S）	0.1	99.13	2
Water molecule（C）	0.02	18.02	10

Table 3 Flory-Huggins interaction parameter χij and the corresponding DPD repulsion parameter aij between different species

Species	PES?H₂O	PES?NMP	NMP?H₂O
$χ i j$	2.18	0.16	0.27
$α i j$	32.62	25.56	25.94

Table 3 Flory-Huggins interaction parameter χij and the corresponding DPD repulsion parameter aij between different species

Species	PES?H₂O	PES?NMP	NMP?H₂O
$χ i j$	2.18	0.16	0.27
$α i j$	32.62	25.56	25.94

References 38

1	Nunes S. P.， Culfaz⁃Emecen P. Z.， Ramon G. Z.， Visser T.， Koops G. H.， Jin W.， Ulbricht M.， J. Membr. Sci.， 2020， 598， 117761
2	Kausar A.， Polym. Plast. Technol. Eng.， 2017， 56（13）， 1421—1437
3	Wang D. M.， Lai J. Y.， Curr. Opin. Chem. Eng.， 2013， 2（2）， 229—237
4	Tang Y. H.， Lin Y. K.， Ford D. M.， Qian X.， Cervellere M. R.， Millett P. C.， Wang X.， J. Membr. Sci.， 2021， 640， 119810
5	Groot R. D.， Warren P. B.， J. Chem. Phys.， 1997， 107（3）， 4423
6	Bai J. L.， Liu D.， Wang R.， Chinese J. Polym. Sci.， 2021， 39（9）， 1217—1224
7	Ruiz⁃Morales Y.， Alvarez⁃Ramirez F.， Energy Fuels， 2021， 35（11）， 9294—9311
8	Sofos F.， Chatzoglou E.， Liakopoulos A.， Comput. Part. Mech.， 2021， 1—15
9	Wang X. L.， Qian H. J.， Chen L. J.， Lu Z. Y.， Li Z. S.， J. Membr. Sci.， 2008， 311（1/2）， 251—258
10	Lin H. H.， Tang Y. H.， Matsuyama H.， Wang X. L.， J. Membr. Sci.， 2018， 548， 288—297
11	Tang Y. H.， Ledieu E.， Cervellere M. R.， Millett P. C.， Ford D. M.， Qian X.， J. Membr. Sci.， 2020， 599， 117826
12	Wang Z. G.， J. Chem. Phys.， 2002， 117（1）， 481—500
13	van der Haven D. L. H.， Kohler S.， Schreiner E.， In 't Veld P. J.， J. Phys. Chem. B， 2021， 125（27）， 7485—7498
14	Wang J. M.， Wolf R. M.， Caldwell J. W.， Kollman P. A.， Case D. A.， J. Comput. Chem.， 2004， 25（9）， 1157—1174
15	Cornell W. D.， Cieplak P.， Bayly C. I.， Gould I. R.， Merz K. M.， Ferguson D. M.， Spellmeyer D. C.， Fox T.， Caldwell J. W.， Kollman P. A.， J. Am. Chem. Soc.， 1995， 117（19）， 5179—5197
16	Vanommeslaeghe K.， Hatcher E.， Acharya C.， Kundu S.， Zhong S.， Shim J.， Darian E.， Guvench O.， Lopes P.， Vorobyov I.， Mackerell A. D. Jr.， J. Comput. Chem.， 2010， 31（4）， 671—690
17	Frisch M. J.， Trucks G. W.， Schlegel H. B.， Scuseria G. E.， Robb M. A.， Cheeseman J. R.， Scalmani G.， Barone V.， Mennucci B.， Petersson G. A.， Nakatsuji H.， Caricato M.， Li X.， Hratchian H. P.， Izmaylov A. F.， Bloino J.， Zheng G.， Sonnenberg J. L.， Hada M.， Ehara M.， Toyota K.， Fukuda R.， Hasegawa J.， Ishida M.， Nakajima T.， Honda Y.， Kitao O.， Nakai H.， Vreven T.， Montgomery J. A.， Jr.， Peralta J. E.， Ogliaro F.， Bearpark M.， Heyd J. J.， Brothers E.， Kudin K. N.， Staroverov V. N.， Kobayashi R.， Normand J.， Raghavachari K.， Rendell A.， Burant J. C.， Iyengar S. S.， Tomasi J.， Cossi M.， Rega N.， Millam J. M.， Klene M.， Knox J. E.， Cross J. B.， Bakken V.， Adamo C.， Jaramillo J.， Gomperts R.， Stratmann R. E.， Yazyev O.， Austin A. J.， Cammi R.， Pomelli C.， Ochterski J. W.， Martin R. L.， Morokuma K.， Zakrzewski V. G.， Voth G. A.， Salvador P.， Dannenberg J. J.， Dapprich S.， Daniels A. D.， Farkas O.， Foresman J. B.， Ortiz J. V.， Cioslowski J.， Fox D. J.， Gaussian 09， Revision B.01， Gaussian Inc.， Wallingford CT， 2010
18	Case D. A.， Betz R. M.， Cerutti D. S.， Cheatham T. E. Ⅲ， Darden T. A.， Duke R. E.， Giese T. J.， Gohlke H.， Goetz A. W.， Homeyer N.， Izadi S.， Janowski P.， Kaus J.， Kovalenko A.， Lee T. S.， LeGrand S.， Li P.， Lin C.， Luchko T.， Luo R.， Madej B.， Mermelstein D.， Merz K. M.， Monard G.， Nguyen H.， Nguyen H. T.， Omelyan I.， Onufriev A.， Roe D. R.， Roitberg A.， Sagui C.， Simmerling C. L.， Botello⁃Smith W. M.， Swails J.， Walker R. C.， Wang J.， Wolf R. M.， Wu X.， Xiao L.， Kollman P. A.， AMBER 2016， University of California， San Francisco， 2016
19	Salomon‐Ferrer R.， Götz A.， Poole D.， Le Grand S.， Walker R.， J. Chem. Theory. Comput.， 2013， 9， 3878—3888
20	Gotz A. W.， Williamson M. J.， Xu D.， Poole D.， Le Grand S.， Walker R. C.， J. Chem. Theory. Comput.， 2012， 8（5）， 1542—1555
21	Le Grand S.， Comput. Phys. Commun.， 2013， 184， 374—380
22	Wiebe H.， Louwersheimer J.， Weinberg N.， Mol. Phys.， 2015， 113（21）， 3176—3181
23	Luchko T.， Gusarov S.， Roe D. R.， Simmerling C.， Case D. A.， Tuszynski J.， Kovalenko A.， J. Chem. Theory. Comput.， 2010， 6（3）， 607—624
24	Español P.， Warren P.， EPL， 1995， 30（4）， 191—196
25	Chen L. J.， Qian H. J.， Lu Z. Y.， Li Z. S.， Sun C. C.， J. Phys. Chem. B， 2006， 110（47）， 24093—24100
26	Ortiz V.， Nielsen S. O.， Discher D. E.， Klein M. L.， Lipowsky R.， Shillcock J.， J. Phys. Chem. B， 2005， 109（37）， 17708—17714
27	Martinez L.， Andrade R.， Birgin E. G.， Martinez J. M.， J. Comput. Chem.， 2009， 30（13）， 2157—2164
28	Zhu Y. L.， Liu H.， Li Z. W.， Qian H. J.， Milano G.， Lu Z. Y.， J. Comput. Chem.， 2013， 34（25）， 2197—2211
29	Laradji M.， Mouritsen O. G.， Toxvaerd S.， Zuckermann M. J.， Phys. Rev. E， 1994， 50（2）， 1243—1252
30	Willems T. F.， Rycroft C. H.， Kazi M.， Meza J. C.， Haranczyk M.， Micropor. Mesopor. Mat.， 2012， 149（1）， 134—141
31	Xiao L. Y.， Ji D. H.， Phys. Bull.， 2017，（9）， 89—93
	肖立勇，纪登辉. 物理通报， 2017，（9）， 89—93
32	Guillen G. R.， Pan Y.， Li M， Hoek E. M. V.， Ind. Eng. Chem. Res.， 2011， 50（7）， 3798—3817
33	Hwang J. R.， Koo S. H.， Kim J. H.， Higuchi A.， Tak T. M.， J. Appl. Polym. Sci.， 1996， 60（9）， 1343—1348
34	Mosqueda⁃Jimenez D. B.， Narbaitz R. M.， Matsuura T.， Chowdhury G.， Pleizier G.， Santerre J. P.， J. Membr. Sci.， 2004， 231（1/2）， 209—224
35	Miyano T.， Matsuura T.， Sourirajan S.， Chem. Eng. Commun.， 2010， 95（1）， 11—26
36	King J. S.， Boyer W.， Wignall G. D.， Ullman R.， Macromol.， 1985， 18（4）， 709—718
37	Kaznessis Y. N.， Hill D. A.， Maginn E. J.， J. Chem. Phys.， 1998， 109（12）， 5078—5088
38	Barzin J.， Sadatnia B.， Polym.， 2007， 48（6）， 1620—1631

[1]	ZHENG Qiuguang,LIU Hailiang,XIAO Changfa. Preparation and Performance of Poly(vinylidene chloride-co-vinyl chloride) Porous Membranes via Thermally Induced Phase Separation^† [J]. Chem. J. Chinese Universities, 2019, 40(4): 841.
[2]	LIANG Xu, QIN Lijuan, ZHANG Yatao, LIU Jindun. Preparation and Properties of Poly-2-methacryloyloxyethyl Phosphorylcholine Grafted Silica/Polyethersulfone Composite Membrane^† [J]. Chem. J. Chinese Universities, 2018, 39(3): 598.
[3]	RONG Jingjing,MA Lan,ZHU Youliang,HUANG Yineng,SUN Zhaoyan. Simulation of Perforated Lamelar Structures of Diblock Copolymer Induced by Surface Patterns^† [J]. Chem. J. Chinese Universities, 2018, 39(12): 2805.
[4]	WANG Li, WANG Chu, ZHOU Jian. Dissipative Particle Dynamics Simulations on the pH-responsive Gating of Block Copolymer Brush Modified Nanopores^† [J]. Chem. J. Chinese Universities, 2018, 39(1): 85.
[5]	SONG Qingsong, ZHANG Jingnan, LIU Yong. Mesoscale Simulation of a Melt Electrospinning Jet in a Periodically Changing Electric Field [J]. Chem. J. Chinese Universities, 2017, 38(6): 966.
[6]	WANG Wei, XU Jiali, LIN Yuanfei, LI Xueyu, MENG Lingpu, LI Liangbin. Effect of Hot Stretching on the Structure of Polypropylene Microporous Membranes with in situ Small Angle X-Ray Scattering^† [J]. Chem. J. Chinese Universities, 2017, 38(11): 2128.
[7]	LIU Xuewu,CHEN Shuhua,ZHAN Shiping. Experimental Study and Theoretical Phase Diagram Calculation for Polystyrene Membranes Prepared by Supercritical CO₂-induced Phase Inversion^† [J]. Chem. J. Chinese Universities, 2016, 37(8): 1573.
[8]	XU Fanhua, HENG Xiao, REN Jianxue, ZHOU Hengwei. Simulation Study of the Phase Separation and Self-assembly of Nanoparticles Coated with Ligands^† [J]. Chem. J. Chinese Universities, 2016, 37(6): 1115.
[9]	XIA Qingcheng, MAO Fei, YANG Yong, HAN Jing, LIU Xiaohui, YANG Jiazhi, SUN Dongping. Properties of CeO₂/PTFE/Nafion Composite Membranes Prepared by Magnetron Sputtering^† [J]. Chem. J. Chinese Universities, 2016, 37(11): 2108.
[10]	LIU Linlin, YANG Zhongzhi. Self-assembly Morphological Control of Block Copolymers Simulated via the Combination of Dissipative Particle Dynamics and ABEEM Polarizable Force Field^† [J]. Chem. J. Chinese Universities, 2015, 36(11): 2179.
[11]	YU Liang, ZHANG Yatao, LIU Jindun. Preparation and Characterization of Modified Graphene Oxide/Polyethersulfone Positively Charged Hybrid Nanofiltration Membrane^† [J]. Chem. J. Chinese Universities, 2014, 35(5): 1100.
[12]	LIU Xiaohan, GUO Hongxia. Dissipative Particle Dynamics Simulation of the Phase Behavior of T-shaped Ternary Amphiphiles Possessing Long Rod-like Mesogens^† [J]. Chem. J. Chinese Universities, 2014, 35(2): 440.
[13]	XIE Yu, LÜ Zhong-Yuan, SUN Zhao-Yan, AN Li-Jia. Dissipative Particle Dynamics Simulation Study on the Micellization and Gelation Behavior of PEO-PPO-PEO Solution [J]. Chem. J. Chinese Universities, 2013, 34(6): 1454.
[14]	XUE Yao-Hong, ZHAO Yi-Wu, FAN Jing-Tao, HAN Cheng, JIANG Zhen-Gang, YANG Hua-Min, LIU Hong. Computer Simulation of Phase Separation in Binary Polymer Brush Systems [J]. Chem. J. Chinese Universities, 2013, 34(1): 242.
[15]	ZHOU Bo, LIN Ya-Kai, MA Wen-Zhong, TANG Yuan-Hui, TIAN Ye, WANG Xiao-Lin. Preparation of Ethylene Chlorotrifluoroethylene Co-polymer Membranes via Thermally Induced Phase Separation [J]. Chem. J. Chinese Universities, 2012, 33(11): 2585.