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Swelling and Inflation in Polyelectrolyte Complexes

Cite this: Macromolecules 2019, 52, 2, 610–619
Publication Date (Web):December 31, 2018
https://doi.org/10.1021/acs.macromol.8b01838
Copyright © 2018 American Chemical Society
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Abstract

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The properties of polyelectrolyte complexes, PECs, made from blended polycations, Pol+, and polyanions, Pol–, are routinely studied under conditions where they are at least partially swollen with water. Water plasticizes PECs, transforming them from an intractable, glassy, and brittle state when dry to tough and viscoelastic when wet. In the present work the supreme efficiency of water, compared to other solvents on a polarity scale, in swelling a PEC is illustrated. Using a PEC of poly(diallyldimethylammonium) and poly(styrenesulfonate) with precisely determined density, we show that swelling tracks a Dimroth–Reichardt polarity scale until the molecular volume exceeds ∼50 Å3, whereupon the degree of swelling drops sharply. Long-term (>1 year) swelling of this PEC in pure water reveals an instability, wherein the material substantially inflates, generating large pores even though T < Tg. The mechanism for this instability is attributed to a small population of counterions, resulting from slight nonstoichiometry of polyelectrolytes, as well as the polymers themselves, a contribution estimated using Des Cloizeaux’s theory of osmotic pressure for overlapping chains. Low concentrations of salt in the bathing solution are enough to overcome the osmotic pressure within the PEC, and it remains dimensionally stable over the long time periods studied. The universal practice of rinsing PECs, whether they are in macroscopic or thin-film morphology, in pure water should be re-evaluated.

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  5. Belda Amelia Junisu, Iris Ching-Ya Chang, Ya-Sen Sun. Film Instability Induced by Swelling and Drying. Langmuir 2022, 38 (43) , 13009-13020. https://doi.org/10.1021/acs.langmuir.2c01173
  6. Mo Yang, Swapnil L. Sonawane, Zachary A. Digby, Jin G. Park, Joseph B. Schlenoff. Influence of “Hydrophobicity” on the Composition and Dynamics of Polyelectrolyte Complex Coacervates. Macromolecules 2022, 55 (17) , 7594-7604. https://doi.org/10.1021/acs.macromol.2c00267
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  8. Samir Abou Shaheen, Rachel L. Abbett, Khalil Akkaoui, Joseph B. Schlenoff. Long-Range Electron Transfer through Ultrathin Polyelectrolyte Complex Films: A Hopping Model. The Journal of Physical Chemistry C 2021, 125 (41) , 22797-22808. https://doi.org/10.1021/acs.jpcc.1c06040
  9. YuLing Chen, Kenneth R. Shull. Processing Polyelectrolyte Complexes with Deep Eutectic Solvents. ACS Macro Letters 2021, 10 (10) , 1243-1247. https://doi.org/10.1021/acsmacrolett.1c00494
  10. Yuhui Chen, Mo Yang, Samir Abou Shaheen, Joseph B. Schlenoff. Influence of Nonstoichiometry on the Viscoelastic Properties of a Polyelectrolyte Complex. Macromolecules 2021, 54 (17) , 7890-7899. https://doi.org/10.1021/acs.macromol.1c01154
  11. Elif Nur Durmaz, Sevil Sahin, Ettore Virga, Sissi de Beer, Louis C. P. M. de Smet, Wiebe M. de Vos. Polyelectrolytes as Building Blocks for Next-Generation Membranes with Advanced Functionalities. ACS Applied Polymer Materials 2021, 3 (9) , 4347-4374. https://doi.org/10.1021/acsapm.1c00654
  12. Yuhui Chen, Mo Yang, Joseph B. Schlenoff. Glass Transitions in Hydrated Polyelectrolyte Complexes. Macromolecules 2021, 54 (8) , 3822-3831. https://doi.org/10.1021/acs.macromol.0c02682
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  14. Lu Li, Artem M. Rumyantsev, Samanvaya Srivastava, Siqi Meng, Juan J. de Pablo, Matthew V. Tirrell. Effect of Solvent Quality on the Phase Behavior of Polyelectrolyte Complexes. Macromolecules 2021, 54 (1) , 105-114. https://doi.org/10.1021/acs.macromol.0c01000
  15. Sabrina S. Alam, Youngwoo Seo, Yakov Lapitsky. Highly Sustained Release of Bactericides from Complex Coacervates. ACS Applied Bio Materials 2020, 3 (12) , 8427-8437. https://doi.org/10.1021/acsabm.0c00763
  16. Scott P. O. Danielsen, Sergey Panyukov, Michael Rubinstein. Ion Pairing and the Structure of Gel Coacervates. Macromolecules 2020, 53 (21) , 9420-9442. https://doi.org/10.1021/acs.macromol.0c01360
  17. Mohsen Ghasemi, Sean Friedowitz, Ronald G. Larson. Analysis of Partitioning of Salt through Doping of Polyelectrolyte Complex Coacervates. Macromolecules 2020, 53 (16) , 6928-6945. https://doi.org/10.1021/acs.macromol.0c00797
  18. Samir Abou Shaheen, Mo Yang, Banghao Chen, Joseph B. Schlenoff. Water and Ion Transport through the Glass Transition in Polyelectrolyte Complexes. Chemistry of Materials 2020, 32 (14) , 5994-6002. https://doi.org/10.1021/acs.chemmater.0c01217
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  30. Jiarui Chen, Shanshan Xu, Chuyang Y. Tang, Binjie Hu, Begum Tokay, Tao He. Stability of layer-by-layer nanofiltration membranes in highly saline streams. Desalination 2023, 555 , 116520. https://doi.org/10.1016/j.desal.2023.116520
  31. Thomas J. Kolibaba, Callie I. Higgins, Nathan C. Crawford, Joseph R. Samaniuk, Jason P. Killgore. Sustainable Additive Manufacturing of Polyelectrolyte Photopolymer Complexes. Advanced Materials Technologies 2023, 8 (9) https://doi.org/10.1002/admt.202201681
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  35. Rafael F.N. Quadrado, André R. Fajardo. Vapor-induced polyelectrolyte complexation of chitosan/pectin: A promising strategy for the preparation of hydrogels for controlled drug delivery. Journal of Molecular Liquids 2022, 361 , 119604. https://doi.org/10.1016/j.molliq.2022.119604
  36. Chenjun Dong, Rongrong He, Shanshan Xu, Hailong He, Hao Chen, Yue-Biao Zhang, Tao He. Layer-by-layer (LBL) hollow fiber nanofiltration membranes for seawater treatment: Ion rejection. Desalination 2022, 534 , 115793. https://doi.org/10.1016/j.desal.2022.115793
  37. Jun Gao, Qiang‐wei Zhan, Ziyao Tang, Yan Huang. The Critical Transition from Soluble Complexes to Colloidal Aggregates of Polyelectrolyte Complexes at Non‐Stoichiometric Charge Ratios. Macromolecular Rapid Communications 2022, 43 (7) , 2100880. https://doi.org/10.1002/marc.202100880
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  40. Dezhong Liu, Liping Zhu, Wentao Huang, Shuguang Yang. Humidity induced relaxation transition of hydrogen-bonded complex fibers. Polymer 2021, 225 , 123794. https://doi.org/10.1016/j.polymer.2021.123794
  41. Artem M. Rumyantsev, Nicholas E. Jackson, Juan J. de Pablo. Polyelectrolyte Complex Coacervates: Recent Developments and New Frontiers. Annual Review of Condensed Matter Physics 2021, 12 (1) , 155-176. https://doi.org/10.1146/annurev-conmatphys-042020-113457
  42. Frances J. Morin, Marissa L. Puppo, Jennifer E. Laaser. Decoupling salt- and polymer-dependent dynamics in polyelectrolyte complex coacervates via salt addition. Soft Matter 2021, 17 (5) , 1223-1231. https://doi.org/10.1039/D0SM01412E
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