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Cononsolvency

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Schematic representation of the cononsolvency effect of a polymer in mixed solution.

Cononsolvency is a phenomenon where two solvents that can typically readily dissolve a polymer, when mixed, at certain ratios of these two solvents, are no longer able to dissolve the polymer. This phenomenon is in contrast to cosolvency where two solvents that are both poor at dissolving a material, but when the two poor solvents admixed, can form a mixed solvent capable of dissolving the material.

The first works of both experimental and theoretical about the cononsolvency effect were published in the late 1970s.[1][2] Since then, numerous studies focused on a manifold of different polymers that featured the cononsolvency effect in water and various organic cosolvents such as methanol, ethanol, and acetone.[3][4][5] Typically poly(acrylamide)s such as poly(N-isopropylacrylamide) show the cononsolvency effect,[6][7][8] while this effect is also known for other homopolymers and for more complex systems e.g., diblock copolymer, polyelectrolytes,[9][10] crosslinked microgels,[11][12] micelles,[13] and grafted polymer brushes.[10] [14] Recently, it was also shown that thermo-responsive thin films exhibit the cononsolvency effect in a mixed solvent vapor phase,[15][16][17][18] which can be explained by a decreased volume phase transition temperature, the thin-film analogy of a lower critical solution temperature. These experimental studies are supported by a growing number of simulation studies.[19][20][21][22]

After 45 years of research, the origin of the molecular mechanism behind the cononsolvency effect in a mixture of solvents remains not fully resolved yet. To date, researchers have considered various interactions between polymer and solvent/cosolvent as possible factors leading to the cononsolvency effect, such as competitive hydrogen bonding of the solvent and cosolvent with the polymer,[20][23][24] hydrophobic hydration of particular functional groups of the polymer,[25] cosolvent induced geometric frustration,[26][27] excluded-volume interactions due to the surfactant-like behavior of amphiphilic cosolvents,[28][29] as well as the three body effects, i.e., temporary bridging of one or more individual polymer chains by the cosolvent.[30][31][32][33]

In literature, cononsolvency was reported almost exclusively for polymers in aqueous solution. This, however, does not mean that cononsolvency cannot happen in non-aqueous solutions. For example, poly(methyl methacrylate) shows the cononsolvency effect in the binary mixtures of two organic solvents (chlorobutane and amyl acetate[34]).

References

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  1. ^ Wolf, B. A.; Willms, M. M. (September 1978). "Measured and calculated solubility of polymers in mixed solvents: Co-nonsolvency". Die Makromolekulare Chemie. 179 (9): 2265–2277. doi:10.1002/macp.1978.021790914. ISSN 0025-116X.
  2. ^ De Gennes, P.G. (1976). "Conformation of a polymer chain in certain mixed solvents". Journal de Physique Lettres. 37 (4): 59–61. doi:10.1051/jphyslet:0197600370405900. ISSN 0302-072X.
  3. ^ Winnik, Francoise M.; Ringsdorf, H.; Venzmer, J. (1990-04-01). "Methanol-water as a co-nonsolvent system for poly(N-isopropylacrylamide)". Macromolecules. 23 (8): 2415–2416. Bibcode:1990MaMol..23.2415W. doi:10.1021/ma00210a048. ISSN 0024-9297.
  4. ^ Crowther, H. M.; Vincent, B. (1998-01-23). "Swelling behavior of poly- N -isopropylacrylamide microgel particles in alcoholic solutions". Colloid & Polymer Science. 276 (1): 46–51. doi:10.1007/s003960050207. ISSN 0303-402X. S2CID 93950244.
  5. ^ Costa, Ricardo O. R; Freitas, Roberto F. S (2002-01-01). "Phase behavior of poly(N-isopropylacrylamide) in binary aqueous solutions". Polymer. 43 (22): 5879–5885. doi:10.1016/S0032-3861(02)00507-4. ISSN 0032-3861.
  6. ^ Yamauchi, Hideo; Maeda, Yasushi (2007-11-01). "LCST and UCST Behavior of Poly(N-isopropylacrylamide) in DMSO/Water Mixed Solvents Studied by IR and Micro-Raman Spectroscopy". The Journal of Physical Chemistry B. 111 (45): 12964–12968. doi:10.1021/jp072438s. ISSN 1520-6106. PMID 17949072.
  7. ^ Zhu, Peng Wei; Napper, Donald H. (1996-06-21). "Volume phase transitions of poly(N-isopropylacrylamide) latex particles in mixed water-N,N-dimethylformamide solutions". Chemical Physics Letters. 256 (1): 51–56. Bibcode:1996CPL...256...51Z. doi:10.1016/0009-2614(96)00420-4. ISSN 0009-2614.
  8. ^ Dalkas, Georgios; Pagonis, Konstantinos; Bokias, Georgios (2006-01-03). "Control of the lower critical solution temperature—type cononsolvency properties of poly(N-isopropylacrylamide) in water—dioxane mixtures through copolymerisation with acrylamide". Polymer. 47 (1): 243–248. doi:10.1016/j.polymer.2005.10.115. ISSN 0032-3861.
  9. ^ Chen, Zhiyun; Yu, Sihan; Liu, Doudou; Shi, Shaoxiong; Shen, Weiguo (2018-09-01). "Solvation Behaviors of Poly(acrylic acid) in Mixed Solvents of 2-Butoxyethanol + Water". Journal of Solution Chemistry. 47 (9): 1539–1552. doi:10.1007/s10953-018-0809-x. ISSN 1572-8927. S2CID 106294052.
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  12. ^ Maccarrone, Simona; Scherzinger, Christine; Holderer, Olaf; Lindner, Peter; Sharp, Melissa; Richtering, Walter; Richter, Dieter (2014-09-09). "Cononsolvency Effects on the Structure and Dynamics of Microgels". Macromolecules. 47 (17): 5982–5988. Bibcode:2014MaMol..47.5982M. doi:10.1021/ma500954t. ISSN 0024-9297.
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  15. ^ Kreuzer, Lucas P.; Lindenmeir, Christoph; Geiger, Christina; Widmann, Tobias; Hildebrand, Viet; Laschewsky, André; Papadakis, Christine M.; Müller-Buschbaum, Peter (2021-02-09). "Poly(sulfobetaine) versus Poly(N-isopropylmethacrylamide): Co-Nonsolvency-Type Behavior of Thin Films in a Water/Methanol Atmosphere". Macromolecules. 54 (3): 1548–1556. Bibcode:2021MaMol..54.1548K. doi:10.1021/acs.macromol.0c02281. ISSN 0024-9297. S2CID 234184714.
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  24. ^ Backes, Sebastian; Krause, Patrick; Tabaka, Weronika; Witt, Marcus U.; Mukherji, Debashish; Kremer, Kurt; von Klitzing, Regine (2017-10-17). "Poly(N-isopropylacrylamide) Microgels under Alcoholic Intoxication: When a LCST Polymer Shows Swelling with Increasing Temperature". ACS Macro Letters. 6 (10): 1042–1046. doi:10.1021/acsmacrolett.7b00557. PMID 35650939.
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  27. ^ Tavagnacco, Letizia; Zaccarelli, Emanuela; Chiessi, Ester (2020-01-01). "Molecular description of the coil-to-globule transition of Poly(N-isopropylacrylamide) in water/ethanol mixture at low alcohol concentration". Journal of Molecular Liquids. 297: 111928. arXiv:1910.09352. doi:10.1016/j.molliq.2019.111928. ISSN 0167-7322. S2CID 204800909.
  28. ^ Bharadwaj, Swaminath; Nayar, Divya; Dalgicdir, Cahit; van der Vegt, Nico F. A. (2020-11-11). "A cosolvent surfactant mechanism affects polymer collapse in miscible good solvents". Communications Chemistry. 3 (1): 165. doi:10.1038/s42004-020-00405-x. ISSN 2399-3669. PMC 9814688. PMID 36703319.
  29. ^ Bharadwaj, Swaminath; Nayar, Divya; Dalgicdir, Cahit; van der Vegt, Nico F. A. (2021-04-07). "An interplay of excluded-volume and polymer–(co)solvent attractive interactions regulates polymer collapse in mixed solvents". The Journal of Chemical Physics. 154 (13): 134903. doi:10.1063/5.0046746. ISSN 0021-9606. PMID 33832270.
  30. ^ Sommer, Jens-Uwe (2017-03-14). "Adsorption–Attraction Model for Co-Nonsolvency in Polymer Brushes". Macromolecules. 50 (5): 2219–2228. doi:10.1021/acs.macromol.6b02231. ISSN 0024-9297.
  31. ^ Mukherji, Debashish; Marques, Carlos M.; Kremer, Kurt (2014-09-12). "Polymer collapse in miscible good solvents is a generic phenomenon driven by preferential adsorption". Nature Communications. 5 (1): 4882. Bibcode:2014NatCo...5.4882M. doi:10.1038/ncomms5882. ISSN 2041-1723. PMC 4175582. PMID 25216245.
  32. ^ Zhu, Peng-wei; Chen, Luguang (2019-02-11). "Effects of cosolvent partitioning on conformational transitions and chain flexibility of thermoresponsive microgels". Physical Review E. 99 (2): 022501. Bibcode:2019PhRvE..99b2501Z. doi:10.1103/PhysRevE.99.022501. PMID 30934277. S2CID 91187258.
  33. ^ Yong, Huaisong; Sommer, Jens-Uwe (2022-12-27). "Cononsolvency Effect: When the Hydrogen Bonding between a Polymer and a Cosolvent Matters". Macromolecules. 55 (24): 11034–11050. doi:10.1021/acs.macromol.2c01428. ISSN 0024-9297. S2CID 254329617.
  34. ^ Fernández-Piérola, Inés; Horta, Arturo (1980-10-01). "Co-nonsolvency of PMMA". Polymer Bulletin. 3 (5): 273–278. doi:10.1007/BF00254873. ISSN 1436-2449. S2CID 98808729.
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