Abstract
Copolymer hydrogels formed from cationic and aromatic monomers with identical monomer compositions but different average sequences were synthesized by free-radical copolymerization in various solvents. We found that hydrogels with one-component-rich segments are mechanically stronger than those with adjacent-rich monomer sequences in water, while hydrogels with a rich cation-π adjacent sequence showed excellent mechanical strength and underwater adhesion in saltwater (0.7 M NaCl). The molecular mechanisms for these behaviors are discussed in terms of polymer structures. This work reveals the importance of monomeric sequences in determining hydrogel properties and provides a facile approach to develop hydrogels with different properties but the same monomer composition.
Similar content being viewed by others
References
Webber MJ, Appel EA, Meijer EW, Langer R. Nat Mater, 2016, 15: 13–26
Fan H, Gong JP. Macromolecules, 2020, 53: 2769–2782
Lutz JF, Ouchi M, Liu DR, Sawamoto M. Science, 2013, 341: 1238149
Lutz JF, Lehn JM, Meijer EW, Matyjaszewski K. Nat Rev Mater, 2016, 1: 16024
Martens S, Holloway JO, Du Prez FE. Macromol Rapid Commun, 2017, 38: 1700469
Ouchi M, Sawamoto M. Polym J, 2017, 50: 83–94
Pasini D, Takeuchi D. Chem Rev, 2018, 118: 8983–9057
Meier MAR, Barner-Kowollik C. Adv Mater, 2019, 31: 1806027
Solleder SC, Schneider RV, Wetzel KS, Boukis AC, Meier MAR. Macromol Rapid Commun, 2017, 38: 1600711
Ida S, Kawahara T, Kawabata H, Ishikawa T, Hirokawa Y. Gels, 2018, 4: 22
Kimura M, Fukumoto K, Watanabe J, Takai M, Ishihara K. Biomaterials, 2005, 26: 6853–6862
Odian G. Principles of Polymerization. 4th Ed. Hoboken: Wiley-Interscience, 2004
Gao H, Miasnikova A, Matyjaszewski K. Macromolecules, 2008, 41: 7843–7849
Lindemann B, Schröder UP, Oppermann W. Macromolecules, 1997, 30: 4073–4077
Fan H, Wang J, Tao Z, Huang J, Rao P, Kurokawa T, Gong JP. Nat Commun, 2019, 10: 5127
Mayo FR, Lewis FM. J Am Chem Soc, 1944, 66: 1594–1601
Matsukata M, Hirata M, Gong JP, Osada Y, Sakurai Y, Okano T. Colloid Polym Sci, 1998, 276: 11–18
Thévenot C, Khoukh A, Reynaud SP, DesbrièRes J, Grassl B. Soft Matter, 2007, 3: 437–447
Mortimer R. Physical Chemistry. 3rd Ed. New York: Academic Press, 2008
Fan H, Guo H, Wang J, Gong JP. Giant, 2020, 1: 100005
Chen L, Sun TL, Cui K, King DR, Kurokawa T, Saruwatari Y, Gong JP. J Mater Chem A, 2019, 7: 17334–17344
Fan H, Wang J, Gong JP. Adv Funct Mater, 2021, 31: 2009334
Acknowledgements
This work was supported by JSPS KAKENHI Grant (JP17H06144, JP17H06376, JP21K14676), and Institute for Chemical Reaction Design and Discovery (WPI-ICReDD) established by World Premier International Research Initiative (WPI), MEXT, Japan. The authors thank Mr. Yoshiyuki Saruwatari at Osaka Organic Chemistry Co., Ltd., Japan for providing monomers.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest The authors declare no conflict of interest.
Electronic supplementary material
Rights and permissions
About this article
Cite this article
Fan, H., Cai, Y. & Gong, J.P. Facile tuning of hydrogel properties by manipulating cationic-aromatic monomer sequences. Sci. China Chem. 64, 1560–1568 (2021). https://doi.org/10.1007/s11426-021-1010-3
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11426-021-1010-3