Sol–gel transitions of comb-like polymethacrylate copolymers by mechano-thermal stimuli in water
Sonogelation by supramolecular gelators is highlighted as a paradigm shift for their potential applications in material and biomedical sciences. Yet, these materials require organic solvents and low-frequency ultrasound, limiting their utility. Here, a comb-like polymethacrylate copolymer is synthes...
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sg-ntu-dr.10356-1611362022-08-16T07:47:42Z Sol–gel transitions of comb-like polymethacrylate copolymers by mechano-thermal stimuli in water Jonnalagadda, Umesh Sai Nguyen, Tuan Minh Li, Feifei Lee, Jim H. C. Liu, Xu Goto, Atsushi Kwan, James J. School of Chemical and Biomedical Engineering School of Physical and Mathematical Sciences Institute of Chemical and Engineering Sciences, A*STAR Engineering::Chemical engineering Gelation Smart Polymers Sonogelation by supramolecular gelators is highlighted as a paradigm shift for their potential applications in material and biomedical sciences. Yet, these materials require organic solvents and low-frequency ultrasound, limiting their utility. Here, a comb-like polymethacrylate copolymer is synthesized with 2,6-bis(1-methylbenzimidazolyl)-4-oxypyridine tridentate ligand randomly distributed on poly(ethylene glycol) side chains. Upon addition of zinc perchlorate salt, this copolymer rapidly forms a hydrogel after exposure to either mechanical (i.e., ultrasound) or thermal stimuli. Spectroscopic analysis, to elucidate the mechanism, indicates metal ion coordination to ligand as well as the carbonyl and ethylene glycol units; interestingly, 1H-NMR suggests that the coordination between tridentate ligand moiety and Zn2+ is unexpectedly weaker in water than in acetonitrile. Investigations by dynamic light scattering indicates that the copolymer forms nanodispersions in excess salt, which coalesces to form a hydrogel by either heating or high intensity focused ultrasound (HIFU). Rheological quantification of these gels suggests stronger crosslinking by HIFU compared to heating. Agency for Science, Technology and Research (A*STAR) Nanyang Technological University National Medical Research Council (NMRC) Funding was provided by A*STAR, RIE2020-AME-IAF-PP (A1786a0029), and NTU Start-Up Grant (M4081814). This research was supported by the Singapore Ministry of Health's National Medical Research Council under its NMRC/OFYIRG/0034/2017. 2022-08-16T07:47:42Z 2022-08-16T07:47:42Z 2020 Journal Article Jonnalagadda, U. S., Nguyen, T. M., Li, F., Lee, J. H. C., Liu, X., Goto, A. & Kwan, J. J. (2020). Sol–gel transitions of comb-like polymethacrylate copolymers by mechano-thermal stimuli in water. Macromolecular Chemistry and Physics, 221(13), 2000088-. https://dx.doi.org/10.1002/macp.202000088 1022-1352 https://hdl.handle.net/10356/161136 10.1002/macp.202000088 2-s2.0-85086266960 13 221 2000088 en A1786a0029 M4081814 NMRC/OFYIRG/0034/2017 Macromolecular Chemistry and Physics © 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. All rights reserved. |
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Engineering::Chemical engineering Gelation Smart Polymers Jonnalagadda, Umesh Sai Nguyen, Tuan Minh Li, Feifei Lee, Jim H. C. Liu, Xu Goto, Atsushi Kwan, James J. Sol–gel transitions of comb-like polymethacrylate copolymers by mechano-thermal stimuli in water |
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Sonogelation by supramolecular gelators is highlighted as a paradigm shift for their potential applications in material and biomedical sciences. Yet, these materials require organic solvents and low-frequency ultrasound, limiting their utility. Here, a comb-like polymethacrylate copolymer is synthesized with 2,6-bis(1-methylbenzimidazolyl)-4-oxypyridine tridentate ligand randomly distributed on poly(ethylene glycol) side chains. Upon addition of zinc perchlorate salt, this copolymer rapidly forms a hydrogel after exposure to either mechanical (i.e., ultrasound) or thermal stimuli. Spectroscopic analysis, to elucidate the mechanism, indicates metal ion coordination to ligand as well as the carbonyl and ethylene glycol units; interestingly, 1H-NMR suggests that the coordination between tridentate ligand moiety and Zn2+ is unexpectedly weaker in water than in acetonitrile. Investigations by dynamic light scattering indicates that the copolymer forms nanodispersions in excess salt, which coalesces to form a hydrogel by either heating or high intensity focused ultrasound (HIFU). Rheological quantification of these gels suggests stronger crosslinking by HIFU compared to heating. |
author2 |
School of Chemical and Biomedical Engineering |
author_facet |
School of Chemical and Biomedical Engineering Jonnalagadda, Umesh Sai Nguyen, Tuan Minh Li, Feifei Lee, Jim H. C. Liu, Xu Goto, Atsushi Kwan, James J. |
format |
Article |
author |
Jonnalagadda, Umesh Sai Nguyen, Tuan Minh Li, Feifei Lee, Jim H. C. Liu, Xu Goto, Atsushi Kwan, James J. |
author_sort |
Jonnalagadda, Umesh Sai |
title |
Sol–gel transitions of comb-like polymethacrylate copolymers by mechano-thermal stimuli in water |
title_short |
Sol–gel transitions of comb-like polymethacrylate copolymers by mechano-thermal stimuli in water |
title_full |
Sol–gel transitions of comb-like polymethacrylate copolymers by mechano-thermal stimuli in water |
title_fullStr |
Sol–gel transitions of comb-like polymethacrylate copolymers by mechano-thermal stimuli in water |
title_full_unstemmed |
Sol–gel transitions of comb-like polymethacrylate copolymers by mechano-thermal stimuli in water |
title_sort |
sol–gel transitions of comb-like polymethacrylate copolymers by mechano-thermal stimuli in water |
publishDate |
2022 |
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https://hdl.handle.net/10356/161136 |
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1743119612164177920 |