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Strong and Tough Polyion-Complex Hydrogels from Oppositely Charged Polyelectrolytes: A Comparative Study with Polyampholyte Hydrogels

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Title: Strong and Tough Polyion-Complex Hydrogels from Oppositely Charged Polyelectrolytes: A Comparative Study with Polyampholyte Hydrogels
Authors: Luo, Feng Browse this author
Sun, Tao Lin Browse this author
Nakajima, Tasuku Browse this author
King, Daniel R. Browse this author
Kurokawa, Takayuki Browse this author
Zhao, Yu Browse this author
Ihsan, Abu Bin Browse this author
Li, Xufeng Browse this author
Guo, Honglei Browse this author
Gong, Jian Ping Browse this author →KAKEN DB
Issue Date: 12-Apr-2016
Publisher: American Chemical Society
Journal Title: Macromolecules
Volume: 49
Issue: 7
Start Page: 2750
End Page: 2760
Publisher DOI: 10.1021/acs.macromol.6b00235
Abstract: Oppositely charged homopolyelectrolytes were found to form strong, tough, and self-healing polyion-complex (PIC) hydrogels, similar to polyampholytes (PA) which have opposite charges randomly distributed on the same polymer chains. The excellent mechanical performances of these two novel hydrogels are the results of dynamic ionic bonds formation between entangled polymer chains. For the PIC system, only interchain bonding occurs, while for the PA system both inter- and intrachain bonding exist. In addition, the ion pairs are expected to form stronger bonding in the PIC system than those in the PA system. In this work, we performed a comparative study of PIC hydrogels with the PA hydrogels. The PIC hydrogels are synthesized by sequential homopolymerization of cationic and anionic monomers at varied formulation, and their swelling and mechanical properties are systematically studied in comparison to the PA hydrogels that were synthesized from random copolymerization of anionic monomers and cationic monomers of the similar formulation. Different from the PA system which only forms tough hydrogels around zero net charge composition without chemical cross-linking, the PIC system forms tough physical hydrogels even at weakly offbalanced charge composition. At the charge-balanced composition, the low entanglement concentration of homocharged polyelectrolyte chains leads to tough PIC hydrogels formation at much lower concentrations than that of PA hydrogels. As a result, the PIC hydrogels are much tougher than the PA hydrogels prepared at the same monomer composition. In similar to PA hydrogels, the PIC hydrogels also exhibit broad dynamic mechanical spectra, indicating the formation of ion complexes with widely ranged bond strength. The PIC hydrogels have strong viscoelasticity in comparison with PA hydrogels. However, the two systems show the similar activation energies of the dynamic mechanical spectra. The SEM microstructural observation shows that the PIC hydrogels have segregated structure while PA hydrogels are more homogeneous.
Rights: This document is the Accepted Manuscript version of a Published Work that appeared in final form in Macromolecules, copyright ©2016 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see
Type: article (author version)
Appears in Collections:生命科学院・先端生命科学研究院 (Graduate School of Life Science / Faculty of Advanced Life Science) > 雑誌発表論文等 (Peer-reviewed Journal Articles, etc)

Submitter: 龔 剣萍 (Gong Jian Ping)

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