2024-03-28T15:17:36Zhttps://eprints.lib.hokudai.ac.jp/dspace-oai/requestoai:eprints.lib.hokudai.ac.jp:2115/831642022-11-17T02:08:08Zhdl_2115_20055hdl_2115_8527Polyzwitterions as a Versatile Building Block of Tough Hydrogels: From Polyelectrolyte Complex Gels to Double-Network GelsYin, HaiyanKing, Daniel RSun, Tao LinSaruwatari, YoshiyukiNakajima, TasukuKurokawa, TakayukiGong, Jian Pingdouble-network hydrogelinterpenetrating network hydrogelpolyelectrolyte complexpolyzwitteriontoughnessbiomaterials430The high water content of hydrogels makes them important as synthetic biomaterials, and tuning the mechanical properties of hydrogels to match those of natural tissues without changing chemistry is usually difficult. In this study, we have developed a series of hydrogels with varied stiffness, strength, and toughness based on a combination of poly(2-acrylamido-2-methylpropane sulfonic acid) (PAMPS), a strong acidic polyelectrolyte, and poly-N-(carboxymethyl)-N,N-dimethyl-2-(methacryloyloxy) ethanaminium) (PCDME), a polyzwitterion with a weak acidic moiety. We demonstrate that modifying the true molar ratio, R, of PCDME to PAMPS results in four unique categories of hydrogels with different swelling ratios and Young’s moduli. When R < 1, a negatively charged polyelectrolyte gel (PE) is formed; when 1 < R < 3, a tough and viscoelastic polyelectrolyte complex gel (PEC) is formed; when 3 < R < 6.5, a conventional, elastic interpenetrating network gel (IPN) is formed; and when R > 6.5, a tough and stiff double-network gel (DN) is formed. Both the PEC and DN gels exhibit high toughness and fracture stress, up to 1.8 and 1.5 MPa, respectively. Importantly, the PEC gels exhibit strong recovery properties along with high toughness, distinguishing them from DN gels. Without requiring a change in chemistry, we can tune the mechanical response of hydrogels over a wide spectrum, making this a useful system of soft and hydrated iomaterials.American Chemical Society(ACS)Journal Articleapplication/pdfhttp://hdl.handle.net/2115/83164https://eprints.lib.hokudai.ac.jp/dspace/bitstream/2115/83164/2/ACS%20applied%20materials%20%26%20interfaces_2020.pdf1944-8244AA12406529ACS Applied Materials & Interfaces124450068500762020-11-04enginfo:doi/10.1021/acsami.0c15269This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS applied materials & interfaces, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see To access the final edited and published work see https://dx.doi.org/10.1021/acsami.0c15269.author