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Water-Triggered Ductile–Brittle Transition of Anisotropic Lamellar Hydrogels and Effect of Confinement on Polymer Dynamics

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‡ § Graduate School of Life Science, Faculty of Advanced Life Science, and §Soft Matter GI-CoRE, Hokkaido University, N21W11, Kita-ku, Sapporo 001-0021, Japan
Department of Chemistry, University of Dhaka, Dhaka, Bangladesh
*E-mail [email protected], Tel/fax + 81-11-706-9011 (J.P.G.).
Cite this: Macromolecules 2017, 50, 20, 8169–8177
Publication Date (Web):October 4, 2017
Copyright © 2017 American Chemical Society

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    We study the effect of dehydration on the structure and mechanical properties of anisotropic lamellar hydrogels, consisting of alternative stacking of several thousands of nanoscale rigid bilayers from amphiphilic poly(dodecyl glyceryl itaconate) (PDGI) and submicroscale soft hydrogel layers from hydrophilic polyacrylamide (PAAm) networks. We found that the layered microstructure is well preserved with dehydration, and a ductile–brittle transition occurs at the critical water content. This transition is related to the rubbery–glassy transition of the PAAm layers, which occurs at 58 wt % water content and is much higher than 26 wt % of bulk PAAm hydrogels. Such specific behavior of the lamellar hydrogels indicates that the dynamics of the submicroscale PAAm hydrated layer intercalated between the rigid bilayers are very different from its bulk state.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.macromol.7b01438.

    • Additional results and discussions related to microstructure analysis (SEM) of the substantially dehydrated samples, thermogravimetric analysis (TGA) for measuring water content, photographs of the dumbbell-shaped samples at different water content, toughness of gels, and differential scanning calorimetry (DSC) for measuring enthalpy change of different water content gels (PDF)

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