Improvement of Mechanical Strength and Fatigue Resistance of Double Network Hydrogels by Ionic Coordination Interactions

自愈水凝胶 材料科学 韧性 离子键合 共价键 网络结构 离子强度 琼脂 化学工程 氢键 复合材料 离子 化学 分子 计算机科学 高分子化学 工程类 有机化学 机器学习 水溶液 生物 遗传学 细菌
作者
Qiang Chen,Xiaoqiang Yan,Lin Zhu,Hong Chen,Bing Jiang,Dandan Wei,Lina Huang,Jia Yang,Baozhong Liu,Jie Zheng
出处
期刊:Chemistry of Materials [American Chemical Society]
卷期号:28 (16): 5710-5720 被引量:259
标识
DOI:10.1021/acs.chemmater.6b01920
摘要

Double network hydrogels (DN gels) are considered as one of the toughest soft materials. However, conventional chemically linked DN gels often lack high self-recovery and fatigue resistance properties due to permanent damage of covalent bonds upon deformation. Current strategies to improve self-recovery and fatigue resistance properties of tough DN gels mainly focus on the manipulation of the first network structure. In this work, we proposed a new design strategy to synthesize a new type of Agar/PAMAAc-Fe3+ DN gels, consisting of an agar gel as the first physical network and a PAMAAc-Fe3+ gel as the second chemical–physical network. By introducing Fe3+ ions into the second network to form strong coordination interactions, at optimal conditions, Agar/PAMAAc-Fe3+ DN gels can achieve extremely high mechanical properties (σf of ∼8 MPa, E of ∼8.8 MPa, and W of ∼16.7 MJ/m3), fast self-recovery (∼50% toughness recovery after 1 min of resting), and good fatigue resistance compared to properties of cyclic loadings by simply controlling acrylic acid (AAc) content in the second network. The high toughness and fast recovery of Agar/PAMAAc-Fe3+ DN gel is mainly attributed to energy dissipation through reversible noncovalent bonds in both networks (i.e., hydrogen bonds in the agar network and Fe3+ coordination interactions in the PAMAAc network). The time-dependent recovery of Agar/PAMAAc-Fe3+ gels at room temperature and the absence of recovery in Agar/PAMAAc gels also confirm the important role of Fe3+ coordination interactions in mechanical strength, self-recovery, and fatigue resistance of DN gels. Different mechanistic models were proposed to elucidate the mechanical behaviors of different agar-based DN gels. Our results offer a new design strategy to improve strength, self-recovery, and fatigue resistance of DN gels by controlling the structures and interactions in the second network. We hope that this work will provide an alterative view for the design of tough hydrogels with desirable properties.
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