Small dop of comonomer, giant shift of dynamics: α-methyl-regulated viscoelasticity of poly(methacrylamide) hydrogels

IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY GIANT Pub Date : 2024-09-23 DOI:10.1016/j.giant.2024.100342
Xin Guan , Zhiheng Zhou , Xinzhen Fan , Wenchao Xu , Yijie Jin , Chuanzhuang Zhao
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Abstract

α-Methyl groups play significant roles in the regulation of water molecules within both small molecular systems and bio-macromolecular systems. Systematically studying the influence of α-methyl on the dynamics of water molecules within hydrogel systems is therefore worthwhile. In this study, we prepared a series of hydrogen-bonded (H-bonded) hydrogels with varying densities of α-methyl groups by copolymerizing methacrylamide (MAm) with its α-methyl-absent analogue, acrylamide (Am). Introducing a small amount of Am (≤6 mol%) into the polymer chain resulted in significant shifts in the viscoelasticity of the hydrogels. The hydrogels exhibit a “time-temperature-α-methyl equivalence”, meaning that introduction of α-methyl-absent monomer has effects similar to elevating temperature and prolonging observation time on the dynamic properties. Based on low-field nuclear magnetic resonance spectroscopy and Raman scattering, a “hydrophilic defects-assisted H-bonds dissociation” mechanism is proposed, depicting that the α-methyl-absent monomer can disturb the rearrangement of water molecules surrounding the polymer chain and accelerate chain dissociation. These findings enabled the copolymer hydrogels with functions such as fast self-healing and tunable interface adhesion.
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少量共聚物掺入,动力学巨变:α-甲基调节聚(甲基丙烯酰胺)水凝胶的粘弹性
在小分子体系和生物大分子体系中,α-甲基对水分子的调节都起着重要作用。因此,系统研究α-甲基对水凝胶体系中水分子动力学的影响是有价值的。在本研究中,我们通过甲基丙烯酰胺(MAm)与不含α-甲基的类似物丙烯酰胺(Am)共聚,制备了一系列具有不同α-甲基密度的氢键(H-键)水凝胶。在聚合物链中引入少量 Am(≤6 摩尔%)可显著改变水凝胶的粘弹性。水凝胶表现出 "时间-温度-α-甲基等效",即引入α-甲基缺失单体对动态特性的影响类似于升高温度和延长观察时间。基于低场核磁共振光谱和拉曼散射,提出了 "亲水缺陷辅助 H 键解离 "机理,说明α-甲基缺失单体可干扰聚合物链周围水分子的重排,加速链解离。这些发现使共聚物水凝胶具有快速自愈合和可调界面粘附性等功能。
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来源期刊
GIANT
GIANT Multiple-
CiteScore
8.50
自引率
8.60%
发文量
46
审稿时长
42 days
期刊介绍: Giant is an interdisciplinary title focusing on fundamental and applied macromolecular science spanning all chemistry, physics, biology, and materials aspects of the field in the broadest sense. Key areas covered include macromolecular chemistry, supramolecular assembly, multiscale and multifunctional materials, organic-inorganic hybrid materials, biophysics, biomimetics and surface science. Core topics range from developments in synthesis, characterisation and assembly towards creating uniformly sized precision macromolecules with tailored properties, to the design and assembly of nanostructured materials in multiple dimensions, and further to the study of smart or living designer materials with tuneable multiscale properties.
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