Anomalous enhanced swelling of charged copolymer gels

IF 4.1 2区 化学 Q2 POLYMER SCIENCE Polymer Pub Date : 2024-12-13 DOI:10.1016/j.polymer.2024.127934
Esli Diepenbroek, E. Stefan Kooij, Sissi de Beer
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Abstract

Copolymer gels are a class of hydrogels that possess at least two different monomers within the same polymer chain. A common method for synthesizing copolymer gels is the one-pot free radical polymerization reaction. In charged copolymer gels, however, this fabrication method has previously led to anomalous, and often unexplained, material properties. In this paper, we report on the anomalous, enhanced swelling of anionic poly(3-sulfopropylmethacrylate-co-2-hydroxyethylmethacrylate) (P(SPMA-co-HEMA)) hydrogels, whereby we provide experimental results and a theoretical framework to explain this swelling behavior. The swelling ratio of our copolymer gels exhibits a local optimum at 25 mol% SPMA before transiting into a linear trend between charge density and gel swelling. A kinetic study of P(SPMA-co-HEMA) copolymerization reactions revealed that a transition in copolymer architecture is taking place, from a gradient (0–50 mol%) to a random (50–100 mol%) chain character with increasing SPMA content. With Flory-Rehner’s theoretical framework, we investigate why this change in copolymer architecture leads to enhanced swelling. For gradient copolymer gels, the difference in charge distribution likely enhances the local ionic driving force, and herewith the swelling. With the ability to tune the swelling behavior by controlling the copolymer architecture, we open further possibilities to study architecture-dependent properties, such as visco-elastic and stimuli-responsive behavior, or pH- and salt-dependent swelling.

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带电共聚物凝胶的异常膨胀增强
共聚物凝胶是一类水凝胶,在同一聚合物链中至少有两种不同的单体。合成共聚凝胶的常用方法是单锅自由基聚合反应。然而,在带电共聚凝胶中,这种制造方法曾导致异常的材料特性,而且往往无法解释。在本文中,我们报告了阴离子聚(3-磺丙基甲基丙烯酸酯-2-羟乙基甲基丙烯酸酯)(P(SPMA-co-HEMA))水凝胶的异常增强溶胀,并提供了实验结果和理论框架来解释这种溶胀行为。共聚物凝胶的溶胀率在∼∼25 mol% SPMA 时达到局部最优,然后电荷密度与凝胶溶胀之间呈线性趋势。对 P(SPMA-co-HEMA)共聚反应的动力学研究表明,随着 SPMA 含量的增加,共聚物的结构正在发生从梯度(0-50 摩尔%)到无规(50-100 摩尔%)链特性的转变。利用 Flory-Rehner 的理论框架,我们研究了共聚物结构的这种变化导致溶胀增强的原因。对于梯度共聚物凝胶而言,电荷分布的差异可能会增强局部离子驱动力,从而促进溶胀。有了通过控制共聚物结构来调节溶胀行为的能力,我们就有可能进一步研究依赖于结构的特性,如粘弹性和刺激响应行为,或 pH 值和盐依赖性溶胀。
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来源期刊
Polymer
Polymer 化学-高分子科学
CiteScore
7.90
自引率
8.70%
发文量
959
审稿时长
32 days
期刊介绍: Polymer is an interdisciplinary journal dedicated to publishing innovative and significant advances in Polymer Physics, Chemistry and Technology. We welcome submissions on polymer hybrids, nanocomposites, characterisation and self-assembly. Polymer also publishes work on the technological application of polymers in energy and optoelectronics. The main scope is covered but not limited to the following core areas: Polymer Materials Nanocomposites and hybrid nanomaterials Polymer blends, films, fibres, networks and porous materials Physical Characterization Characterisation, modelling and simulation* of molecular and materials properties in bulk, solution, and thin films Polymer Engineering Advanced multiscale processing methods Polymer Synthesis, Modification and Self-assembly Including designer polymer architectures, mechanisms and kinetics, and supramolecular polymerization Technological Applications Polymers for energy generation and storage Polymer membranes for separation technology Polymers for opto- and microelectronics.
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