Thermadapt shape memory AB-copolymer networks exhibiting tunable properties and kinetics of topological rearrangement

IF 4.5 3区 工程技术 Q1 CHEMISTRY, APPLIED
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Abstract

Polycaprolactone (PCL) based thermadapt shape memory polymers (SMPs) have exhibited superiority over traditional analogues by allowing shape-editing to reconfigure permanent shapes into more complex geometrical shapes, driven by the pursuit of advanced functionalities for high-value applications. Nevertheless, although transesterification-based PCL networks exhibit impressive shape reconfigurability as prototypical thermadapt SMPs, there are still constraints in terms of the need for significant flexibility in architectural adjustment and property modulation without compromising reconfigurability, which would be relevant for practical applications. Here, we present a simple yet efficient strategy to create PCL-based thermadapt SMPs that possess a highly tunable structure and properties, as well as exceptional reconfigurability. The family of SMPs, called thermadapt shape memory AB copolymer networks (AB-CPNs), was synthesized by UV-initiated free radical polymerization between PCL diacrylate as crosslinker and 4-hydroxybutyl acrylate (HBA) as comonomer. The thermadapt AB-CPNs allow for significant structural alterations with 0 wt% to 70 wt% HBA while maintaining excellent shape memory and shape reconfigurability effects. The insertion of the polymer segment containing free hydroxyls not only promises tunable material properties but also makes network rearrangement easier since dynamic hydroxy-ester bonds are more active than dynamic ester-ester bonds. It is envisioned that the thermadapt shape memory AB-CPNs with widely tunable macroscopic properties will drive progress in the real-world applications of SMP devices with complicated geometric structures.

Abstract Image

具有可调特性和拓扑重排动力学的热适应形状记忆 AB 聚合物网络
基于聚己内酯(PCL)的热适应形状记忆聚合物(SMP)在追求高价值应用的高级功能性的推动下,通过形状编辑将永久形状重新配置为更复杂的几何形状,表现出优于传统同类产品的优势。然而,尽管基于酯交换反应的 PCL 网络作为热适应 SMP 的原型,表现出了令人印象深刻的形状可重构性,但在实际应用中,由于需要在不影响可重构性的前提下实现结构调整和属性调节的极大灵活性,因此仍然存在一些限制因素。在这里,我们提出了一种简单而高效的策略,用于制造基于 PCL 的热适应 SMP,这种 SMP 具有高度可调的结构和特性,以及卓越的可重构性。该系列 SMP 被称为热适应形状记忆 AB 共聚物网络(AB-CPNs),是以 PCL 二丙烯酸酯为交联剂、4-羟基丁基丙烯酸酯(HBA)为共聚单体,通过紫外光引发的自由基聚合反应合成的。热适应 AB-CPN 可在 0 wt% 至 70 wt% HBA 的范围内实现显著的结构变化,同时保持出色的形状记忆和形状可重构效果。由于动态羟基-酯键比动态酯-酯键更活跃,因此插入含有游离羟基的聚合物段不仅能保证材料的可调特性,还能使网络重排更容易。可以预见,具有广泛可调宏观特性的热适应形状记忆 AB-CPN 将推动具有复杂几何结构的 SMP 器件的实际应用取得进展。
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来源期刊
Reactive & Functional Polymers
Reactive & Functional Polymers 工程技术-高分子科学
CiteScore
8.90
自引率
5.90%
发文量
259
审稿时长
27 days
期刊介绍: Reactive & Functional Polymers provides a forum to disseminate original ideas, concepts and developments in the science and technology of polymers with functional groups, which impart specific chemical reactivity or physical, chemical, structural, biological, and pharmacological functionality. The scope covers organic polymers, acting for instance as reagents, catalysts, templates, ion-exchangers, selective sorbents, chelating or antimicrobial agents, drug carriers, sensors, membranes, and hydrogels. This also includes reactive cross-linkable prepolymers and high-performance thermosetting polymers, natural or degradable polymers, conducting polymers, and porous polymers. Original research articles must contain thorough molecular and material characterization data on synthesis of the above polymers in combination with their applications. Applications include but are not limited to catalysis, water or effluent treatment, separations and recovery, electronics and information storage, energy conversion, encapsulation, or adhesion.
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