Modular design of Diels-Alder reversible networks for the facile production of highly tunable materials

IF 4.5 3区 工程技术 Q1 CHEMISTRY, APPLIED
George Misiakos, Laurens Parmentier, Sandra Van Vlierberghe
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Abstract

Covalent adaptable networks (CANs) have attracted significant attention due to their potential to form crosslinked, yet reprocessable networks. Their ability to rearrange upon exposure to specific stimuli, in combination with properties such as self-healing can advance the development of novel materials, including for additive manufacturing. Thorough understanding of structure-property relations and processing potential will aid future application-driven research in network design as well as material selection. Therefore, a multitude of CANs were synthesized herein, by crosslinking epoxide-based oligomers via the furan-maleimide Diels-Alder reaction, to evaluate small systematic variations of (co)monomer composition, crosslinker length/flexibility and crosslinking density as vectors of tuning the CANs' thermomechanical properties. Networks with glass transition temperatures (Tg) spanning from <−40 °C up to >20 °C and Young's Moduli spanning from 0.2 MPa to >500 MPa were readily attainable. Crosslinker length/flexibility had a profound impact on the tensile properties, while changes in backbone composition provided insight into the impact of secondary interactions versus rigid moieties on mechanical performance. Self-healing at ambient conditions was demonstrated for elastomeric networks, with healing efficiency being enhanced when using longer crosslinkers. Finally, a cell viability and metabolic activity assay provided a preliminary in vitro demonstration of the biocompatibility of these materials.

Abstract Image

模块化设计 Diels-Alder 可逆网络,轻松生产高度可调材料
共价可适应网络(CAN)因其形成交联但可再加工网络的潜力而备受关注。它们在受到特定刺激时能够重新排列,结合自愈合等特性,可推动新型材料的开发,包括用于增材制造的材料。对结构-性能关系和加工潜力的透彻了解将有助于未来在网络设计和材料选择方面开展以应用为导向的研究。因此,本文通过呋喃-马来酰亚胺 Diels-Alder 反应交联环氧化物基低聚物,合成了多种 CAN,以评估(共)单体成分、交联剂长度/柔性和交联密度的微小系统变化,作为调整 CAN 热机械性能的载体。这些网络的玻璃化转变温度(Tg)从 -40 °C 到 20 °C 不等,杨氏模量从 0.2 MPa 到 500 MPa 不等。交联剂的长度/柔性对拉伸性能有着深远的影响,而骨架成分的变化则让人们深入了解了次级相互作用与刚性分子对机械性能的影响。研究还证明了弹性网络在环境条件下的自愈合能力,使用较长的交联剂可提高愈合效率。最后,细胞存活率和新陈代谢活性测定初步证明了这些材料的体外生物相容性。
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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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