A one pot synthesis is applied to control the chain structure and architecture of multiply dynamic polymers, enabling fine tuning of materials properties by choice of polymer chain length or crosslink density. Macromolecules containing both non-covalent linkers based on quadruple hydrogen-bonded 2-(((6-(3-(6-methyl-4-oxo-1,4-dihydropyrimidin-2-yl)ureido)hexyl)carbamoyl)oxy)ethyl methacrylate (UPyMA), and thermoresponsive dynamic covalent furan–maleimide based Diels–Alder linkers are explored. The primary polymer's architecture was controlled by reversible addition-fragmentation chain transfer (RAFT) polymerization, with the dynamic non-covalent (UPyMA) and dynamic covalent furfuryl methacrylate (FMA) units incorporated into the same backbone. The materials are crosslinked, taking advantage of the “click” chemistry properties of the furan–maleimide reaction. The polymer materials showed stimulus-responsive thermomechanical properties with a decrosslinking temperature increasing with the polymer's primary chain length and crosslink density. The polymers had good thermally promoted self-healing properties due to the dynamic covalent Diels–Alder bonds. Besides, the materials had excellent stress relaxation characteristics induced by the exchange of the hydrogen bonds in UPyMA units.

中文翻译：

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控制聚合物体系结构以设计具有多个动态链接器的动态网络材料

一锅合成可用于控制多动态聚合物的链结构和体系结构，从而可以通过选择聚合物链长或交联密度来微调材料性能。包含两个基于四氢键合的2-（（（（6-（3-（6-甲基-4-oxo-1,4-二氢嘧啶-2-基）脲基）己基）氨基甲酰基）氧基的非共价接头的大分子探索了甲基丙烯酸乙酯（UPyMA）和基于热响应性动态共价呋喃-马来酰亚胺的Diels-Alder接头。通过可逆的加成-断裂链转移（RAFT）聚合反应控制主聚合物的结构，其中动态非共价（UPyMA）和动态共价甲基丙烯酸糠酯（FMA）单元并入同一骨架。这些材料是交联的，利用呋喃-马来酰亚胺反应的“点击”化学性质。聚合物材料显示出刺激响应的热机械性能，其中去交联温度随聚合物的主链长度和交联密度而增加。由于动态共价Diels-Alder键，该聚合物具有良好的热促进自修复性能。此外，由于UPyMA单元中氢键的交换，该材料具有优异的应力松弛特性。