Soft materials can sustain large, elastic, and reversible deformations, finding widespread use as elastomers and hydrogels. These materials constitute 3-D polymer networks and are typically synthesized by cross-linking polymer chains or copolymerizing monomer and cross-linker. Seminal investigations have enabled control over the network architecture by cross-linking chains of poly(dimethylsiloxane), poly(1,4-butadiene), or tetra-poly(ethylene glycol); however, as soft materials become attractive for robotics, electronics, and prosthetics, codesigning the network architecture, mechanical, and functional properties has become pressing. We investigate the relationship among reaction pathway, network architecture, and mechanical properties in poly(ethyl glycidyl ether) networks synthesized by epoxide ring-opening polymerization with two organoaluminum catalysts. The key result is that uncontrolled polymerizations yield loosely cross-linked, entangled, soft, and extensible networks, whereas more controlled polymerizations, instead, lead to highly cross-linked, stiff, and brittle networks. Such catalytic control over network architecture and mechanical properties could enable design of novel soft, tough, and functional materials.

中文翻译：

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用有机铝催化剂控制聚醚网络的结构和机械性能

软材料可以承受大的、弹性的和可逆的变形，被广泛用作弹性体和水凝胶。这些材料构成 3-D 聚合物网络，通常通过交联聚合物链或共聚单体和交联剂来合成。开创性的研究通过交联聚（二甲基硅氧烷）、聚（1,4-丁二烯）或四聚（乙二醇）链实现了对网络结构的控制；然而，随着软材料对机器人、电子设备和假肢的吸引力越来越大，对网络架构、机械和功能特性进行协同设计变得迫在眉睫。我们研究了反应途径、网络结构、用两种有机铝催化剂通过环氧化物开环聚合合成的聚（乙基缩水甘油醚）网络的力学性能和力学性能。关键结果是，不受控制的聚合产生松散交联、缠结、柔软和可延展的网络，而更多受控聚合反而导致高度交联、僵硬和易碎的网络。这种对网络结构和机械性能的催化控制可以实现新型柔软、坚韧和功能性材料的设计。