Guanine and cytosine‐containing acrylic supramolecular networks
Guanine and cytosine‐containing acrylic supramolecular networks
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DOI：
10.1002/pol.20230320
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发表时间：
2023-08
影响因子：
3.4
通讯作者：
Boer Liu;G. Spiering;Rose K. McDonough;R. Moore;T. Long
中科院分区：
文献类型：
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作者：
Boer Liu;G. Spiering;Rose K. McDonough;R. Moore;T. Long
本文描述了鸟嘌呤和胞嘧啶-含超分子共聚物的合成和表征，其灵感来自于脱氧核糖核酸中的鸟嘌呤和胞嘧啶核碱基对。区域选择性迈克尔加成使得核碱基能够有效地安装在含丙烯酸酯的单体上，这使得使用传统的自由基共聚制备一系列核碱基功能化丙烯酸酯和丙烯酸正丁酯共聚物成为可能。含鸟嘌呤的共聚物表现出比含胞嘧啶的共聚物类似物更好的热性能、热机械性能和更明确的形态结构，这是由于其相对强的鸟嘌呤自结合，从而扩大了机械增强聚合物网络的潜在应用。含有鸟嘌呤和胞嘧啶的共混共聚物通过鸟嘌呤和胞嘧啶之间的多个氢键形成了超分子结构。超分子共混物表现出中等的热力学和形态特性，这表明鸟嘌呤和胞嘧啶单元在随机共聚物组成中没有完全结合。这项工作为鸟嘌呤-胞嘧啶自相互作用和互补相互作用下丙烯酸共聚物的结构-性能-形态关系提供了有价值的基础理解，为增强机械和形态性能的超分子设计提供了新的认识。
This manuscript describes the synthesis and characterization of guanine and cytosine‐containing supramolecular copolymers, which are inspired from the guanine and cytosine nucleobase pair in deoxyribonucleic acid. Regioselective Michael‐addition allowed the efficient installation of the nucleobases on acrylate‐containing monomers, which enabled the preparation of a series of nucleobase‐functionalized acrylate and n‐butyl acrylate copolymers using conventional free radical copolymerization. Guanine‐containing copolymers exhibited superior thermal properties, thermomechanical performance, and more defined morphological structure than cytosine‐containing copolymer analogs due to the relatively strong guanine self‐association, thus expanding the potential applications for mechanically reinforced polymeric networks. Blending guanine‐ and cytosine‐containing copolymers formed a supramolecular structure through multiple hydrogen bonding between guanine and cytosine units. The supramolecular blend exhibited intermediate thermomechanical and morphological properties, which suggested that guanine and cytosine units were not fully associated in the random copolymer composition. This work provides valuable fundamental understanding of structure–property‐morphology relationships in acrylic copolymers with the presence of guanine‐cytosine self‐ and complementary interactions, suggesting new understanding in supramolecular design for enhanced mechanical and morphological properties.