碳二亚胺
嬉戏
复分解
聚合
亲核细胞
高分子
化学
高分子化学
组合化学
聚合物
材料科学
有机化学
催化作用
生物化学
作者
Jeff Johnson,Samuel W. Kaplan,J. Tóth,Zian Wang,Mitchell Maw,Sergei S. Sheiko,Aleksandr V. Zhukhovitskiy
出处
期刊:ACS central science
[American Chemical Society]
日期:2023-05-11
卷期号:9 (6): 1104-1110
被引量:3
标识
DOI:10.1021/acscentsci.3c00032
摘要
Controlled incorporation of nitrogen into macromolecular skeletons is a long-standing challenge whose resolution would enable the preparation of soft materials with the scalability of man-made plastics and functionality of Nature's proteins. Nylons and polyurethanes notwithstanding, nitrogen-rich polymer backbones remain scarce, and their synthesis typically lacks precision. Here we report a strategy that begins to address this limitation founded on a mechanistic discovery: ring-opening metathesis polymerization (ROMP) of carbodiimides followed by carbodiimide derivatization. An iridium guanidinate complex was found to initiate and catalyze ROMP of N-aryl and N-alkyl cyclic carbodiimides. Nucleophilic addition to the resulting polycarbodiimides enabled the preparation of polyureas, polythioureas, and polyguanidinates with varied architectures. This work advances the foundations of metathesis chemistry and opens the door to systematic investigations of structure-folding-property relationships in nitrogen-rich macromolecules.
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