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A topological polymer network with Cu(Ⅱ)-coordinated reversible imidazole-urea locked unit constructs an ultra-strong self-healing elastomer

查看全文 作　　者：Lei [1]Yang;Zenghe [1]Liu;Rasoul Esmaeely [2]Neisiany;Jiaming [1]Lou;Yifan [1]Guo;Luzhi [1]Zhang;Huijie [3]Liu;Shuo [1]Chen;Shijia [1]Gu;Zhengwei [1]You 高影响力作者 机构地区：[1]State Key Laboratory for Modification of Chemical Fibers and Polymer Materials,Institute of Functional Materials,College of Materials Science and Engineering,Donghua University,Shanghai 201620,China;[2]Department of Materials and Polymer Engineering,Faculty of Engineering,Hakim Sabzevari University,Sabzevar 9617976487,Iran;[3]Key Laboratory of Textile Science&Technology,Ministry of Education,College of Textiles,Donghua University,Shanghai 201620,China高影响力机构 出　　处：《Science China Chemistry》索引2023年第66卷第3期,共10页高影响力期刊 基　　金：supported by the National Key Research and Development Program of China(2021YFC2101800);the National Natural Science Foundation of China(52173117,21991123);the Belt&Road Young Scientist Exchanges Project of Science and Technology Commission Foundation of Shanghai(20520741000);the Natural Science Foundation of Shanghai(20ZR1402500);the Ningbo 2025 Science and Technology Major Project(2019B10068);the Science and Technology Commission of Shanghai(20DZ2254900,20DZ2270800);the Fundamental Research Funds for the Central Universities,DHU Distinguished Young Professor Program(LZA2019001). 摘　　要：It is exceedingly desired, but difficult to construct self-healing materials with both excellent mechanical properties and healing efficiency, which are usually realized by using mutually exclusive methods. Here, we reconcile this contradiction by utilizing copper-bis-(imidazole-2-yl)-methane-urea(Cu-BIMU) locked units based on novel designed dynamic imidazole-urea bonds with coupled multiple noncovalent bonds(coordination bonds, π-π stacking bonds, and hydrogen bonds). The coordination of Cu(II) greatly reduces the electron-cloud density of imidazole, which lowers the free energy barrier of imidazole-urea bonds and promotes their reversible dissociation, as demonstrated by the density functional theory and small-molecule model reaction. The topological design of Cu-BIMU polyurethane(Cu-BIMU-PU), which concentrates multiple crosslinking-in-one locked unit to avoid the formation of excessive crosslinking sites to ensure high chain mobility, facilitates self-healing. Accumulative extensive intermolecular interactions endowed excellent mechanical properties to the resulting Cu-BIMU-PU elastomer with a tensile strength of 65.3 MPa, among the highest ever-reported value. This work provides a novel molecular design principle for fabricating high-performance dynamic polymers. 关 键 词：topological polymer network SELF-HEALING ELASTOMER urea bonds
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