Bioinspired design of elastomeric vitrimers with sacrificial metal-ligand interactions leading to supramechanical robustness and retentive malleability

Materials & Design

卷:192

Baochun Guo¹  Fang Liu²  Shifeng Fang²  Siwu Wu²  Zhenghai Tang² 

[1] Corresponding author.;

[2] Department of Polymer Materials and Engineering, State Key Laboratory of Pulp and Paper Engineering, South China University of Technology, Guangzhou 510640, PR China;

关键词: Elastomer;    Vitrimers;    Silyl ether;    Sacrificial bonds;    Reinforcement;   

DOI  :  

来源: DOAJ

【 摘 要 】

Most elastomeric vitrimers suffer from mechanical weakness in practical applications. Inspired by the development of strong and tough biomaterials relying on sacrificial bond-detachment mechanisms, herein we describe the biomimetic design of elastomeric vitrimers with mechanical robustness, preservable malleability, and recyclability by engineering sacrificial metal-ligand coordination bonds into exchangeable networks. In particular, we use a commercially available metal complex, aluminum acetylacetonate (Al(acac)3), to catalyze cross-linking based on the silylation reaction between hydroxylated natural rubber and hydrosilanes, thus introducing dynamic silyl ether-based architectures into the rubber matrix. At the same time, the Al3+ ions can interact with the free oxygen-containing moieties on the rubber skeleton, enabling labile Al3+O coordination bonds in the covalent framework to substantially dissipate mechanical energy through reversible bond detachment/reattachment upon deformation. As the organic acetylacetonate ligands of Al(acac)3 can facilitate the dispersion of Al3+ ions in the matrix, incorporating a small amount of organometallic complex (0.68 wt% of elastomer matrix) achieves an unparalleled improvement of the strength, modulus, and toughness of the resulting vitrimers. Moreover, due to their temperature-dependent nature, the Al3+O coordination bonds will partially dissociate at elevated temperatures, which only slightly compromises the topological rearrangements of the silyl ether-based network, but barely affects the reprocessability.

【 授权许可】

Unknown