A novel self-catalytic cooperative multiple dynamic moiety: towards rigid and tough but more healable polymer networks

A formidable scientific challenge for the development of self-healing polymers is how to rationally design molecular architectures that could integrate both highly efficient healing functions and excellent mechanical performances. Here, we present a novel rigid and tough but more healable polymer network enabled by self-catalytic cooperative multiple dynamic moieties (CMDMs) containing metal-ligand coordinations, multiple hydrogen bonds and reversible urea bonds. The strength and toughness of the materials are improved significantly via strong supramolecular interactions of CMDMs, resulting in a modulus, tensile strength and toughness up to 797.4 MPa, 73.6 MPa and 218.2 MJ m(-3), respectively. The metal-ligand coordinations of CMDMs facilitate the dynamic exchange reactions between the urea bonds of CMDMs through a self-catalytic mechanism, providing the material with a much higher healing efficiency of 90% compared with 48% for the control sample without metal-ligand coordinations. CMDMs provide a novel paradigm for designing robust healable materials by integrating dynamic covalent bonds and supramolecular interactions into one single moiety.

Automated summary

CMDMs is a novel rigid, tough, and more healable polymer network enabled by self-catalytic cooperative multiple dynamic moieties containing metal-ligand coordinations, multiple hydrogen bonds, and reversible urea bonds. The strength and toughness of the materials are significantly improved via strong supramolecular interactions of CMDMs, and the material achieves a much higher healing efficiency through metal-ligand coordinations.