Biomimetic Impact Protective Supramolecular Polymeric Materials Enabled by Quadruple H-Bonding

Nature has been inspiring scientists to fabricate impact protective materials for applications in various aspects. However, it is still challenging to integrate flexible, stiffness-changeable, and protective properties into a single polymer, although these merits are of great interest in many burgeoning areas. Herein, we report an impact-protective supramolecular polymeric material (SPM) with unique impact-hardening and reversible stiffness-switching characteristics by mimicking sea cucumber dermis. The emergence of softness–stiffness switchability and subsequent protective properties relies on the dynamic aggregation of the nanoscale hard segments in soft transient polymeric networks modulated by quadruple H-bonding. As such, we demonstrate that our SPM could efficiently reduce the impact force and increase the buffer time of the impact. Importantly, we elucidate the underlying mechanism behind the impact hardening and energy dissipation in our SPM. Based on these findings, we fabricate impact- and puncture-resistant demos to show the potential of our SPM for protective applications.