Efficiently healable, recyclable, and dynamically assembled high-filled energetic composites using an insulin-inspired triple dynamic network

Abstract

Highly filled composites often exhibit limited crack-healing capacity because of the inadequate dynamic exchange mechanisms in the polymer networks, compromising safety and applicability. Herein, we propose an insulin-inspired triple dynamic network incorporating van der Waals forces, disulfide bonds, and multiple hydrogen bonds. The fast metathesis of van der Waals forces and disulfide bonds dissipates mechanical energy and enables room-temperature healing ability. Furthermore, the effective regulation of multiple hydrogen bonds, particularly quadruple hydrogen bonds in the pendant groups, optimizes the balance between mechanical robustness and healing efficiency. The optimum energetic polymer had a high mechanical toughness (9.76 MJ m⁻³), room-temperature healing efficiency (96.1% after 48 h), and energy level (Q = 1657.1 J g⁻¹). To demonstrate its applicability, we utilized the above polymer as the continuous phase, while employing a typical oxidizer (1,3,5-trinitro-1,3,5-trazinane, RDX) and metallic fuel (aluminium powder) as the dispersion phase to construct energetic composites with a solid content of 80 wt%. The prepared composites exhibited superior crack healing and recycling efficiency at 60 °C. Additionally, various energetic composites can be dynamically assembled to enable regulated energy-output functions. This study presents an approach for developing highly loaded dynamic energetic materials with superior properties and broad applicability.