Dynamic diselenide-mediated graphene composite networks: towards shape-reprogrammable and conductivity-stable flexible electronics

Abstract

Current flexible electronics often suffer from an inherent trade-off between deformability and functional stability, limiting their ability to achieve programmable, reconfigurable shape morphing. To overcome this limitation, we propose a synergistic material design strategy that integrates dynamic covalent chemistry with functional nanofillers. Herein, a multi-stimuli-responsive shape memory polyurethane (MS-SMPU) network was constructed by crosslinking with triethanolamine and photo-responsive diselenide bonds. This dynamic network enables highly efficient photo-thermal actuation, achieving superior shape fixity (>90%) and recovery ratios (>80%), along with a significantly accelerated recovery rate (<2 s). Molecular dynamics simulations further reveal that macroscopic shape-memory properties are only weakly dependent on polymer molecular weight, offering a versatile criterion for network design. Crucially, by incorporating graphene oxide to form a robust conductive network, the resulting composite (MS-SMPU-G) exhibits ultrastable electrical conductivity under varying deformations and enables remote light-controlled circuit reconfiguration. This work not only resolves the conflict between shape morphing and conductivity stability but also demonstrates a versatile platform for adaptive soft robotics and next-generation programmable electronics.