Decoupling conductivity and mechanics: Rational design of pre-constructed 3D skeletal organogels via interfacial...

Conductive gels face an intrinsic trade-off between electrical conductivity and mechanical robustness, as conventional single-network or filled composite designs couple these functions. Here, we present a generalizable strategy to fundamentally overcome this constraint by architecturally decoupling the charge transport pathway from the mechanical load-bearing matrix. We demonstrate this concept by constructing a three-dimensional (3D) graphitic carbon skeleton (derived from carbonized melamine foam) as a pre-formed, continuous conductive scaffold. This rigid framework is subsequently infiltrated with a ductile poly(vinyl alcohol)/glycerol/water gel precursor via centrifugal assistance, followed by solvent exchange and wet-annealing to reinforce the matrix. In this architecture, the uninterrupted carbon network provides stable electron transport (0.35 S m^-1), while the physically cross-linked PVA network, optimized through hierarchical hydrogen bonding and crystallization, delivers high mechanical performance (tensile strength ≈ 3.1 MPa, toughness ≈ 7.5 MJ m^-3, fracture strain >310%). This decoupled design not only resolves the classic performance trade-off but also imparts multifunctionality, including stable piezoresistive sensing across a wide temperature range (-20 to 120 °C) and efficient photothermal conversion. This work establishes a robust and versatile platform for designing high-performance, environmentally resilient conductive materials for soft electronics by moving from material-centric compositions to architecture-defined functionalities.