Multiscale MD-FEA Investigation on Large-Deformation Mechanical Behaviors of Hydrogels Modified with Ionic Liquids

Hydrogels incorporated with ionic liquids (ILs) demonstrate broad application prospects in the fields of wearable flexible sensors and human physiological monitoring. Nevertheless, the intrinsic correlation between microscale intermolecular interactions and macroscale nonlinear mechanical responses under large tensile deformation has not yet been fully clarified. In this work, a coupled numerical framework integrating molecular dynamics (MD) and finite element method (FEM) was adopted to explore the mechanical behaviors of poly(acrylic acid)/N,N’-bis(acryloyl)cystamine/ionic liquid (PAA/NB/IL) hydrogels under large deformation. A series of molecular models with graded IL doping levels were established to characterize the structural rearrangement and energy change characteristics during uniaxial tension. Numerical results from MD simulations reveal that the addition of ILs strengthens non-covalent interactions such as van der Waals forces and electrostatic attractions, and further drives covalent bond stretching and angular deformation to bear external loads under high-strain conditions. Meanwhile, a generalized Maxwell constitutive model, whose Prony-series parameters were fitted by experimental stress-relaxation data, was introduced into FEM numerical calculations. The simulated quasi-static tensile properties are highly consistent with experimental measurements. Comprehensive analysis demonstrates that the mechanical enhancement induced by ILs stems from the synergistic effect of covalent structural deformation and the reconstruction of non-covalent interactions, which offers valuable theoretical guidance for the development of hydrogel materials applied in large-deformation engineering scenarios.