LAUSR

While the characteristics of the macroscopic mechanical behavior of organic aerogels are well known, the mechanisms responsible for the substructural evolution of their networks under mechanical deformation are not fully understood. Herein, organic aerogels from the aqueous sol−gel polymerization of resorcinol with formaldehyde are first prepared. Specifically, the resorcinol to water (R:W) molar ratio is varied for obtaining diverse highly open‐cellular porous structures with mean pore sizes ranging between 30 and 50 nm. The corresponding network structures are then characterized and exhibit different morphological and mechanical properties. Furthermore, a micromechanical constitutive model based on the pore‐wall kinematics is proposed. While the arrays of particles forming the pore walls are moderately connected, the pore walls are considered to behave as solid beams under mechanical deformation. Moreover, the damage mechanisms in the pore walls that result in the network collapse are defined. All model parameters are shown to be physically derived, and their sensitivity to the macroscopic network behavior is analyzed. The model predictions are shown to be in good agreement with the experimental stress−strain data of the different aerogels.