Computational Mechanics Model to Evaluate the Structural Maintenance of Catenated Hydrogen-Bonded Organic Frameworks

Hydrogen-bonded organic frameworks (HOFs) have recently been highlighted as next-generation structural materials owing to their lightweight nature, mechanical flexibility, and chemical selectivity. However, despite extensive research efforts, the understanding of the structural behavior of nanometer-sized HOFs remains confined to empirical observations. Using molecular dynamics, we uncover how HOF lattices respond mechanically from energy gradients and deformation tests. This highlights that catenation acts as a key source for reduced atomic fluctuations, effective shear redistribution, and emerging auxetic deformation under in-plane loading. In particular, we demonstrate the robustness of HOF substrates modeled after biomolecular exoskeletons, proposing an engineering perspective on computational methodologies for advancing the structural design of porous organic materials.