Solvent-free routes are central to sustainable synthesis and processing. Topochemical polymerization offers lattice-directed access to polymers with high structural fidelity, which have potential applications across sustainable materials, responsive systems and energy-related technologies. However, its generality is constrained by the need for precise, static preorganization of reactive groups in crystals—an intrinsically fragile, often unpredictable outcome of subtle intermolecular packing.
The researchers introduce dynamical fluid lattices into the topochemical framework by using core-shell columnar liquid crystals. The intrinsic molecular motions within these fluid lattices create temporary proximity of reactive sites to activate the reaction without ideal preorganization, while the anisotropic columnar architecture directs chain growth to produce well-defined linear helical polymers with near-quantitative conversion. Despite their covalent nature, the polymers display temperature-dependent dissipative depolymerization behavior that enables full monomer regeneration. Authors further demonstrate human-interactive, temporary information encryption as a proof-of-principle application.