Molecular Clogging Organogels with Excellent Solvent Maintenance, Adjustable Modulus, and Advanced Mechanics for Impact Protection

Abstract Inspired by mechanically interlocking supramolecular materials, exploiting the size difference between the bulky solvent and the cross‐linked network mesh, a molecular clogging (MC) effect is developed to effectively inhibit solvent migration in organogels. A bulky solvent (branched citrate ester, BCE) with a molecular size above 1.4 nm is designed and synthesized. Series of MC‐Gels are prepared by in situ polymerization of crosslinked polyurea with BCE as the gel solvent. The MC‐Gels are colorless, transparent, and highly homogeneous, show significantly improved stability than gels prepared with small molecule solvents. As solvent migration is strongly inhibited by molecular clogging, the solvent content of the gels can be precisely controlled, resulting in a series of MC‐Gels with continuously adjustable mechanics. In particular, the modulus of MC‐Gel can be regulated from 1.3 GPa to 30 kPa, with a variation of 43 000 times. The molecular clogging effect also provides MC‐Gels with unique high damping (maximum damping factor of 1.9), impact resistant mechanics (high impact toughness up to 40.68 MJ m⁻³). By applying shatter protection to items including eggs and ceramic armor plates, the potential of MC‐Gels as high strength, high damping soft materials for a wide range of applications is well demonstrated.