Physical Polyurethane Hydrogels via Charge Shielding through Acids or Salts

Physical hydrogels with tunable stress‐relaxation and excellent stress recovery are formed from anionic polyurethanes via addition of acids, monovalent salts, or divalent salts. Gel properties can be widely adjusted through pH, salt valence, salt concentration, and monomer composition. We propose and investigate a novel gelation mechanism based on a colloidal system interacting through charge repulsion and chrage shielding, allowing a broad use of the material, from acidic (pH 4-5.5) to pH‐neutral hydrogels with Young's moduli ranging from 10 to 140 kPa.