Tough and Fatigue Resistant Biomimetic Hydrogels of Interlaced Self-Assembled Conjugated Polymer Belts with a Polyelectrolyte Network

Supertough biomimetic hydrogels have been fabricated through in situ synthesis and guided assembling of positively charged conjugated polymer belts by using a parent poly(2-acrylamido-2-methylpropanesulfonic acid)/poly(acrylamide) double network (PAMPS/PAAm DN) gel template. The interpenetrating structures of the poly(3,4-ethylenedioxythiophene) (PEDOT) belt mesh and PAMPS/PAAm host network have been confirmed by SEM, CLSM, and Raman spectroscopy. The presence of PEDOT belts improves the Young's modulus, compressive strength, and toughness of the biomimetic (BM) hydrogels, in comparison to the parent DN gels. Cyclic tensile (300% strain) and compressive (even 90% strain) loadings demonstrate extraordinary fatigue resistance of these BM gels. Upon ten cycles, the compressive toughness remained about 1000 J m–2, which is comparable to that of articular cartilage. The internal fracture behavior and fatigue resistance of these biomimetic interpenetrating hydrogels are further investigated. These extremely tough and fatigue resistant BM hydrogels may find applications as promising substitutes for load-bearing tissues.