High-performance poly(acrylic acid) hydrogels formed with a block copolymer crosslinker containing amino-acid derivatives

Two block copolymers containing two amino-acid derivatives, PEO-b-PLAA and PEO-b-PAAC, were fabricated through atom transfer radical polymerization (ATRP) or reversible addition-fragmentation chain transfer polymerization (RAFT). Then, they were employed as a macro-crosslinker to prepare high-performance poly(acrylic acid) (PAA) hydrogels named "PxAy" or "TyAz". There were numerous synergistic noncovalent interactions with hydrogen bonds between the macro-crosslinker and PAA chains, as well as entanglement of polymer chains. Hence, the hydrogels exhibited desirable mechanical properties and self-healing abilities. For PxAy hydrogels, the maximum fracture elongation and fracture strength were 9800% and 120.01 kPa, respectively. Moreover, the enhanced physical interaction enabled the hydrogels to have rapid self-healing abilities without stimulation. The hydrogels showed >80% self-healing efficiency and exhibited ∼10-3 S cm-1 electrical conductivity upon the introduction of KCl. Meanwhile, benefitting from doubling the number of carboxyl groups in the macro-crosslinker of the TyAz hydrogels compared with the PxAy hydrogels, the mechanical properties of TyAz hydrogels could be promoted further and notch-insensitivity could be observed. Tough, adhesive, self-healable, and conductive PAA hydrogels with different structures of amino-acid derivatives could aid the development of macro-crosslinkers.