Effect of end-block chain length on rheological properties of ABA triblock copolymer hydrogels

End-block length dependence of the hydrogel relaxation dynamics was investigated using PEO-based ABA triblock copolymer solutions in an aqueous solvent. Both ends of PEO were capped with hydrophobic poly(isopropyl glycidyl ether-co-ethyl glycidyl ether) exhibiting a lower critical solution temperature (LCST) behavior, resulting in the transition between sol and gel with temperature. Despite the nearly identical hydrophobicity of the end-blocks, the sol-to-gel transition temperature is found to be significantly dependent on the end-block length. Particularly, a small increment of the end-block length leads to significantly slower relaxation dynamics which is attributed to the thermodynamic barrier of end-block extraction. Hydrogels with an appropriate relaxation time show excellent injectability and self-healing ability, yet extremely slow relaxation dynamics result in brittle hydrogels. These results are discussed in terms of current understanding of the hydrogel relaxation dynamics and particular attention is paid to the issue of the chain dynamics between aggregated cores.