Effect of branched structure on microphase separation and electric field induced bending actuation behaviors of poly(urethane–urea) elastomers

Polyurethane elastomers as a type of electroactive polymers have wide applications in soft actuators, soft sensors and energy harvesting due to their high dielectric constant, high electrostriction coefficients, easy processing and structure adjustability, and superior biocompatibility etc. However, the relationship between microstructure and electromechanical properties of EAEs has not been fully understood. In this work, we fabricated the branch structured poly(urethane–urea) elastomers (PUUs) using hydroxy-terminated polybutadiene as soft segment, isophorone diisocyanate and 4,4-diaminodicyclohexylmethane as hard segment, and hydroxyl-terminated four-armed polycaprolactone (PCL410) as branch structured chain extender for improving bending actuation performances, and understanding the relationship between structure and electromechanical properties. The degree of branched structure of PUUs were adjusted by the content of PCL410. The microphase separation kinetics of PUUs was enhanced as increase of PCL410 content, whereas the degree of microphase separation and hard domain size of PUUs were reduced. The mechanical loss and bending actuation stress of PUUs were significantly improved by incorporation of small amount of branched structure into PUU chains. The PUU with 2.60 mol.% of PCL410 showed 5.16 mm of bending displacement and 5.16 Pa of bending actuation stress at 7.2 kV (corresponding to 180 V mm−1 of the nominal electric field), which were 76.3, and 79 times higher than that of PUU without PCL410, respectively. The electric field induced bending actuation mechanism of branch structured PUUs was suggested that the bending actuation mechanism of branch structured PUUs is caused by electrostrictive effect from dipole orientation induced bending deformation of constrained segments and asymmetric charge density distribution on both anode and cathode sides of PUU films. Our results can provide new insight on design novel electroactive polyurethane elastomers.