Investigating Swelling and Bending Response of pH-Sensitive Chitosan-Based Hydrogels

Biocompatible electroactive hydrogels with bidirectional pH-responsive bending are important for the creation of biomedical actuators. This study developed chitosan/carboxymethylcellulose (CS/CMC) semi-interpenetrating networks (SIPNs) with different volume ratios, which were crosslinked with glutaraldehyde. The swelling and bending behaviors of SPINs were systematically characterized as a function of the pH of the solution and the magnitude of the applied electric field. The hydrogels exhibited pH-dependent bidirectional actuation, with the maximum swelling of 4.67–6.00 at pH ≈ 3.9 and minimum swelling of 1.58–2.53 at pH ≈ 5.7. The SPINs with CS/CMC = 1:1 composition achieved the highest bending angle of 77° at pH ≈ 5.7, while cathodic bending up to an angle of −13.7° was observed in basic conditions. The electromechanical response was significantly enhanced by decreasing the electrode distance and increasing the applied voltage. The observed correlation between the composition, swelling behavior, and bending performance was explained in terms of the electrostatic interactions between NH3+ and COO− groups present in the CS/CMC mixtures. These findings provided novel insight into the ongoing efforts for the development of non-toxic electroactive hydrogels with tailored electromechanical bending behavior necessary for use as artificial muscles and biomedical actuators.