Mechanically Adaptive and Shape‐Memory Behaviour of Chitosan‐Modified Cellulose Whisker/Elastomer Composites in Different pH Environments

Biomimetic polymer composites with water‐active mechanically adaptive and shape‐memory behaviour in different pH environments are synthesised by using chitosan‐modified cellulose whiskers (CS‐CWs) as the stimulus‐responsive phase and thermoplastic polyurethane (TPU) as the resilient matrix. The effect of surface modification on the mechanically adaptive behaviour of CS‐CW/TPU composites is investigated by using three representative solutions with various pH values. The results show that surface modification significantly enhances the modulus contrast under wet and dry conditions with the acidic solution as the stimulus, while maintaining the high modulus contrast with the basic solution as the stimulus. CS‐CW/TPU composites also exhibit excellent shape‐memory effects in all three solutions that are comparable to those pristine CW/TPU composites. Furthermore, activation of force generation in the stretched CS‐CW/TPU composites by water absorption/desorption was observed.