Combined role of stearic acid and maleic anhydride in the development of thermoplastic starch-based materials with ultrahigh ductility and durability.

The diverse properties reported for starch-based materials indicate their potential for use in the preparation of biodegradable flexible actuators. However, their natural brittleness and lack of durability after modification limit their practical application. Therefore, we propose a strategy for preparing flexible starch-based composites. The results of macro/micro property characterizations and molecular dynamics simulations indicated that using starch, maleic anhydride, and stearic acid (SA), the mobility of the starch chains was enhanced and retrogradation was inhibited through the synergistic effects induced by chain breaking, complex formation with SA, and esterification of the starch molecules. In addition, the elongation at break of the modified starch (MS) reached 2070 %, and considerable ductility (>1000 %) as well as well-complexed structure were maintained after six months. Furthermore, the MS was able to undergo self-healing after fracture or a temperature-controlled stiffness transition. Moreover, it underwent complete degradation in soil within 30 d. Finally, an actuator was prepared by doping the MS with nano-FeO particles to realize a dual magnetic and optical response. Dynamic monitoring was also achieved based on the electrical signal, thereby demonstrating the broad application scope of this material in the development of biodegradable flexible actuators.