Ion-Conducting Thermoresponsive Films Based on Polymer-Grafted Cellulose Nanocrystals.

Mechanically robust, thermoresponsive, ion-conducting nanocomposite films are prepared from poly(2-phenylethyl methacrylate)-grafted cellulose nanocrystals (). One-component nanocomposite films of the polymer-grafted nanoparticle (PGN) are imbibed with 30 wt % imidazolium-based ionic liquid to produce flexible ion-conducting films. These films with 1-hexyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide () not only display remarkable improvements in toughness (>25 times) and tensile strength (>70 times) relative to the corresponding films consisting of the ionic liquid imbibed in the two-component CNC/PPMA nanocomposite but also show higher ionic conductivity than the corresponding neat PPMA with the same weight percent of ionic liquid. Notably, the one-component film containing 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ( exhibits temperature-responsive ionic conduction. The ionic conductivity decreases at around 60 °C as a consequence of the lower critical solution temperature phase transition of the grafted polymer in the ionic liquid, which leads to phase separation. Moreover, holding the film at room temperature for 24 h returns the film to its original homogenous state. These materials exhibit properties relevant to thermal cutoff safety devices (e.g., thermal fuse) where a reduction in conductivity above a critical temperature is needed.