Environmentally friendly regenerated cellulose films with improved dielectric properties via manipulating the hydrogen bonding network

Polymer dielectrics with a high energy density, an outstanding breakdown strength, and a low dielectric loss are currently in great demand in the field of film capacitors. Here, on the basis of fundamental understanding of dielectric relaxation in cellulose, environmentally friendly regenerated cellulose-based dielectrics were fabricated by manipulating their intrinsic hydrogen bonding network, in which hydroxyl groups of cellulose were reacted with epichlorohydrin (ECH) to simultaneously reduce the density of the intra- and intermolecular hydrogen bonding networks and the crystallinity for activating the movement of polar groups. As a result, when the molar ratio of ECH to glucose units of cellulose is 1:1, the regenerated cellulose-based dielectrics exhibited the highest dielectric constant of 9.7 at 103 Hz with the dielectric loss in an order of 10−2 and an energy density of 2.16 J/cm3 with a high charge–discharge efficiency of >85% at 200 MV/m. This methodology presented here provides a promising avenue for designing and improving the dielectric properties of cellulose-based dielectrics.