Strong, tough, and freeze-tolerant all-natural cellulose-based ionic conductor enabled by multiscale cellulose networks

Soft ionic conductors are widely used in flexible electronics. However, the simultaneous enhancement of their mechanical properties and ionic conductivity remains challenging. This paper reports the successful development of a strong and tough cellulose-based ionic conductor with exceptional mechanical properties and high ionic conductivity by in situ dissolution and reorganization of the fiber matrix of filter paper to create a multiscale structure. The resulting ionic conductor exhibits a fracture strength of 14.13 MPa and a fracture energy of up to 2.84 MJ/m³, exceeding most reported ionic conductors. It also exhibits an impressive ionic conductivity of up to 76.3 mS/cm. Results of experiments on its use in a flexible quasi-solid-state zinc-hybrid supercapacitor show its remarkable features, such as a high capacity of 218 mAh/g, an energy density of 217 Wh/kg, and a power density of 17,520 W/kg. Furthermore, it exhibits excellent temperature resistance, working effectively even at −60 °C. In addition, by incorporating kirigami structures, we fabricated a strain sensor with the cellulose-based ionic conductor with a high gauge factor, as well as a piezoresistive sensor for handwriting recognition and a capacitance pressure sensor for force mapping with wide range and sensitivity. This study opens up new possibilities for fabricating flexible electronics with superior performance using sustainable and renewable resources.