Ionic conductive cellulose hydrogels are some of the most promising candidates for flexible sensors. However, it is difficult to simultaneously prepare cellulose hydrogels with high mechanical strength, good ionic conductivity, and antifreeze performance. In this work, a natural clay (attapulgite)-reinforced cellulose hydrogel was fabricated. Through a one-pot method, cellulose and attapulgite were dispersed in a concentrated ZnCl2 solution. The obtained hydrogel exhibited a dual network of hydrogen bonds and Zn2+-induced ionic interactions. Attapulgite serves as an inorganic filler that can regulate the hydrogen-bonding density among cellulose molecules and provides abundant channels for fast ion transport. By optimizing the attapulgite loading, a mechanically strong (compressive strength up to 1.10 MPa), tough (fracture energy up to 0.36 MJ m-3), highly ionic conductive (4.15 S m-1), and freezing-tolerant hydrogel was prepared. These hydrogels can be used for sensitive and stable human motion sensing, demonstrating their great potential for healthcare applications.
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