Deploying cationic cellulose nanofiber confinement to enable high iodine loadings towards high energy and high-temperature Zn-I${}_2$ battery

High iodine loading and high-temperature adaptability of the iodine cathode are prerequisites to achieving high energy density at full battery level and promoting the practical application for the zinc-iodine (Zn-I${}_2$) battery. However, it would aggravate the polyiodide shuttle effect when employing high iodine loading and working temperature. Here, a sustainable cationic cellulose nanofiber (cCNF) was employed to confine the active iodine species through strong physiochemical adsorption to enlarge the iodine loading and stabilize it even at high temperatures. The cCNF could accommodate dual-functionality by enlarging the iodine loading and suppressing the polyiodide shuttle effect, owing to the unique framework structure with abundant surface positive charges. As a result, the iodine cathode based on the cCNF could deliver high iodine mass loading of 14.1 mg cm${}^{-2}$ with a specific capacity of 182.7 mAh g${}^{-1}$, high areal capacity of 2.6 mAh cm${}^{-2}$, and stable cycling over 3000 cycles at 2 A g${}^{-1}$, thus enabling a high energy density of 34.8 Wh kg${}^{-1}$ and the maximum power density of 521.2 W kg${}^{-1}$ at a full Zn-I${}_2$ battery level. In addition, even at a high temperature of 60 °C, the Zn-I${}_2$ battery could still deliver a stable cycling. (© 2023 Wiley‐VCH GmbH)