Cesium Phosphotungstate Salt Nanospheres Coated on a 3D Graphene Framework for Lithium Ion Batteries

Traditional cathode materials for lithium‐insertion compounds, such as LiCoO2, LiMn2O4, LiNiO2, and LiFePO4, have been highly successful, but they face severe limitations in terms of energy density and production cost associated with their usage. Therefore, the design of next‐generation energy storage devices, such as molecular cluster batteries, is an important and hot topic in current research. While polyoxometalates have been developed for battery components for several years, common POMs, including H3PW12O40, tend to form heteropoly blues that dissolve in the electrolyte during charging and discharging processes. Hence, finding a polyoxometalates that is less soluble in electrolyte and exhibits certain electrical properties is particularly crucial for lithium‐ion battery cathodes. Here, we report the synthesis of zero‐dimensional Cs3PW12O40 nanospheres, followed by the successful embedding of Cs3PW12O40 nanospheres into three‐dimensional graphene sponge, constructing a novel hybrid material of three‐dimensional graphene@polyoxometalate (rGO@Cs3PW12O40) as a new cathode material for LIBs. The prepared rGO@Cs3PW12O40 half‐cell hybrid exhibits excellent electrochemical performance, with high specific capacity (approximately 240 mAh g‐1 at 50 mA g‐1), outstanding rate capability (95 mAh g‐1 at 2 A g‐1), and exceptional cycling stability (700 cycles at 1 A g‐1). This study provides a new perspective on the application of polyoxometalates in lithium‐ion batteries.