High-Temperature-Mediated Assembly of Polyoxometalate-Induced Ordered Carbonaceous Superstructures

Constructing hierarchical superstructures through one-step bottom-up synthesis poses significant challenges due to strong interactions between additives and micelles, which hinders the formation of heterogeneous configurations. Here, we propose a high-temperature-mediated method to weaken these interactions and manipulate the thermal instability of micellar templates. This approach successfully synthesizes hierarchical superstructures that combine a carbonaceous nanosheet substrate with polyoxometalate (POM)-induced, highly ordered discontinuous nanodots in a single preparation step. The surface nanodots have a diameter of approximately 19 nm and are spaced about 32 nm apart. Besides, the nanodots with various arrangements can be generated by simply adjusting the amount of POM. Importantly, the superstructure features more exposed POM catalytic sites than conventional carbonaceous hybrids lacking surface architectures, resulting in excellent electrochemical performance in lithium-sulfur (Li-S) batteries. This high-temperature-mediated approach offers new insights for designing hierarchical superstructures and functional materials with enhanced activities.