Superstructured Nanocrystals/Dual-Doped Mesoporous Carbon Anodes for High-Performance Sodium-Ion Batteries

Abstract

Two-dimensional ordered superstructures have been attracting considerable attention due to their interesting properties and potential applications. However, designing ideal functional superstructures with excellent electrochemical properties is still a major challenge, and an in-depth understanding of the structure-activity relationship of electrodes remains to be achieved. To elucidate this critical issue, herein, we rationally designed and synthesized for the first time superstructured TiO₂/dual-doped mesoporous carbon anodes using confined space and surface coassembly strategies. Our method primarily relied on the larger interlayer space few-layered MXene and its negatively charged surface, allowing hexamethylenetetramine intercalation and surface electrostatic adsorption. The superstructured TiO₂/dual-doped mesoporous carbon was successfully assembled by the thermal decomposition of a confined carbon precursor. Subsequently, the comparison of Na⁺-storage properties of various anodes was carried out based on the results of structural characterization techniques and electrochemical analysis methods. The results showed that the optimized anode (N/O-C@TiO₂-20) can deliver a reversible capacity of 165 mA h g^-1 after 1000 cycles at a current density of 1 A g^-1, indicating excellent electrochemical properties. The enhancement can be attributed to the synergistic effect of carbon domains, defective nanocrystals, and a covalently coupled interface between TiO₂ and mesoporous carbon. Our work not only offered a new strategy for the assembly and regulation of superstructures to promote the electrochemical performance but also enlightened the rational design of advanced anodes for sodium-ion battery application.