Interface Engineering Enhances Pseudocapacitive Contribution to Alkali Metal Ion Batteries

Increasing the pseudocapacitive contribution has been regarded as an effective means to overcome slow diffusion-limited redox mechanism in electrode materials. Enhanced pseudocapacitive contribution by interface engineering holds huge potential in improving the electrochemical performance of composite electrodes owing to the effective manipulation of ionic transfer kinetics. In this work, the Sb2S3@TiO2 composite with a nitrogen-doped three-dimensional carbon skeleton was designed as the anode for lithium (sodium)-ion batteries (LIBs/SIBs), which delivered significantly enhanced pseudocapacitive contribution. Sb2S3 acted as the main contributor of high capacity, while the addition of amorphous TiO2 suppressed the excessive growth of Sb2S3 on the three-dimensional carbon framework and improved the stability of composite electrodes. Moreover, the edge positions of Sb2S3 and TiO2 are abundant. The combination of TiO2 and Sb2S3 eliminated the band gap of the material, greatly improved the electronic conductivity and pseudocapacitance contribution, thus accelerating the reaction kinetics, which verifies by the first-principles calculation results. Benefit from this, the featured anode exhibited ultralong cycle life and improved rate performance, with a specific capacity of 451.5 mA h g–1 for 200 cycles at 0.5 A g–1 (LIBs) and 300.5 mA h g–1 for 1600 cycles at 0.5 A g–1 (SIBs). This work provides some insights into enhanced pseudocapacitive contribution to multi-battery charge storage by manipulating the interface effect of electrode materials.