MXene-Derived Ti_nO_(2n_1) Quantum Dots Distributed on Porous Carbon Nanosheets for Stable and Long-Life Li-S Batteries: Enhanced Polysulfide Mediation via Defect Engineering

摘要

The application of Li-S batteries has been hindered by the shuttling behavior and sluggish reaction kinetics of polysulfides. Here an effective polysulfide immobilizer and catalytic promoter is developed by proposing oxygen-vacancy-rich TinO2n-1 quantum dots (OV-T(n)QDs) decorated on porous carbon nanosheets (PCN), which are modulated using Ti3C2Tx MXene as starting materials. The T(n)QDs not only confine polysulfides through strong chemisorption but also promote polysulfide conversion via redox-active catalysis. The introduction of oxygen vacancies further boosts the immobilization and conversion of polysulfides by lowering the adsorption energy and shortening the bond lengths. The PCN provides a physical polysulfide confinement as well as a flexible substrate preventing OV-T(n)QDs from aggregation. Moreover, the two building blocks are conductive, thereby effectively improving the electron/charge transfer. Finally, the ultrasmall size of QDs along with the porous structure endows OV-T(n)QDs@PCN with large specific surface area and pore volume, affording adequate space for S loading and volume expansion. Therefore, the OV-T(n)QDs@PCN/S delivers a high S loading (79.1 wt%), good rate capability (672 mA h g(-1) at 2 C), and excellent long-term cyclability (88% capacity retention over 1000 cycles at 2 C). It also exhibits good Li+ storage under high S-mass loading and lean electrolyte.