Lithium-sulfur batteries (LSBs) are very promising for large-scale electrochemical energy storage. However, dissolution and shuttling of lithium polysulfides (LiPSs) intermediates have severely affected their overall electrochemical properties and limited their practical application. Designing polar cathode hosts that can effectively bind LiPSs and simultaneously promote their redox conversion is crucial for realizing high-performance LSBs. Herein, we report bronze TiO2 (TiO2-B) nanosheets (~5 nm in thickness) chemically bonded with carbon as a novel multifunctional cathode host for advanced LSBs. Experimental observation and first-principles density functional theory (DFT) calculations reveal that the TiO2-B with exposed (100) plane and Ti3+ ions exhibited high chemical affinity toward polysulfides and effectively confined them at surface. Meantime, Ti3+ ions and interface coupling with carbon promoted electronic conductivity of the composite cathode, leading to enhanced redox conversion kinetics of LiPSs during charge/discharge. Consequently, the as-assembled TiO2-B/S cathode manifested high capacity (1165 mAh/g at 0.2 C), excellent rate capability (244 mAh/g at 5 C) and outstanding cyclability (572 mAh/g over 500 cycles at 0.2 C). This work sheds insights on rational design and fabrication of novel functional electrode materials for beyond Li-ion batteries.
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