A high sulfur loading cathode is the most crucial component for lithium-sulfur batteries (LSBs) to obtain considerable energy density for commercialization applications. The major challenges associated with high sulfur loading electrodes are poor material utilization caused via the nonconductivity of the charged product (S) and the discharged product (Li2S), poor stability arisen from dissolution of lithium polysulfides (LiPSs) into most organic electrolytes and pulverization, and structural damage of the electrode caused by large volumetric expansion. A multifunctional synergistic composite enables ultrahigh sulfur content for advanced LSBs, which comprises the sulfur particle encapsulated with an ion-selective polymer with conductive carbon nanotubes and dispersed around Magnéli phase Ti4O7 (MS-3) by the bottom-up method. The ion-selective polymer provides a physical shield and electrostatic repulsion against the shuttling of polysulfides with negative charge, whereas it can permit the transmission of lithium ion (Li+) through the polymer membrane, and the carbon nanotubes twined around the sulfur promote electronic conductivity and sulfur utilization as well as strong chemical adsorption of LiPSs by means of Ti4O7. Because of this hierarchical construction, the cathode possesses a lofty final sulfur loading of 72% and large sulfur areal mass loading of 3.56 mg cm-2, which displays the large areal specific capacity of 4.22 mA h cm-2. In the same time, it can provide excellent cyclic performance with the corresponding capacity attenuation ratio of 0.08% per cycle at 0.5 C after 300 cycles. Especially, while sulfur areal mass loading is sharply enhanced to 5.11 mg cm-2, the MS-3 composite exhibits a large initial areal capacity of 5.04 mA h cm-2 and still keeps a high reversible capacity of 696 mA h g-1 at 300th cycle even at a 1.0 C. The design of high sulfur content cathodes is a viable approach for boosting practical commercialized application of LSBs.
Keywords: chemisorption; electrostatic repulsion; high sulfur content; lithium sulfur; shuttle effect.