Supercritical CO2 Synthesis of Freestanding Se1-xSx Foamy Cathodes for High-Performance Li-Se1-xSx Battery

Selenium-sulfur solid solutions (Se 1- x S x ) are considered to be a new class of promising cathodic materials for high-performance rechargeable lithium batteries owing to their superior electric conductivity than S and higher theoretical specific capacity than Se. In this work, high-performance Li-Se 1- x S x batteries employed freestanding cathodes by encapsulating Se 1- x S x in a N-doped carbon framework with three-dimensional (3D) interconnected porous structure (NC@SWCNTs) are proposed. Se 1- x S x is uniformly dispersed in 3D porous carbon matrix with the assistance of supercritical CO 2 (SC-CO 2 ) technique. Impressively, NC@SWCNTs host not only provides spatial confinement for Se 1- x S x and efficient physical/chemical adsorption of intermediates, but also offers a highly conductive framework to facilitate ion/electron transport. More importantly, the Se/S ratio of Se 1- x S x plays an important role on the electrochemical performance of Li- Se 1- x S x batteries. Benefiting from the rationally designed structure and chemical composition, NC@SWCNTs@Se 0.2 S 0.8 cathode exhibits excellent cyclic stability (632 mA h g−1 at 200 cycle at 0.2 A g −1 ) and superior rate capability (415 mA h g −1 at 2.0 A g −1 ) in carbonate-based electrolyte. This novel NC@SWCNTs@Se 0.2 S 0.8 cathode not only introduces a new strategy to design high-performance cathodes, but also provides a new approach to fabricate freestanding cathodes towards practical applications of high-energy-density rechargeable batteries.