Electronic structure modulation of yttrium sites with heteroanions coordination enhances the bidirectional catalytic performance of lithium-sulfur batteries

Abstract

Oxyfluorides exhibit unique properties, including catalytic activity and electrical conductivity. However, to date, there has been minimal application of oxyfluorides in the field of lithium-sulfur (Li-S) batteries. This study synthesizes yttrium oxyfluoride-doped semi-encapsulated porous carbon nanofibers (YOF@PCNFs) using through electrospinning strategy for the separator coating in Li-S batteries. The precisely engineered OF heteroanionic environment surrounding the Y cation can adjust the lattice spacing and electronic density of the catalyst. This enhancement improves interactions between the active sites and the reactants, intermediates, and products, reduces the energy barrier for polysulfide (LiPSs) conversion, and enhances the bidirectional catalytic conversion capability of LiPSs. Furthermore, the semi-encapsulated structure helps inhibit polysulfide shuttle and ensures uniform Li-ion deposition. Improved catalysts and the interconnected special structure can establish a series of polysulfides conversion factories which operate efficiently over the long term through a “confinement-adsorption-catalysis-desorption” process, thereby enhancing battery cycling stability. The assembled Li-S full cell exhibits a high initial capacity of 1013.2 mAh/g at 1 mA cm−2 and maintains steady operation over 1500 cycles, with a minimal capacity decay rate of only 0.039 % per cycle. Even at a high current density of 4 mA cm−2, it operates for 200 cycles with an exceptionally low decay rate of 0.081 % per cycle. The study provides an anion hybrid strategy for typical metal catalysts, offering design guidelines for tailored advanced Li-S catalysts.