Dynamically regulated redox shuttling and nucleation of lithium polysulfides through the built-in ferroelectric field

Abstract

Sulfur is highly desired for energy storage devices by virtue of its high theoretical specific capacity and natural abundance. Yet the lithium-sulfur battery becomes practically unstable due to the migration of lithium polysulfides (LiPSs), which is the major challenge for its widespread application. Here, we demonstrate that the polysulfide redox shuttling can be kinetically buffered, which relies on a rational design of ferroelectric/carbon interfaces in a silica-based host structure. In situ TEM observation shows that a robust sulfur host is constructed by spatially embedding ferroelectric BaTiO₃ nanodots within both the shell and bulk of a yolk-shell microsphere. During the electrochemical cycling process, the as-prepared composite material functions as a LiPSs pocket. It facilitates the reversible LiPSs conversion, giving rise to long-term stabilization of lithium-sulfur battery. This is due to the synergetic effect of the built-in polarization electric field and abundant LiPSs nucleation sites at internal ferroelectric/carbon interfaces. Furthermore, we show that the nucleation and growth of Li₂S_n can be regulated by the designed polarization electric field in the yolk-shell structure. This study further highlights the potential of physical field towards high-performance lithium-slfur batteries.