Understanding the Nature of Absorption/Adsorption in Nanoporous Polysulfide Sorbents for the Li–S Battery

The possibility of achieving high-energy, long-life storage batteries has tremendous scientific and technological significance. A prime example is the Li–S cell, which can offer a 3–5-fold increase in energy density compared with conventional Li-ion cells, at lower cost. Despite significant recent advances, there are challenges to its wide-scale implementation. Upon sulfur reduction, intermediate soluble lithium polysulfides readily diffuse into the electrolyte, causing capacity fading and poor Coulombic efficiency in the cell. Herein, we increase the capacity retention and cycle life of the Li–S cell through the use of nanocrystalline and mesoporous titania additives as polysulfide reservoirs and examine the role of surface adsorption vs pore absorption. We find that the soluble lithium polysulfides are preferentially absorbed within the pores of the nanoporous titania at intermediate discharge/charge. This provides the major factor in stabilizing capacity although surface binding (adsorption) also plays a more minor role. A cell containing TiO2 with a 5 nm pore diameter exhibited a 37% greater discharge capacity retention after 100 cycles than a cell without the titania additive, which was optimum compared to the other titania that were examined.