biostudies-literatureLee BJNational Research Foundation of Korea (NRF)U.S. Department of Energy (DOE)4629https://www.ebi.ac.uk/biostudies/studies/S-EPMC9360432biostudies-literatureUnknown13(1)Lithium-sulfur batteries have theoretical specific energy higher than state-of-the-art lithium-ion batteries. However, from a practical perspective, these batteries exhibit poor cycle life and low energy content owing to the polysulfides shuttling during cycling. To tackle these issues, researchers proposed the use of redox-inactive protective layers between the sulfur-containing cathode and lithium metal anode. However, these interlayers provide additional weight to the cell, thus, decreasing the practical specific energy. Here, we report the development and testing of redox-active interlayers consisting of sulfur-impregnated polar ordered mesoporous silica. Differently from redox-inactive interlayers, these redox-active interlayers enable the electrochemical reactivation of the soluble polysulfides, protect the lithium metal electrode from detrimental reactions via silica-polysulfide polar-polar interactions and increase the cell capacity. Indeed, when tested in a non-aqueous Li-S coin cell configuration, the use of the interlayer enables an initial discharge capacity of about 8.5 mAh cm^-2 (for a total sulfur mass loading of 10 mg cm^-2) and a discharge capacity retention of about 64 % after 700 cycles at 335 mA g^-1 and 25 °C.Nature communicationsDevelopment of high-energy non-aqueous lithium-sulfur batteries via redox-active interlayer strategy.PMC93604322016M1A2A2937137DE-AC02-06CH113572019R1A2C2086770Zuo XBZhao CXu GLAmine KLiu XLee BJKang THLi TYu JSPark HYJung YYu JHKang JXu WfalseDevelopment of high-energy non-aqueous lithium-sulfur batteries via redox-active interlayer strategy.Lithium-sulfur batteries have theoretical specific energy higher than state-of-the-art lithium-ion batteries. However, from a practical perspective, these batteries exhibit poor cycle life and low energy content owing to the polysulfides shuttling during cycling. To tackle these issues, researchers proposed the use of redox-inactive protective layers between the sulfur-containing cathode and lithium metal anode. However, these interlayers provide additional weight to the cell, thus, decreasing the practical specific energy. Here, we report the development and testing of redox-active interlayers consisting of sulfur-impregnated polar ordered mesoporous silica. Differently from redox-inactive interlayers, these redox-active interlayers enable the electrochemical reactivation of the soluble polysulfides, protect the lithium metal electrode from detrimental reactions via silica-polysulfide polar-polar interactions and increase the cell capacity. Indeed, when tested in a non-aqueous Li-S coin cell configuration, the use of the interlayer enables an initial discharge capacity of about 8.5 mAh cm^-2 (for a total sulfur mass loading of 10 mg cm^-2) and a discharge capacity retention of about 64 % after 700 cycles at 335 mA g^-1 and 25 °C.2022-01-01T00:00:00Z2022 Aug2025-04-05T08:55:57.913Z2025-04-05T08:55:57.913ZS-EPMC93604323594111010.1038/s41467-022-31943-8