Abbas, S.A.Ali, M.Hakeem, A.S.Saeed Alzahrani, A.S.Meena, M.L.Javid, M.2026-02-042024ACS Sustainable Chemistry and Engineering, 2024, 12, 14, pp. 5564-5574https://doi.org/10.1021/acssuschemeng.3c08293https://idr.nitk.ac.in/handle/123456789/21182The severe shuttling of dissolved lithium polysulfides (LiPSs) (Li<inf>2</inf>S<inf>x</inf>, 4 ≤ x ≤ 8) and the generation of lithium dendrites upon cycling have hampered the safety and performance of lithium-sulfur batteries (LSB). Herein, we report the strategy of tuning the surface energy of the pristine separator with γ-AlO(OH) nanocapsules to address the aforementioned problems. The enhanced surface energy from 26.62 to 63.64 mJ m-2 yields multiple benefits, including impeding the migrating polysulfides by chemically binding them with γ-AlO(OH) nanocapsules, enhancing the lithium-ion migration through the separator by promoting hydrophilicity in the separator and mitigating the generation of lithium dendrites by a uniform distribution of Li+ on top of lithium metal via interaction with γ-AlO(OH) nanocapsules. Live discharging of the H-cell demonstrated that the LiPS mitigation can be curtailed by using γ-AlO(OH) nanocapsules modified separator (BNC). Moreover, the BNC separator’s thermally insulating properties render the Li-S battery stable behavior while cycling at an even temperature of 75 °C. The spray coating technology used for coating γ-AlO(OH) nanocapsules on top of pristine separator offers a scalable solution for commercializing such modified separators. © 2024 American Chemical Society.Aluminum compoundsCoatingsInterfacial energyLithium compoundsLithium sulfur batteriesLithium-ion batteriesNanocapsulesSeparatorsSulfur compoundsDendrite growthEnhanced surfaceIon migrationLithium dendriteLithium ionsLithium polysulphideLithium/sulfur batteriesPerformancePolysulfide shuttlesPolysulphidesPolysulfidesTuning Surface Energy of Pristine Separator with γ-AlO(OH) Nanocapsules for Inhibiting Lithium Polysulfide Shuttle and Lithium Dendrite Growth