Publication date: 28th August 2024
The safety and stability concerns with liquid electrolytes of Li batteries are prompting their replacement by solid-state conductors; however, ion mobilities of conventional solid electrolytes do not match up to their liquid counterparts. To address this challenge, we have been exploring fast-ion or superionic solids based on earth abundant selenides and sulfides, where cations form a “liquid-like” network within a rigid anion cage allowing cation mobilities rivaling those of liquid electrolytes. Whereas superionicity is attained in these materials only at elevated temperatures, we find that in nanocrystals of copper selenide and sulfide the superionic phase is attained at lower temperatures than in the bulk. From electronic structure investigations and in-situ electron microscopy studies of copper selenide, we find that the key factor in this effect is compressive strain prevalent in nanocrystals, which also makes ion-transport pathways energetically feasible. Superionic transport achieved in nanostructures can be extended to macroscopic length scales by assembling solids from the nanostructures. Copper selenide nanowires exhibit an ionic conductivity of 4 S/cm which is an order-of-magnitude higher than that in bulk copper selenide. This record high conductivity results from the combination of crystalline paths for conduction in the axial direction with nanoscale confinement in the radial direction. These advances pave the way for fast-ion solid electrolytes.
This work was supported by the Energy and Biosciences Institute through the EBI−Shell program.
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