Conditions Extrêmes et Matériaux : Haute Température et Irradiation

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J.Bidal, M.Becuwe, C.Hadad, B.Fleutot, C.Davoisne, M.Deschamps, B.Porcheron, A.Nguyen Van Nhien, 'Hybrid electrolytes based on optimized Ionic liquid quantity tethered on ZrO2 Nanoparticles for Solid-state Lithium-ion conduction', ACS Appl. Mater. Interfaces 13(13) 15159–15167 (2021) doi:10.1021/acsami.0c22422

This paper describes the simple, highly reproducible, and robust synthesis of a new solid organic/inorganic electrolyte based on the ionic liquid (IL) 1-butyl-3-(carboxyundecyl)imidazolium bis(trifluoromethylsulfonyl)imide tethered to zirconia nanoparticles (15–25 nm) by coordination and named ZrO2@IL. The IL monolayer formation, ensured by two-dimensional solid-state NMR, at the nanoparticles’ surface considerably reduces both the IL’s consumption and the IL amount at the ZrO2 surface compared to the IL-based hybrid electrolytes reported in the literature. After LiTFSI, used as a lithium source, content optimization (26 wt %), the hybrid exhibits unprecedented stable conductivity passing from 0.6 × 10–4–1 to 0.15 × 10–4–1, respectively, from 85 °C to room temperature (25 °C). Unlike silica which is commonly adopted for this type of hybrid material, zirconia makes it possible to produce more impact-resistant pellets that are easier to compact, thus being favorable for accurate conductivity studies and battery development by electrode/composite/solid electrolyte layer stacking. The ZrO2@IL/LiTFSI solid hybrid electrolyte’s thermal stability (up to 300 °C) and performance make this electrolyte suitable for lithium conduction in all-solid-state batteries.