Combinatorial Study of Deformable Lithium Chloroboracite Solid Electrolytes

In lithium-ion batteries, solid electrolytes are an attractive alternative to their liquid counterpart due to their potential for improved energy density, lifespan and safety. The major drawback is their lower ionic conductivity, which is worsened in the case of ceramic materials by the inability of these electrolytes to form efficient contacts with other components of the battery due to their lack of deformability. Li4B7O12Cl and Li4B4Ga3O12Cl-type chloroboracites are types of solid electrolytes that have received attention for their ability to be made in a deformable glassy state and then further crystallized into the conductive phase by heating to about 525 °C. This leads to a promising approach of designing a solid battery by first mixing the glassy material with the active cathode material and then heating the mixture to convert the electrolyte to the conductive phase while maintaining the intimate mixing. However, very few compositions have been studied, and no work includes determination of the deformability of the material nor does previous work include the other necessary properties for solid electrolytes such as a large stability window. Since the elemental composition of the electrolytes greatly influences their proprieties, a thorough study to find the ideal composition from innumerable doping possibilities is clearly necessary. Herein, we have adapted a high-throughput glass synthesis approach to the synthesis of chloroboracites. For the two test materials (Li4B7O12Cl and Li4B4Ga3O12Cl) we obtain phase pure materials after re-crystallization that match the results from literature. Our combinatorial approach also yields ionic conductivities in agreement with prior literature. We further identify challenges not reported previously such as poor stability against humidity leading to proton conduction, and a limited stability window. Beyond the proof of concept, we have used the high throughput screening to test the effect of up to 62 elements simultaneously. This facilitates the generation of information about the elemental dopant’s influence on conductivity, deformability and any other relevant characteristics pertaining to electrolytes in all solid-state batteries. Importantly, we identified thulium as the dopant that improved both deformability of the glass and ionic conductivity of the recrystalized chloroboracite when used at a modest 2% doping level. This thorough screening of these materials will dramatically accelerate our testing and development of these promising materials.

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