Low electronic conductivity of Li 7 La 3 Zr 2 O 12 solid electrolytes from first principles

摘要: Lithium-rich garnets such as Li 7 La 3 Zr 2 O 12 (LLZO) are promising solid electrolytes with potential application in all-solid-state batteries that use lithium-metal anodes. The practical use of garnet electrolytes is limited by pervasive lithium-dendrite growth, which leads to short-circuiting and cell failure. One proposed mechanism of lithium-dendrite growth is the direct reduction of lithium ions to lithium metal within the electrolyte, and lithium garnets have been suggested to be particularly susceptible to this dendrite-growth mechanism due to high electronic conductivities relative to other solid electrolytes. The electronic conductivities of LLZO and other lithium-garnet solid electrolytes, however, are not yet well characterized. Here, we present a general scheme for calculating the intrinsic electronic conductivity of a nominally insulating material under variable synthesis conditions from first principles, and apply this to the …