Garnet-based solid state batteries benefitting from an ionic/electronic mixed conductive interface constructed by lithiation of porous FeS2

Abstract

Garnet-based solid-state lithium metal batteries are considered as the potential candidates for the next-generation energy storage systems due to their high energy density, wide operating temperature, and high safety. However, the poor wettability of the lithium metal anode/garnet interface, the large interface resistance, and the risk of lithium dendrites growing and even penetrating electrolytes during cycling limit the practical application of garnet-based solid-state lithium metal batteries. In this work, a porous network FeS2 with an amorphized structure is prepared by using the solvothermal method and used as the Li/garnet interface modification layer. The porous FeS2 can be in situ converted into a Li2S/Fe mixed conductive layer by the thermal lithiation of molten metallic lithium. This mixed conductive layer can significantly reduce the interface resistance, ensure the close contact between Li and garnet, and inhibit the growth of lithium dendrites. The interface resistance of the modified Li/FeS2-LLZTO (LLZTO is Li6.5La3Zr1.5Ta0.5O12) interface at 60 °C is as small as 15.20 Ω cm2. The ionic conductivity of fully lithiated FeS2 is estimated to be 1.58 × 10−6 S cm−1 at room temperature. The Li/FeS2-LLZTO/Li symmetrical cell can cycle stably for more than 400 h at a high current density of 400 μA cm−2, with the voltage polarization of only about 25 mV, and can withstand a larger current density of 600 μA cm−2 without the polarization exceeding 50 mV. These results demonstrate the feasibility of in situ lithiation of porous iron sulfide into a mixed ion/electron conductive layer as a solid-state garnet interface modification strategy and provide the new interface method for the development of high-performance solid-state lithium metal batteries.