Sustainable Interfaces between Si Anodes and Garnet Electrolytes for Room-Temperature Solid-State Batteries

Solid-state batteries (SSBs) have seen a resurgence of research interests in recent years for their potential to offer high energy density and excellent safety far beyond current commercialized lithium-ion batteries. The compatibility of Si anodes and Ta-doped Li₇La₃Zr₂O₁₂ (Li_6.4La₃Zr_1.4Ta_0.6O₁₂, LLZTO) solid electrolytes and the stability of the Si anode have been investigated. It is found that Si layer anodes thinner than 180 nm can maintain good contact with the LLZTO plate electrolytes, leading the Li/LLZTO/Si cells to exhibit excellent cycling performance with a capacity retention over 85% after 100 cycles. As the Si layer thickness is increased to larger than 300 nm, the capacity retention of Li/LLZTO/Si cells becomes 77% after 100 cycles. When the thickness is close to 900 nm, the cells can cycle only for a limited number of times because of the destructive volume change at the interfaces. Because of the sustainable Si/LLZTO interfaces with the Si layer anodes with a thickness of 180 nm, full cells with the LiFePO₄ cathodes show discharge capacities of 120 mA h g^-1 for LiFePO₄ and 2200 mA h g^-1 for the Si anodes at room temperature. They cycle 100 times with a capacity retention of 72%. These results indicate that the combination between the Si anodes and the garnet electrolytes is a promising strategy for constructing high-performance SSBs.