A Full Oxide-Based Solid-State Lithium Battery and Its Unexpected Cathode Degradation Mechanism

Fabricating full oxide garnet type Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO)-based solid-state batteries has posed challenges, particularly in cosintering cathode composites. In this research, we achieve high-performance cathode composites through ultrafast cosintering, facilitated by residual lithium as a sintering agent under an O 2 atmosphere. These composites demonstrate compatibility with various cathode materials including LiCoO 2 and LiNi 1/3 Co 1/3 Mn 1/3 O 2 in an LLZTO-based composite. Significantly, our findings reveal that residual stress on the cathode active material plays a pivotal role in degradation during cycling. The rigid LLZTO framework constrains volume changes in the cathode material during (de)lithiation, leading to mechanical failure. This discovery challenges prior assumptions about the primary susceptibility of the cathode/electrolyte interface to electro-chemo-me…