Developing a Double Protection Strategy for High-Performance Spinel LiNi0.5Mn1.5O4 Cathodes

LiNi0.5Mn1.5O4 is a promising cathode material with high-voltage and three-dimensional lithium-ion transport channels. Rapid capacity degradation due to HF corrosion has been a great challenge hindering the application of high-voltage cathode materials. Herein, a double protection strategy for high-performance LiNi0.5Mn1.5O4 cathodes has been designed using Li6.4La3Zr1.4Ta0.6O12 (LLZTO) with both high ionic conductivity and high surface basicity as the modifier of the poly(vinylidene fluoride) (PVDF) binder and the HF scavenger. It has been demonstrated that the modified PVDF binder possesses a higher Li+ diffusion coefficient than incipient PVDF, resulting in better overall electrochemical properties. Meanwhile, the result of first-principles calculations revealed that the reaction between HF and LLZTO has higher chemical reactivity than that between HF and LiNi0.5Mn1.5O4. The scanning electron microscopy images further confirmed that the insoluble byproducts produced by HF corrosion deposit on the surface of LLZTO particles only because of the high chemical reactivity between HF and LLZTO, while the LNMO particles are well preserved. The modified LNMO-LLZTO cathode presents better cycling stability (even at elevated temperature) and rate capability than the LNMO cathode. This work provides a novel design strategy for high-performance lithium-ion batteries.