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.
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