Improvement of the Electrochemical Performance of LiNi_0.8Co_0.1Mn_0.1O₂ via Atomic Layer Deposition of Lithium-Rich Zirconium Phosphate Coatings

Owing to its high energy density, LiNi0.8Co0.1Mn0.1O2 (NMC811) is a cathode material of prime interest for electric vehicle battery manufacturers. However, NMC811 suffers from several irreversible parasitic reactions that lead to severe capacity fading and impedance buildup during prolonged cycling. Thin surface protection films coated on the cathode material mitigate degradative chemomechanical reactions at the electrode–electrolyte interphase, which helps to increase cycling stability. However, these coatings may impede the diffusion of lithium ions, and therefore, limit the performance of the cathode material at a high C-rate. Herein, we report on the synthesis of zirconium phosphate (ZrxPOy) and lithium-containing zirconium phosphate (LixZryPOz) coatings as artificial cathode–electrolyte interphases (ACEIs) on NMC811 using the atomic layer deposition technique. Upon prolonged cycling, the ZrxPOy- and LixZryPOz-coated NMC811 samples show 36.4 and 49.4% enhanced capacity retention, respectively, compared with the uncoated NMC811. Moreover, the addition of Li ions to the LixZryPOz coating enhances the rate performance and initial discharge capacity in comparison to the ZrxPOy-coated and uncoated samples. Using online electrochemical mass spectroscopy, we show that the coated ACEIs largely suppress the degradative parasitic side reactions observed with the uncoated NMC811 sample. Our study demonstrates that providing extra lithium to the ACEI layer improves the cycling stability of the NMC811 cathode material without sacrificing its rate capability performance.