Li_0.5La_0.5TiO₃ as an Ionic Conducting Additive Enhancing the High-Voltage Performance of LiNi_0.8Mn_0.1Co_0.1O₂ Cathodes in Lithium-Ion Batteries

Although high-voltage (e.g., >4.3 V_vsLi) operation can increase specific capacity and energy of Ni-rich NMC cathodes, it accelerates the oxidative decomposition of electrolytes and surface degradation of NMC cathodes, leading to rapid capacity fading. This work presents a novel approach that employs Li_0.5La_0.5TiO₃ (LLTO) solid-electrolyte as a Li-ion conductor and surface passivation agent to stabilize the cathode/electrolyte interphase (CEI) layer of the LiNi_0.8Mn_0.1Co_0.1O₂ (NMC811) cathode and enhance its high-voltage performances. The LLTO particles improve Li-ion transportation across the CEI layer, as evidenced by its reduced impedance in Nyquist plots. Furthermore, passivation of CEI by LLTO mitigates parasitic reactions (e.g., transition metal dissolution) that occur on the graphite solid electrolyte interphase layer during extended cycles of pouch-cells. As a result, pouch-cells with the 1 or 5 wt % LLTO-blended NMC811 cathodes can deliver 19-23% increase in specific capacity and improved cycle life (1000 cycles) at high voltages (up to 4.4 V), comparing to bare NMC811 cathodes. Post-mortem characterization of pouch-cells quantitatively identified the degradation sources of NMC811 cathode at high-voltages, which highlighted the improvement mechanisms of LLTO blended-cathodes.