Improving the long-term electrochemical performances of Li-rich cathode material by encapsulating a three-in-one nanolayer

Abstract

With large specific capacity, wide voltage window, and high energy density, Li-rich layered oxides have been considered as a promising cathode candidate for advanced lithium-ion batteries (LIBs). However, their commercial application is challenging due to severe capacity degradation and voltage fading caused by irreversible oxygen evolution and phase transition upon repeated cycling. This work proposes an effective strategy to improve the long-term electrochemical performances of Li_1.2Mn_0.56Ni_0.17Co_0.07O₂ (LMNCO) by constructing multifunctional nanolayers composed of element-doping, layered-spinel heterostructural connection, and fast ion conductor shell via a facile method. The Li_0.09B_0.97PO₄ (LBPO) coating shell acts as a fast ion carrier and physical screen to promote Li⁺ diffusion and isolate side reactions at the cathode-electrolyte interface; moreover, two-phase transitional region provides three-dimensional channel to facilitate Li⁺ transport and inhibit phase transition. Besides, B³⁺ and PO₄³⁻-doping collaborates with oxygen vacancies to stabilize lattice oxygen and restrain oxygen evolution from the bulk active cathode. The optimized LMNCO@LBPO material exhibits a superior capacity retention of 78.6%, higher than that of the pristine sample (49.3%), with the mitigated voltage fading of 0.73 mV per cycle after 500 cycles at 1 C. This study opens up an avenue for the surface modification to the electrochemical properties and perspective application of Li-rich cathodes in high-performance LIBs.