Stabilizing the Electrode/Electrolyte Interface of LiNi0.8Co0.15Al0.05O2 through Tailoring Aluminum Distribution in Microspheres as Long-Life, High-Rate, and Safe Cathode for Lithium-Ion Batteries

The unstable electrode/electrolyte interface of high-capacity LiNi0.8Co0.15Al0.05O2 (NCA) cathodes, especially at a highly delithiated state, usually leads to the transformation of layered to spinel and/or rock-salt phases, resulting in drastic capacity fade and poor thermal stability. Herein, the Al-increased and Ni-,Co-decreased electrode surface is fabricated through tailoring element distribution in micrometer-sized spherical NCA secondary particles via coprecipitation and solid-state reactions, aimed at stabilizing the electrode/electrolyte interface during continuous cycles. As expected, it shows much extended cycle life, 93.6% capacity retention within 100 cycles, compared with that of 78.5% for the normal NCA. It also delivers large reversible capacity of about 140 mAh g–1 even at 20 C, corresponding to energy density of around 480 Wh kg–1, which is enhanced by 45% compared to that of the normal NCA (about 330 Wh kg–1). Besides, the delayed heat emission temperature and reduced heat generation mean remarkably improved thermal stability. These foregoing improvements are ascribed to the Al-increased spherical secondary particle surface that stabilizes the electrode/electrolyte interface by protecting inner components from directly contacting with electrolyte and suppressing the side reaction on electrode surface between high oxidizing Ni4+ and electrolyte.