Constructing oxygen-deficient shell on Li-rich cathodes by spark plasma sintering for high-performance lithium-ion batteries

Abstract

Lithium-rich layered oxides (LROs) are considered as promising cathodes in building next-generation lithium-ion batteries (LIBs) with superior charge-discharge capacity. Nevertheless, LROs are confronted with irreversible oxygen loss accompanied with surface-to-bulk degradation upon cycling. To inhibit the oxygen release and to increase the lifespan of LROs, we report on an innovative strategy to rapidly construct an ultrathin oxygen-deficient shell layer covering the surface of LROs’ particles via a sparking plasma sintering (SPS) technique. It is demonstrated that the inner structure of the LROs’ particles is maintained, whereas the surface of the particles forms a thin shell (∼5 nm) consisting of a considerable amount of oxygen vacancies. Benefitting from the existence of an oxygen-deficient shell, the cathode activation is facilitated and the oxygen loss is suppressed, leading to enhanced capacity and prominent cyclability under long cycling. The modified LRO exhibits outstanding electrochemical performance, delivering a maximum capacity of 187.67 mAh g−1 and a capacity retention of 95.71% after 200 cycles at 250 mA g−1. Our work evidences that SPS is a fast and effective approach to construct oxygen-deficient shell on LRO cathodes for high-performance LIBs.

Keywords

• Lithium-rich layered oxides
• Lithium-ion batteries
• Surface modification
• Oxygen vacancies
• Cycling stability