Abstract

The irreversible evolution of oxygen for lithium-rich manganese-based cathode (LRMC) is the main challenge which will induce accelerated migration of transition metal ions and structural transformation, thus resulting in serious voltage attenuation and capacity decay. Herein, a facile and high-effective oxygen vacancy engineering of hydrogenation treatment is proposed for introducing oxygen vacancy on the surface of LRMC to suppress the irreversible evolution of oxygen. X-ray diffraction (XRD) Rietveld refinement, X-ray photoelectron spectroscopy and electron paramagnetic spectroscopy demonstrate the successful introduction of oxygen vacancy on the surface of LRMC. The changes of physicochemical properties of LRMC after hydrogenation treatment are investigated through systematical electrochemical performance tests and scanning electron microscopy and transmission electron microscopy. The investigative results reveal that the presence of oxygen vacancy can significantly improve the structural stability, electrical conductivity and Li+ diffusion kinetics of the LRMC materials. Especially, the optimized H500-LRMC shows excellent electrochemical performances including the enhanced cyclic stability with a capacity retention of 221.8 mAh g−1 and a capacity retention rate of 94.11% after 100 cycles. Therefore, the well-designed oxygen vacancy engineering through hydrogenation treatment is a promising strategy for the development and industrialization of the high-performance LRMC.

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