Lattice and Local Electronic Structure Modulation Enables Ultra-Long-Life Li-Rich Cathode Materials

Abstract

Effectively alleviating severe performance deterioration including rapid capacity decay and continuous voltage fading of Li-rich layered oxide (LLO) cathodes by suppressing the irreversible oxygen release and transition metal (TM) migration is a critical challenge during prolonged cycling. Herein, we report a Sb-doped LLO (SLLO) cathode with shortened TMoct–TMoct distance and modulated local electronic structure, which can significantly enhance the oxygen vacancy formation energy and TM migration energy barriers. Therefore, the SLLO cathode showcases an impressive energy density of 1052 Wh kg–1 at 0.2 C and an outstanding rate capability of 214 mAh g–1 at 5 C with a remarkable capacity retention of 79.2% even after 1000 cycles. It should be pointed out that it exhibits greatly enhanced voltage stability with an outstanding voltage retention of 86.2% after cycling 1600 times at 10 C. This work provides a prototype for significantly enhancing the reversibility in electrochemical reactions of high-capacity layered cathode materials.