Lattice engineering of high-entropy olivine-type lithium metal phosphate as high-voltage cathodes

Engineering of high-entropy cathode materials for lithium-ion batteries has been actively pursued owing to the outstanding conductivity of high-entropy materials benefited from the maximum entropy and unique antisite disordering structure. Olivine lithium metal phosphates such as LiMnPO4 and LiNiPO4 feature high working voltages but low capacities due to their insulation nature. In this work, the synthesis of the high-entropy lithium metal phosphate materials (HELMPs) is realized by combining mechanochemistry with a calcination method. By regulating lattice of HELMPs, the high-entropy Li(Mn0.35Fe0.35Co0.1Mg0.1Ca0.1)PO4 reveals three typical high-voltage plateaus in charge-discharge curves corresponding to the redox of Fe, Mn, and Co in the voltage range of 2.0-4.9 V vs Li+/Li, and a much higher initial capacity than LiMnPO4 (104 vs 15 mAh g-1).