Abstract

High-voltage Li2CoPO4F (∼5 V vs. Li/Li+) with double-layer surface coating has been successfully prepared for the first time. The Li3PO4-coated Li2CoPO4F shows a high reversible capacity of 154 mA h g−1 (energy density up to 700 W h kg−1) at 1 C current rate, and excellent rate capability (141 mA h g−1 at 20 C). XRD and MAS NMR results show that Li2CoPO4F can be indexed as an orthorhombic structure with space group Pnma and coexists with Li3PO4. The XPS depth profiles and TEM analysis reveal that the as-prepared material has a double-layer surface coating, with a carbon outer layer and a Li3PO4 inner layer, which greatly enhances the transfer kinetics of the lithium ions and electrons in the material and stabilizes the electrode/electrolyte interface. Using LiBOB as an electrolyte additive is another way to further stabilize the electrode/electrolyte interface, and the LiBOB has a synergistic effect with the Li3PO4 coating layer. In this way, the Li2CoPO4F cathode material exhibits excellent long-term cycling stability, with 83.8% capacity retention after 150 cycles. The excellent cycling performance is attributed to the LiBOB electrolyte additive and the Li3PO4 coating layer, both of which play an important role in stabilizing the charge transfer resistance of Li2CoPO4F upon cycling.

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