Effect of Prelithiation Process for Hard Carbon Negative Electrode on the Rate and Cycling Behaviors of Lithium-Ion Batteries

Abstract

Two prelithiation processes (shallow Li-ion insertion, and thrice-repeated deep Li-ion insertion and extraction) were applied to the hard carbon (HC) negative electrode (NE) used in lithium-ion batteries (LIBs). LIB full-cells were assembled using Li(Ni0.5Co0.2Mn0.3)O2 positive electrodes (PEs) and the prelithiated HC NEs. The assembled full-cells were charged and discharged under a low current density, increasing current densities in a stepwise manner, and then constant under a high current density. The prelithiation process of shallow Li-ion insertion resulted in the high Coulombic efficiency (CE) of the full-cell at the initial charge-discharge cycles as well as in a superior rate capability. The prelithiation process of thrice-repeated Li-ion insertion and extraction attained an even higher CE and a high charge-discharge specific capacity under a low current density. However, both prelithiation processes decreased the capacity retention during charge-discharge cycling under a high current density, ascertaining a trade-off relationship between the increased CE and the cycling performance. Further elimination of the irreversible capacity of the HC NE was responsible for the higher utilization of both the PE and NE, attaining higher initial performances, but allowing the larger capacity to fade throughout charge-discharge cycling.