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.

Highlights

  • Electric energy storage technologies have been recognized as a powerful solution contributing to the alleviation of the environmental burden [1,2,3]

  • Two types of prelithiation processes were applied to hard carbon (HC) negative electrode (NE), after which the nickel cobalt manganese oxides (NCM)/prelithiated

  • HC full-cells were assembled with CR2032-type coin cells

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Summary

Introduction

Electric energy storage technologies have been recognized as a powerful solution contributing to the alleviation of the environmental burden [1,2,3]. Lithium-ion batteries (LIBs) have recently gained attention for their application as secondary batteries and large-scale energy storage systems (electric vehicles, output leveling of renewable energy, and so on) [4,5,6]. LIBs are generally composed of a positive electrode (PE, alternatively called cathode) of lithium transition metal oxides and a negative electrode (NE, alternatively termed as anode) of carbonaceous materials. PE active material of lithium nickel cobalt manganese oxides (NCM) has the superior features of high electropositive potential, high Li-ion insertion-extraction specific capacity, and reduced cost, when compared to other cobalt-type PE active materials [4,7]. The specific capacity of NCM active materials is dependent on the composition of nickel (Ni), cobalt (Co), and manganese (Mn). Heightening the Ni content can increase the specific capacity of NCM active materials

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