Stabilizing the cationic/anionic redox chemistry of Li-rich layered cathodes by tuning the upper cut-off voltage for high energy-density lithium-ion batteries

Peiyu Hou, Feng Li, Haiyan Zhang, Haitao Huang

Research output: Journal article publicationJournal articleAcademic researchpeer-review

7 Citations (Scopus)

Abstract

Cumulative cationic/anionic redox reactions boost the reversible capacity of Li-rich layered oxides (LLOs) to 300 mA h g-1. However, the voltage/capacity fade is a major obstacle to the application of LLOs in lithium-ion batteries (LIBs). Here a paradigm shift toward tuning the charging voltages, namely a low upper cut-off voltage of 4.5 V (vs. Li/Li+) after an initial activation at 4.6 V, is proposed and the effects of cut-off voltages (4.8 V and 4.5 V) on the stability of cationic/anionic redox chemistries along with structural evolution are also revealed. It is demonstrated that the reversibility of cationic/anionic redox processes can be significantly improved at the low cut-off voltage compared with that at 4.8 V. The structural transitions from the layered to the rock-salt phase along with the valence decrease of Mn ions are consequently mitigated. As a result, the LLOs exhibit a very low capacity/voltage fade of only 4.8%/7.8% after 200 cycles at 0.5C and superior rate capability (195 mA h g-1 at 5C). Additionally, full cells composed of the LLO cathode and a mesocarbon microbead anode show a high energy density exceeding 300 W h kg-1 and improved cycling/voltage stability. This strategy provides a simple and efficient method to stabilize the cationic/anionic redox chemistries of LLOs and thus promotes their practical applications in high energy-density LIBs. This journal is

Original languageEnglish
Pages (from-to)14214-14222
Number of pages9
JournalJournal of Materials Chemistry A
Volume8
Issue number28
DOIs
Publication statusPublished - 28 Jul 2020

ASJC Scopus subject areas

  • Chemistry(all)
  • Renewable Energy, Sustainability and the Environment
  • Materials Science(all)

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