Advantageous surface engineering to boost single-crystal quaternary cathodes for high-energy-density lithium-ion batteries

Hengtai Bai, Kai Yuan, Cheng Zhang, Wujiu Zhang, Xiaoyu Tang, Sainan Jiang, Ting Jin, Yue Ma, Liang Kou, Chao Shen, Keyu Xie

Research output: Contribution to journalArticlepeer-review

22 Scopus citations

Abstract

Single-crystalline Ni-rich cathode active materials (CAMs) are considered as promising candidates for high-energy-density lithium-ion batteries (LIBs) with favorable cycling stability and safety, due to their grain boundaryless characteristics efficiently alleviate the structural degradation of intergranular microcracks in poly-crystalline counterparts. However, their practical application not only suffers from sluggish Li diffusion kinetics, surface reconstruction and parasitic cathode/electrolyte interfacial reactions upon repeated cycling but also encounters chemical instability during storage and slurry processes. Herein, we constructed a uniform LiAlO2/Li3PO4 protective layer with gradient Al doping (LAP modification) on the surface of single-crystalline LiNi0.90Co0.05Mn0.04Al0.01O2 (SC[sbnd]NCMA) CAMs through an in situ modification process to relieve these intrinsic instability issues. This advantageous surface engineering significantly reduces Li+/Ni2+ mixing, inhibits parasitic side reactions and surface phase transformation, and notably improves Li+ diffusion kinetics. Therefore, LAP-modified SC[sbnd]NCMA exhibits superior cycling performance with a capacity retention of 74.4% at a high voltage of 4.5 V after 200 cycles at 1C compared to that of SC[sbnd]NCMA. Moreover, the enhancement of air storage properties after modification was further confirmed by the reduced surface residual lithium, improved rheological properties and well-maintained electrochemical performance. This work provides an effective strategy for the modification of single-crystal Ni-rich cathodes and further accelerates their practical application.

Original languageEnglish
Article number102879
JournalEnergy Storage Materials
Volume61
DOIs
StatePublished - Aug 2023

Keywords

  • Air instability
  • Ni-rich layered oxides
  • Practical application
  • Single-crystalline
  • Superior electrochemical performance
  • Surface engineering

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