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Progress in Chemistry 2020, Vol. 32 Issue (10): 1504-1514 DOI: 10.7536/PC200220 Previous Articles   Next Articles

Special Issue: 锂离子电池

Enhancing the Stability of Lithium-Rich Manganese-Based Layered Cathode Materials for Li-Ion Batteries Application

Zhiyuan Lu1, Yanni Liu1, Shijun Liao1,**()   

  1. 1. The Key Laboratory of Fuel Cells Technology of Guangdong Province, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510641, China
  • Received: Revised: Online: Published:
  • Contact: Shijun Liao
  • About author:
    **e-mail:
  • Supported by:
    National Key Research and Development Program of China(2017YFB0102900); National Key Research and Development Program of China(2016YFB0101201); National Natural Science Foundation of China(21476088); National Natural Science Foundation of China(21776104); Guangdong Provincial Department of Science and Technology(2015B010106012); Guangzhou Science Technology and Innovation Committee(201504281614372); Guangzhou Science Technology and Innovation Committee(2016GJ006)
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Lithium-rich manganese-based layered cathode materials (xLi2MnO3·(1-x)LiMO2, M=Ni, Co, Mn, etc.), owing to their high specific capacity (≥ 250 mAh·g-1), low cost and environmental friendliness, are considered as one of the best candidate cathode materials for the new generation of lithium-ion batteries. However, these materials suffer from severe capacity/voltage fading during the cycle process and low rate capability which seriously hinder commercial development. In this paper, we analyze the structural characteristics and the reasons which lead to the deterioration of the electrochemical performance of the lithium-rich manganese-based layered cathode materials, systematically review the latest progress and achievements on improving the stability of the cathode materials, and the efforts to improve the electrochemical properties of the cathode materials through bulk doping and surface modification. In this process, the effects of bulk doping at different sites and different coating materials on the structure and electrochemical behavior of lithium-rich manganese-based layered cathode materials are further analyzed. Finally, considering the advantages and disadvantages of the two modification methods of bulk doping and surface coating, a joint modification mechanism combining bulk doping and surface coating has been suggested to improve the stability of lithium-rich cathode materials in the long cycle process, and the introduction and prospect of this mechanism are also given.

Contents

1 Introduction

2 Structural characteristic and electrochemical behaviors of lithium-rich manganese-based materials

2.1 Lithium-rich manganese-based materials and its structural characteristic

2.2 Charge-discharge reaction mechanism

2.3 Structural evolution and decay mechanism

3 Bulk doping improves the cycle stability of lith- ium-rich manganese-based materials

3.1 Li site doping

3.2 TM site doping

3.3 O site doping

4 Surface modification improves the cycle stability of lithium-rich manganese-based materials.

4.1 Surface coating

4.2 Surface treatment

5 A joint mechanism

6 Conclusion and outlook

Key words: lithium-rich manganese-based layered cathode materials, cycle stability, bulk doping, surface modification
Fig.1 Crystal structures and XRD of the (a) LiTMO2, (b) Li2MnO3-like, (c) LLi1+xNiaCobMnc[26,27,28,29,30]; (d) Aberration-corrected scanning transmission electron microscopy (STEM) image of the Li[Li0.2Ni0.2Mn0.6]O2 crystal[31]
Fig.2 Lithium-rich manganese-based layered cathode materials (a) galvanostatic charge-discharge voltage profiles measured at 0.1 C, (b) differential capacity (dQ/dV vs E) plots obtained from voltage profiles[48]
Fig.3 (a) The participation degree of different layered oxides in lattice oxygen during the electrochemical reaction process[42]. (b) Schematic of local atomic coordination and electron band structure of Li-excess cathodes, that enables the anionic redox reaction[50]
Fig.4 The mechanism of the lithium-rich layered cathode materials change during the cycle[60]
Fig.5 (a, b) The charge-discharge curves of the unmodified anode material (PLR) and modified anode material (SLR) at 0.1 C, respectively. (c, e) the charge-discharge curves and cycling stability tested at 0.2 C and (d) rate performance of PLR and SLR[68]
Fig.6 Illustration of the C-coating[78]
Table 1 Electrochemical performance of typical modification research works about lithium-rich manganese-based layered cathode materials in recent years
Molecular formula Classification Electrochemical property ref
Capacity retention Rate capacity (mAh·g-1)
Li1.2Mn0.54Ni0.13Co0.13O2 Li site doping 76%→95% (100 cycles) 180→210 at 500 mA·g-1 67
Li1.2Mn0.54Ni0.13Co0.13O2 Li site doping 65%→71% (300 cycles) 81→136 at 1500 mA·g-1 69
Li1.5Mn0.675Ni0.1675Co0.1675O2 TM site doping 78%→ 82% (150 cycles) 65→120 at 5000 mA·g-1 70
Li1.133Mn0.467Ni0.2Co0.2O2 O site doping 83%→97% (50 cycles) 212→236 at 25 mA·g-1 72
SQ〗0.33Li2MnO3·0.67Li
[Mn1/3Ni1/3Co1/3]O2		 C-coating 50%→69% (50 cycles) 75→234 at 2500 mA·g-1 79
Li1.256Ni0.198Co0.082Mn0.689O2.25 Al2O3-coating 82%→95% (60 cycles) 123→189 at 250 mA·g-1 81
Li1.3Mn4/6Ni1/6Co1/6O2.4 AlF3-coating 81%→91% (50 cycles) 53→80 at 1250 mA·g-1 82
Li1.15Ni0.7Co0.11Mn0.57O2 AlPO4-coating 85%→90% (100 cycles) 198→202 at 250 mA·g-1 85
SQ〗0.35Li2MnO3·0.65Li
Ni0.35Mn0.45Co0.20O2		 NH3 heat treatment 89%→ 94% (60 cycles) 163→183 at 1000 mA·g-1 90
Li1.2Mn0.54Ni0.13Co0.13O2 C-coating
& F-doping		 57%→ 89% (500 cycles) 33.3→108.6 at 2500 mA·g-1 92
Li1.20Mn0.54Ni0.13Co0.13O2 ZrF4-coating
& Mo-Doping		 87%→92% (100 cycles) 95.2→117.1 at 1250 mA·g-1 93
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