Crack-free single-crystalline Co-free Ni-rich LiNi0.95Mn0.05O2 layered cathode

Ni Lianshan; Guo Ruiting; Fang Susu; Chen Jun; Gao Jinqiang; Mei Yu; Zhang Shu; Deng Wentao; Zou Guoqiang; Hou Hongshuai; Ji Xiaobo

doi:10.1016/j.esci.2022.02.006

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Jan. 2022

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Ni Lianshan, Guo Ruiting, Fang Susu, Chen Jun, Gao Jinqiang, Mei Yu, Zhang Shu, Deng Wentao, Zou Guoqiang, Hou Hongshuai, Ji Xiaobo. Crack-free single-crystalline Co-free Ni-rich LiNi0.95Mn0.05O2 layered cathode[J]. eScience, 2022, 2(1): 116-124. doi: 10.1016/j.esci.2022.02.006

Citation:

Ni Lianshan, Guo Ruiting, Fang Susu, Chen Jun, Gao Jinqiang, Mei Yu, Zhang Shu, Deng Wentao, Zou Guoqiang, Hou Hongshuai, Ji Xiaobo. Crack-free single-crystalline Co-free Ni-rich LiNi_0.95Mn_0.05O₂ layered cathode[J]. eScience, 2022, 2(1): 116-124. doi: 10.1016/j.esci.2022.02.006

Citation:

Ni Lianshan, Guo Ruiting, Fang Susu, Chen Jun, Gao Jinqiang, Mei Yu, Zhang Shu, Deng Wentao, Zou Guoqiang, Hou Hongshuai, Ji Xiaobo. Crack-free single-crystalline Co-free Ni-rich LiNi_0.95Mn_0.05O₂ layered cathode[J]. eScience, 2022, 2(1): 116-124. doi: 10.1016/j.esci.2022.02.006

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Crack-free single-crystalline Co-free Ni-rich LiNi_0.95Mn_0.05O₂ layered cathode

doi: 10.1016/j.esci.2022.02.006

State Key Laboratory of Powder Metallurgy, College of Chemistry and Chemical Engineering, Central South University, Changsha, Hunan, 410083, PR China

More Information

Corresponding author: Xiaobo Ji xji@csu.edu.cn
Received Date: 2021-12-14
Revised Date: 2022-01-14
Accepted Date: 2022-02-21

Available Online: 2022-03-02

Abstract

Abstract

The rapid growth in global electric vehicles (EVs) sales has promoted the development of Co-free, Ni-rich layered cathodes for state-of-the-art high energy-density, inexpensive lithium-ion batteries (LIBs). However, progress in their commercial use has been seriously hampered by exasperating performance deterioration and safety concerns. Herein, a robust single-crystalline, Co-free, Ni-rich LiNi_0.95Mn_0.05O₂ (SC-NM95) cathode is successfully designed using a molten salt-assisted method, and it exhibits better structural stability and cycling durability than those of polycrystalline LiNi_0.95Mn_0.05O₂ (PC-NM95). Notably, the SC-NM95 cathode achieves a high discharge capacity of 218.2 mAh g⁻¹, together with a high energy density of 837.3 Wh kg⁻¹ at 0.1 C, mainly due to abundant Ni²⁺/Ni³⁺ redox. It also presents an outstanding capacity retention (84.4%) after 200 cycles at 1 C, because its integrated single-crystalline structure effectively inhibits particle microcracking and surface phase transformation. In contrast, the PC-NM95 cathode suffers from rapid capacity fading owing to the nucleation and propagation of intergranular microcracking during cycling, facilitating aggravated parasitic reactions and rock-salt phase accumulation. This work provides a fundamental strategy for designing high-performance single-crystalline, Co-free, Ni-rich cathode materials and also represents an important breakthrough in developing high-safe, low-cost, and high-energy LIBs.
- Single-crystalline,
- Co-free Ni-rich cathodes,
- Intergranular microcracking,
- H2↔H3 phase transition,
- Cycling stability

● It provides insights into the fundamental design of high-performance single-crystalline Co-free Ni-rich cathodes.
● Single-crystalline Co-free Ni-rich LiNi_0.95Co_0.05O₂ cathode was firstly designed and systematically explored.
● The SC-NM95 cathode presents outstanding structural stability and cycling durability.
● The performance degradations of PC-NM95 were attributed to the microcracking formation and structural transformations.

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