中国物理B ›› 2024, Vol. 33 ›› Issue (5): 58201-058201.doi: 10.1088/1674-1056/ad2a72

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Atomistic understanding of capacity loss in LiNiO2 for high-nickel Li-ion batteries: First-principles study

Shuai Peng(彭率)1,2, Li-Juan Chen(陈丽娟)1, Chang-Chun He(何长春)1, and Xiao-Bao Yang(杨小宝)1,2,†   

  1. 1 School of Physics and Optoelectronics, South China University of Technology, Guangzhou 510000, China;
    2 Center of Excellence for Advanced Materials, Dongguan 523808, China
  • 收稿日期:2023-12-19 修回日期:2024-02-09 接受日期:2024-02-19 出版日期:2024-05-20 发布日期:2024-05-20
  • 通讯作者: Xiao-Bao Yang E-mail:scxbyang@scut.edu.cn
  • 基金资助:
    Project supported by the Science Fund of the Guangdong Major Project of Basic and Applied Basic Research, China (Grant No. 2019B030302011) and the Fund of the Science and Technology Program of Guangzhou, China (Grant No. 202201010090).

Atomistic understanding of capacity loss in LiNiO2 for high-nickel Li-ion batteries: First-principles study

Shuai Peng(彭率)1,2, Li-Juan Chen(陈丽娟)1, Chang-Chun He(何长春)1, and Xiao-Bao Yang(杨小宝)1,2,†   

  1. 1 School of Physics and Optoelectronics, South China University of Technology, Guangzhou 510000, China;
    2 Center of Excellence for Advanced Materials, Dongguan 523808, China
  • Received:2023-12-19 Revised:2024-02-09 Accepted:2024-02-19 Online:2024-05-20 Published:2024-05-20
  • Contact: Xiao-Bao Yang E-mail:scxbyang@scut.edu.cn
  • Supported by:
    Project supported by the Science Fund of the Guangdong Major Project of Basic and Applied Basic Research, China (Grant No. 2019B030302011) and the Fund of the Science and Technology Program of Guangzhou, China (Grant No. 202201010090).

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摘要： Combining the first-principles calculations and structural enumeration with recognition, the delithiation process of LiNiO$_{2}$ is investigated, where various supercell shapes are considered in order to obtain the formation energy of Li$_{x}$NiO$_{2}$. Meanwhile, the voltage profile is simulated and the ordered phases of lithium vacancies corresponding to concentrations of 1/4, 2/5, 3/7, 1/2, 2/3, 3/4, 5/6, and 6/7 are predicted. To understand the capacity decay in the experiment during the charge/discharge cycles, deoxygenation and Li/Ni antisite defects are calculated, revealing that the chains of oxygen vacancies will be energetically preferrable. It can be inferred that in the absence of oxygen atom in high delithiate state, the diffusion of Ni atoms is facilitated and the formation of Li/Ni antisite is induced.

关键词: Li-ion battery, ground state, formation energy, oxygen vacancy, Li/Ni antisite

Abstract: Combining the first-principles calculations and structural enumeration with recognition, the delithiation process of LiNiO$_{2}$ is investigated, where various supercell shapes are considered in order to obtain the formation energy of Li$_{x}$NiO$_{2}$. Meanwhile, the voltage profile is simulated and the ordered phases of lithium vacancies corresponding to concentrations of 1/4, 2/5, 3/7, 1/2, 2/3, 3/4, 5/6, and 6/7 are predicted. To understand the capacity decay in the experiment during the charge/discharge cycles, deoxygenation and Li/Ni antisite defects are calculated, revealing that the chains of oxygen vacancies will be energetically preferrable. It can be inferred that in the absence of oxygen atom in high delithiate state, the diffusion of Ni atoms is facilitated and the formation of Li/Ni antisite is induced.

Key words: Li-ion battery, ground state, formation energy, oxygen vacancy, Li/Ni antisite

中图分类号:  (Lithium-ion batteries)

  • 82.47.Aa
63.20.dk (First-principles theory) 31.15.es (Applications of density-functional theory (e.g., to electronic structure and stability; defect formation; dielectric properties, susceptibilities; viscoelastic coefficients; Rydberg transition frequencies))