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Title: Achieving Thermodynamic Stability of Single-Crystal Co-Free Ni-Rich Cathode Material for High Voltage Lithium-Ion Batteries

Abstract

Abstract Ni‐rich layered cathode materials are progressively considered as the standard configuration of high‐energy electric vehicles by virtues of their high capacity and eliminated “range anxiety.” However, the poor cyclic stability and severe cobalt supply crisis would restrain their wide commercial applicability. Here, a cost‐effective single‐crystal Co‐free Ni‐rich cathode material LiNi 0.8 Mn 0.18 Fe 0.02 O 2 (NMF), which outperforms widely commercial polycrystalline LiNi 0.83 Co 0.11 Mn 0.06 O 2 (MNCM) and single‐crystal LiNi 0.83 Co 0.11 Mn 0.06 O 2 (SNCM) is reported. Surprisingly, NMF can compensate for the reversible capacity loss under the designed conditions of high‐temperature and elevated‐voltage, achieving a competitive energy density compared with conventional MNCM or SNCM. Combining operando characterizations and density functional theory calculation, it is revealed that NMF cathode with improved dynamic structure evolution largely alleviates the mechanical strain issue commonly found in Ni‐rich cathode, which can reduce the formation of intragranular cracks and improve the safety performance. Consequently, this new Co‐free NMF cathode can achieve a perfect equilibrium between material cost and electrochemical performance, which not only reduces the production cost by >15%, but also demonstrates excellent thermal stability and cycling performance..

Authors:
 [1];  [2];  [3];  [1];  [1];  [3];  [3];  [3];  [3]; ORCiD logo [4];  [1]
  1. Central South University, Changsha (China)
  2. Central South University, Changsha (China); Zhejiang Power New Energy Co. Ltd., Zhuji (China)
  3. Argonne National Laboratory (ANL), Argonne, IL (United States)
  4. Argonne National Laboratory (ANL), Argonne, IL (United States); Imam Abdulrahman Bin Faisal University (IAU), Dammam (Saudi Arabia). Institute for Research & Medical Consultations (IRMC); Stanford Univ., CA (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
Sponsoring Org.:
USDOE Office of Science (SC); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); National Natural Science Foundation of China (NSFC); US Army Research Laboratory (USARL)
OSTI Identifier:
2310342
Alternate Identifier(s):
OSTI ID: 1983547
Grant/Contract Number:  
AC02-06CH11357; 52070194; 51902347; 51908555; 51822812
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Functional Materials
Additional Journal Information:
Journal Volume: 33; Journal Issue: 23; Journal ID: ISSN 1616-301X
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Co-free Ni-rich cathode; single-crystals; thermal stability; reduced materials costs

Citation Formats

Shen, Jixue, Zhang, Bao, Huang, Weiyuan, Li, Xiao, Xiao, Zhiming, Wang, Jing, Zhou, Tao, Wen, Jianguo, Liu, Tongchao, Amine, Khalil, and Ou, Xing. Achieving Thermodynamic Stability of Single-Crystal Co-Free Ni-Rich Cathode Material for High Voltage Lithium-Ion Batteries. United States: N. p., 2023. Web. doi:10.1002/adfm.202300081.
Shen, Jixue, Zhang, Bao, Huang, Weiyuan, Li, Xiao, Xiao, Zhiming, Wang, Jing, Zhou, Tao, Wen, Jianguo, Liu, Tongchao, Amine, Khalil, & Ou, Xing. Achieving Thermodynamic Stability of Single-Crystal Co-Free Ni-Rich Cathode Material for High Voltage Lithium-Ion Batteries. United States. https://doi.org/10.1002/adfm.202300081
Shen, Jixue, Zhang, Bao, Huang, Weiyuan, Li, Xiao, Xiao, Zhiming, Wang, Jing, Zhou, Tao, Wen, Jianguo, Liu, Tongchao, Amine, Khalil, and Ou, Xing. Wed . "Achieving Thermodynamic Stability of Single-Crystal Co-Free Ni-Rich Cathode Material for High Voltage Lithium-Ion Batteries". United States. https://doi.org/10.1002/adfm.202300081. https://www.osti.gov/servlets/purl/2310342.
@article{osti_2310342,
title = {Achieving Thermodynamic Stability of Single-Crystal Co-Free Ni-Rich Cathode Material for High Voltage Lithium-Ion Batteries},
author = {Shen, Jixue and Zhang, Bao and Huang, Weiyuan and Li, Xiao and Xiao, Zhiming and Wang, Jing and Zhou, Tao and Wen, Jianguo and Liu, Tongchao and Amine, Khalil and Ou, Xing},
abstractNote = {Abstract Ni‐rich layered cathode materials are progressively considered as the standard configuration of high‐energy electric vehicles by virtues of their high capacity and eliminated “range anxiety.” However, the poor cyclic stability and severe cobalt supply crisis would restrain their wide commercial applicability. Here, a cost‐effective single‐crystal Co‐free Ni‐rich cathode material LiNi 0.8 Mn 0.18 Fe 0.02 O 2 (NMF), which outperforms widely commercial polycrystalline LiNi 0.83 Co 0.11 Mn 0.06 O 2 (MNCM) and single‐crystal LiNi 0.83 Co 0.11 Mn 0.06 O 2 (SNCM) is reported. Surprisingly, NMF can compensate for the reversible capacity loss under the designed conditions of high‐temperature and elevated‐voltage, achieving a competitive energy density compared with conventional MNCM or SNCM. Combining operando characterizations and density functional theory calculation, it is revealed that NMF cathode with improved dynamic structure evolution largely alleviates the mechanical strain issue commonly found in Ni‐rich cathode, which can reduce the formation of intragranular cracks and improve the safety performance. Consequently, this new Co‐free NMF cathode can achieve a perfect equilibrium between material cost and electrochemical performance, which not only reduces the production cost by >15%, but also demonstrates excellent thermal stability and cycling performance..},
doi = {10.1002/adfm.202300081},
journal = {Advanced Functional Materials},
number = 23,
volume = 33,
place = {United States},
year = {Wed Mar 15 00:00:00 EDT 2023},
month = {Wed Mar 15 00:00:00 EDT 2023}
}

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