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Single-Crystallization of O3-Type Layered Oxide Cathode for Na-Ion Battery

Journal Article · · Chemistry of Materials
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  1. Xiamen University (China)
  2. Argonne National Laboratory (ANL), Argonne, IL (United States)
  3. Huayou New Energy Technology (Quzhou) Co., LTD, Zhejiang (China)
  4. Contemporary Amperex Technology Co., Limited (CATL), Ningde (China)
  5. Brookhaven National Laboratory (BNL), Upton, NY (United States)
  6. Contemporary Amperex Technology Co., Ningde (China)
+ Show Author Affiliations
The development of high-energy-density Na-ion batteries places significant demands on single-crystal layered oxide cathodes, especially for further high-voltage, solid-state battery scenarios. In the O3-type structure, due to the original sluggish Na ion diffusion kinetics (approximately 1 order of magnitude lower than that of Li-ion), and further hindrance against diffusion kinetics caused by single-crystal architecture, these inherent defects lead to the decline in the electrochemical performance. Herein, we demonstrated that the single crystallization of O3-type NaNi1/3Fe1/3Mn1/3O2 cathode (d50 = 5.04 μm) aggravates surface-to-bulk phase inhomogeneity distribution, which is attributed to the uneven Na ions extraction. Moreover, the Na-depletion of the surface/shell region not only aggravates Na ion diffusion resistance but also leads to a higher valence state of transition-metal elements (e.g., Ni/Fe) near the surface of the single-crystal particle, which further compromises the cathode-electrolyte interface stability. Furthermore, not limited to revealing the challenges, tuning the particle size and moderating quasi-single-crystal strategies have been proven to effectively mitigate the negative uneven distributions of Na ions, phases, and valence/oxidative states, resulting in efficient modification for single crystallization of Na-layered oxide cathodes.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States); Brookhaven National Lab
Sponsoring Organization:
Brookhaven National Lab; Ministry of Science and Technology of China; Natural Science Foundation of China; USDOE Office of Science (SC); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-06CH11357; SC0012704
OSTI ID:
2587365
Alternate ID(s):
OSTI ID: 2589355
Report Number(s):
BNL-228949-2025-JAAM; 197674
Journal Information:
Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 15 Vol. 37; ISSN 1520-5002; ISSN 0897-4756
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

36 MATERIALS SCIENCE
Diffusion
Electrodes
Ions
Oxides
Phase transitions