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Title: Cooling Induced Surface Reconstruction during Synthesis of High-Ni Layered Oxides

Journal Article · · Advanced Energy Materials
ORCiD logo [1];  [2];  [3];  [4];  [3];  [5];  [6];  [6];  [6];  [7];  [8];  [9];  [2];  [6];  [6]; ORCiD logo [3];  [10]
  1. Peking Univ., Beijing (China); Brookhaven National Lab. (BNL), Upton, NY (United States). Sustainable Energy Technologies Dept.
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Science Dept.
  3. Peking Univ., Beijing (China)
  4. Peking Univ., Beijing (China); Brookhaven National Lab. (BNL), Upton, NY (United States). Sustainable Energy Technologies Dept.; Hebei Univ. of Technology, Tianjing (China)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States); Chinese Academy of Sciences (CAS), Ningbo (China). Ningbo Inst. of Materials Technology and Engineering
  6. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source
  7. Cornell Univ., Ithaca, NY (United States). Cornell High Energy Synchrotron Source
  8. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division; Stanford Univ., CA (United States). Materials Science and Engineering; Imam Abdulrahman Bin Faisal Univ. (IAU), Dammam (Saudi Arabia)
  9. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  10. Brookhaven National Lab. (BNL), Upton, NY (United States). Sustainable Energy Technologies Dept.
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Transition metal layered oxides have been the dominant cathodes in lithiumion batteries, and among them, high-Ni ones (LiNixMnyCozO2; x ≥ 0.7) with greatly boosted capacity and reduced cost are of particular interest for largescale applications. The high Ni loading, on the other hand, raises the critical issues of surface instability and poor rate performance. The rational design of synthesis leading to layered LiNi0.7Mn0.15Co0.15O2 with greatly enhanced rate capability is demonstrated, by implementing a quenching process alternative to the general slow cooling. In situ synchrotron X-ray diffraction, coupled with surface analysis, is applied to studies of the synthesis process, revealing cooling-induced surface reconstruction involving Li2CO3 accumulation, formation of a Li-deficient layer and Ni reduction at the particle surface. The reconstruction process occurs predominantly at high temperatures (above 350 °C) and is highly cooling-rate dependent, implying that surface reconstruction can be suppressed through synthetic control, i.e., quenching to improve the surface stability and rate performance of the synthesized materials. These findings may provide guidance to rational synthesis of high-Ni cathode materials.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES); Brookhaven National Laboratory (BNL); South University of Science and Technology of China (SUSTC)
Grant/Contract Number:
SC0012704; AC02‐06CH11357; AC02-06CH11357
OSTI ID:
1574924
Alternate ID(s):
OSTI ID: 1570394; OSTI ID: 1763743
Report Number(s):
BNL-212356-2019-JAAM; BNL-212443-2019-JAAM; TRN: US2001072
Journal Information:
Advanced Energy Materials, Vol. 9, Issue 43; ISSN 1614-6832
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 34 works
Citation information provided by
Web of Science

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Cited By (1)

Using in situ and operando methods to characterize phase changes in charged lithium nickel cobalt aluminum oxide cathode materials journal January 2020

Figures / Tables (5)

Scheme 1(p. 4)figure Scheme 1
Figure 1(p. 5)figure Figure 1
Figure 2(p. 7)figure Figure 2
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Related Subjects

25 ENERGY STORAGE
high‐Ni layered oxide cathodes
lithium‐ion batteries
quenching
solid‐state synthesis
surface reconstruction