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Solid‐State Reaction Heterogeneity During Calcination of Lithium‐Ion Battery Cathode

Journal Article · · Advanced Materials
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  1. Department of Chemistry Seoul National University 1 Gwanak‐ro, Gwanak‐gu Seoul 08826 Republic of Korea
  2. Department of Materials Science and Engineering Yonsei University Seoul 120‐749 Republic of Korea
  3. Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo Park CA 94025 USA
  4. Department of Chemistry Seoul National University 1 Gwanak‐ro, Gwanak‐gu Seoul 08826 Republic of Korea; Department of Materials Science &, Engineering and Research Institute of Advanced Materials (RIAM) Seoul National University 1 Gwanak‐ro, Gwanak‐gu Seoul 08826 Republic of Korea
  5. School of Energy and Environment City University of Hong Kong Hong Kong Hong Kong SAR P. R. China
  6. Materials Research Division Research Institute of Industrial Science and Technology (RIST) Pohang 37673 Republic of Korea
  7. Department of Materials Science &, Engineering and Research Institute of Advanced Materials (RIAM) Seoul National University 1 Gwanak‐ro, Gwanak‐gu Seoul 08826 Republic of Korea

Abstract

During solid‐state calcination, with increasing temperature, materials undergo complex phase transitions with heterogeneous solid‐state reactions and mass transport. Precise control of the calcination chemistry is therefore crucial for synthesizing state‐of‐the‐art Ni‐rich layered oxides (LiNi1‐x‐yCoxMnyO2, NRNCM) as cathode materials for lithium‐ion batteries. Although the battery performance depends on the chemical heterogeneity during NRNCM calcination, it has not yet been elucidated. Herein, through synchrotron‐based X‐ray, mass spectrometry microscopy, and structural analyses, it is revealed that the temperature‐dependent reaction kinetics, the diffusivity of solid‐state lithium sources, and the ambient oxygen control the local chemical compositions of the reaction intermediates within a calcined particle. Additionally, it is found that the variations in the reducing power of the transition metals (i.e., Ni, Co, and Mn) determine the local structures at the nanoscale. The investigation of the reaction mechanism via imaging analysis provides valuable information for tuning the calcination chemistry and developing high‐energy/power density lithium‐ion batteries.

Research Organization:
SLAC National Accelerator Laboratory, Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC02-76SF00515
OSTI ID:
2423931
Journal Information:
Advanced Materials, Journal Name: Advanced Materials Journal Issue: 10 Vol. 35; ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English

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