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Title: Revealing the Atomic Origin of Heterogeneous Li-Ion Diffusion by Probing Na

Journal Article · · Advanced Materials
 [1];  [2];  [3];  [1];  [3];  [4];  [1];  [2];  [1];  [3];  [2];  [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Beijing Univ. of Technology, Beijing (China)
  3. Argonne National Lab. (ANL), Lemont, IL (United States)
  4. Argonne National Lab. (ANL), Lemont, IL (United States); Stanford Univ., Stanford, CA (United States)

Tracing the dynamic process of Li-ion transport at the atomic scale has long been attempted in solid state ionics and is essential for battery material engineering. Approaches via phase change, strain, and valence states of redox species have been developed to circumvent the technical challenge of direct imaging Li; however, all are limited by poor spatial resolution and weak correlation with state-of-charge (SOC). An ion-exchange approach is adopted by sodiating the delithiated cathode and probing Na distribution to trace the Li deintercalation, which enables the visualization of heterogeneous Li-ion diffusion down to the atomic level. In a model LiNi1/3Mn1/3Co1/3O2 cathode, dislocation-mediated ion diffusion is kinetically favorable at low SOC and planar diffusion along (003) layers dominates at high SOC. These processes work synergistically to determine the overall ion-diffusion dynamics. Here, the heterogeneous nature of ion diffusion in battery materials is unveiled and the role of defect engineering in tailoring ion-transport kinetics is stressed.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
National Natural Science Foundation of China (NSFC); National Key Research and Development Program of China; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V). Battery Materials Research (BMR) Program; USDOE Office of Electricity (OE)
Grant/Contract Number:
AC02-06CH11357; 70247A; AC02‐06CH11357
OSTI ID:
1559944
Alternate ID(s):
OSTI ID: 1523674
Journal Information:
Advanced Materials, Vol. 31, Issue 29; ISSN 0935-9648
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 29 works
Citation information provided by
Web of Science

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Cited By (1)

Charge distribution guided by grain crystallographic orientations in polycrystalline battery materials journal January 2020