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

Abstract

Tracing the dynamic process of Li-ion transport at the atomic scale is a long-cherished wish in solid state ionics and essential for battery material engineering. Approaches via phase change, strain, and valence states of redox species are 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). Here, we adopt an ion-exchange approach by sodiating the de-lithiated cathode and probing Na distribution to trace the Li de-intercalation, which enables us to visualize the heterogeneous Li-ion diffusion down to atomic level. In the 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, which work synergistically to determine the ion diffusion dynamics. Our work unveils the heterogeneous nature of ion diffusion in battery material and stresses the role of defect engineering in tailoring ion transport kinetics.

Authors:
 [1];  [2];  [3];  [1];  [4];  [4];  [1];  [2];  [1];  [4];  [2];  [1]
  1. BATTELLE (PACIFIC NW LAB)
  2. Beijing Institute of Technology
  3. ARGONNE NATL LAB
  4. Argonne National Laboratory
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1571506
Report Number(s):
PNNL-SA-137695
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 29
Country of Publication:
United States
Language:
English

Citation Formats

Xiao, Biwei, Wang, Kuan, Xu, Gui-Liang, Song, Junhua, Chen, Zonghai, Amine, Khalil, Reed, David M., Sui, Manling, Sprenkle, Vincent L., Ren, Yang, Yan, Pengfei, and Li, Xiaolin. Revealing the Atomic Origin of Heterogeneous Li-Ion Diffusion by Probing Na. United States: N. p., 2019. Web. doi:10.1002/adma.201805889.
Xiao, Biwei, Wang, Kuan, Xu, Gui-Liang, Song, Junhua, Chen, Zonghai, Amine, Khalil, Reed, David M., Sui, Manling, Sprenkle, Vincent L., Ren, Yang, Yan, Pengfei, & Li, Xiaolin. Revealing the Atomic Origin of Heterogeneous Li-Ion Diffusion by Probing Na. United States. doi:10.1002/adma.201805889.
Xiao, Biwei, Wang, Kuan, Xu, Gui-Liang, Song, Junhua, Chen, Zonghai, Amine, Khalil, Reed, David M., Sui, Manling, Sprenkle, Vincent L., Ren, Yang, Yan, Pengfei, and Li, Xiaolin. Mon . "Revealing the Atomic Origin of Heterogeneous Li-Ion Diffusion by Probing Na". United States. doi:10.1002/adma.201805889.
@article{osti_1571506,
title = {Revealing the Atomic Origin of Heterogeneous Li-Ion Diffusion by Probing Na},
author = {Xiao, Biwei and Wang, Kuan and Xu, Gui-Liang and Song, Junhua and Chen, Zonghai and Amine, Khalil and Reed, David M. and Sui, Manling and Sprenkle, Vincent L. and Ren, Yang and Yan, Pengfei and Li, Xiaolin},
abstractNote = {Tracing the dynamic process of Li-ion transport at the atomic scale is a long-cherished wish in solid state ionics and essential for battery material engineering. Approaches via phase change, strain, and valence states of redox species are 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). Here, we adopt an ion-exchange approach by sodiating the de-lithiated cathode and probing Na distribution to trace the Li de-intercalation, which enables us to visualize the heterogeneous Li-ion diffusion down to atomic level. In the 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, which work synergistically to determine the ion diffusion dynamics. Our work unveils the heterogeneous nature of ion diffusion in battery material and stresses the role of defect engineering in tailoring ion transport kinetics.},
doi = {10.1002/adma.201805889},
journal = {Advanced Materials},
number = 29,
volume = 31,
place = {United States},
year = {2019},
month = {7}
}

Works referenced in this record:

Challenges for Rechargeable Li Batteries
journal, February 2010

  • Goodenough, John B.; Kim, Youngsik
  • Chemistry of Materials, Vol. 22, Issue 3, p. 587-603
  • DOI: 10.1021/cm901452z

Lithium Batteries and Cathode Materials
journal, October 2004

  • Whittingham, M. Stanley
  • Chemical Reviews, Vol. 104, Issue 10, p. 4271-4302
  • DOI: 10.1021/cr020731c