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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 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 LiNi 1/3Mn 1/3Co 1/3O 2 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.

Authors:
 [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)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Natural Science Foundation of China (NNSFC); 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 Delivery and Energy Reliability (OE)
OSTI Identifier:
1559944
Alternate Identifier(s):
OSTI ID: 1523674
Grant/Contract Number:  
AC02-06CH11357; 70247A; AC02‐06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 29; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; dislocation diffusion; ion-exchange; layer diffusion; layered cathode; lithium-ion batteries

Citation Formats

Xiao, Biwei, Wang, Kuan, Xu, Gui -Liang, Song, Junhua, Chen, Zonghai, Amine, Khalil, Reed, David, 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, 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, Sui, Manling, Sprenkle, Vincent L., Ren, Yang, Yan, Pengfei, and Li, Xiaolin. Thu . "Revealing the Atomic Origin of Heterogeneous Li-Ion Diffusion by Probing Na". United States. doi:10.1002/adma.201805889.
@article{osti_1559944,
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 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 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.},
doi = {10.1002/adma.201805889},
journal = {Advanced Materials},
number = 29,
volume = 31,
place = {United States},
year = {2019},
month = {5}
}

Journal Article:
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