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Title: Evolution Of Lattice Structure And Chemical Composition Of The Surface Reconstruction Layer In Li1.2Ni0.2Mn0.6O2 Cathode Material For Lithium Ion Batteries

Abstract

Voltage and capacity fading of layer structured lithium and manganese rich (LMR) transition metal oxide is directly related to the structural and composition evolution of the material during the cycling of the battery. However, understanding such evolution at atomic level remains elusive. Based on atomic level structural imaging, elemental mapping of the pristine and cycled samples and density functional theory calculations, it is found that accompanying the hoping of Li ions is the simultaneous migration of Ni ions towards the surface from the bulk lattice, leading to the gradual depletion of Ni in the bulk lattice and thickening of a Ni enriched surface reconstruction layer (SRL). Furthermore, Ni and Mn also exhibit concentration partitions within the thin layer of SRL in the cycled samples where Ni is almost depleted at the very surface of the SRL, indicating the preferential dissolution of Ni ions in the electrolyte. Accompanying the elemental composition evolution, significant structural evolution is also observed and identified as a sequential phase transition of C2/m →I41→Spinel. For the first time, it is found that the surface facet terminated with pure cation is more stable than that with a mixture of cation and anion. These findings firmly established how themore » elemental species in the lattice of LMR cathode transfer from the bulk lattice to surface layer and further into the electrolyte, clarifying the long standing confusion and debate on the structure and chemistry of the surface layer and their correlation with the voltage fading and capacity decaying of LMR cathode. Therefore, this work provides critical insights for designing of cathode materials with both high capacity and voltage stability during cycling.« less

Authors:
; ; ; ; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1170053
Report Number(s):
PNNL-SA-106363
48379
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Nano Letters, 15(1):514-522
Country of Publication:
United States
Language:
English
Subject:
Lithium ion battery, LMR cathode, surface reconstruction, ion migration, chemical partition; Environmental Molecular Sciences Laboratory

Citation Formats

Yan, Pengfei, Nie, Anmin, Zheng, Jianming, Zhou, Yungang, Lu, Dongping, Zhang, Xiaofeng, Xu, Rui, Belharouak, Ilias, Zu, Xiaotao, Xiao, Jie, Amine, Khalil, Liu, Jun, Gao, Fei, Shahbazian-Yassar, Reza, Zhang, Jiguang, and Wang, Chong M. Evolution Of Lattice Structure And Chemical Composition Of The Surface Reconstruction Layer In Li1.2Ni0.2Mn0.6O2 Cathode Material For Lithium Ion Batteries. United States: N. p., 2015. Web. doi:10.1021/nl5038598.
Yan, Pengfei, Nie, Anmin, Zheng, Jianming, Zhou, Yungang, Lu, Dongping, Zhang, Xiaofeng, Xu, Rui, Belharouak, Ilias, Zu, Xiaotao, Xiao, Jie, Amine, Khalil, Liu, Jun, Gao, Fei, Shahbazian-Yassar, Reza, Zhang, Jiguang, & Wang, Chong M. Evolution Of Lattice Structure And Chemical Composition Of The Surface Reconstruction Layer In Li1.2Ni0.2Mn0.6O2 Cathode Material For Lithium Ion Batteries. United States. doi:10.1021/nl5038598.
Yan, Pengfei, Nie, Anmin, Zheng, Jianming, Zhou, Yungang, Lu, Dongping, Zhang, Xiaofeng, Xu, Rui, Belharouak, Ilias, Zu, Xiaotao, Xiao, Jie, Amine, Khalil, Liu, Jun, Gao, Fei, Shahbazian-Yassar, Reza, Zhang, Jiguang, and Wang, Chong M. Wed . "Evolution Of Lattice Structure And Chemical Composition Of The Surface Reconstruction Layer In Li1.2Ni0.2Mn0.6O2 Cathode Material For Lithium Ion Batteries". United States. doi:10.1021/nl5038598.
@article{osti_1170053,
title = {Evolution Of Lattice Structure And Chemical Composition Of The Surface Reconstruction Layer In Li1.2Ni0.2Mn0.6O2 Cathode Material For Lithium Ion Batteries},
author = {Yan, Pengfei and Nie, Anmin and Zheng, Jianming and Zhou, Yungang and Lu, Dongping and Zhang, Xiaofeng and Xu, Rui and Belharouak, Ilias and Zu, Xiaotao and Xiao, Jie and Amine, Khalil and Liu, Jun and Gao, Fei and Shahbazian-Yassar, Reza and Zhang, Jiguang and Wang, Chong M.},
abstractNote = {Voltage and capacity fading of layer structured lithium and manganese rich (LMR) transition metal oxide is directly related to the structural and composition evolution of the material during the cycling of the battery. However, understanding such evolution at atomic level remains elusive. Based on atomic level structural imaging, elemental mapping of the pristine and cycled samples and density functional theory calculations, it is found that accompanying the hoping of Li ions is the simultaneous migration of Ni ions towards the surface from the bulk lattice, leading to the gradual depletion of Ni in the bulk lattice and thickening of a Ni enriched surface reconstruction layer (SRL). Furthermore, Ni and Mn also exhibit concentration partitions within the thin layer of SRL in the cycled samples where Ni is almost depleted at the very surface of the SRL, indicating the preferential dissolution of Ni ions in the electrolyte. Accompanying the elemental composition evolution, significant structural evolution is also observed and identified as a sequential phase transition of C2/m →I41→Spinel. For the first time, it is found that the surface facet terminated with pure cation is more stable than that with a mixture of cation and anion. These findings firmly established how the elemental species in the lattice of LMR cathode transfer from the bulk lattice to surface layer and further into the electrolyte, clarifying the long standing confusion and debate on the structure and chemistry of the surface layer and their correlation with the voltage fading and capacity decaying of LMR cathode. Therefore, this work provides critical insights for designing of cathode materials with both high capacity and voltage stability during cycling.},
doi = {10.1021/nl5038598},
journal = {Nano Letters, 15(1):514-522},
number = ,
volume = ,
place = {United States},
year = {Wed Jan 14 00:00:00 EST 2015},
month = {Wed Jan 14 00:00:00 EST 2015}
}