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Title: Structural Evolution of LixNiyMnzCo1-y-zO2 Cathode Materials during High-Rate Charge and Discharge

Abstract

Ni-rich lithium transition metal oxides have received significant attention due to their high capacities and rate capabilities determined via theoretical calculations. Although the structural properties of these materials are strongly correlated with the electrochemical performance, their structural stability during the high-rate electrochemical reactions has not been fully evaluated yet. In this work, transmission electron microscopy is used to investigate the crystallographic and electronic structural modifications of Ni-based cathode materials at a high charge/discharge rate of 10 C. It is found that the high-rate electrochemical reactions induce structural inhomogeneity near the surface of Ni-rich cathode materials, which limits Li transport and reduces their capacities. Furthermore, this study establishes a correlation between the high-rate electrochemical performance of the Ni-based materials and their structural evolution, which can provide profound insights for designing novel cathode materials having both high energy and power densities.

Authors:
 [1];  [2]; ORCiD logo [2];  [3];  [4]; ORCiD logo [2]
  1. Korea Institute of Science and Technology (KIST), Seoul (Republic of Korea); Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Korea Institute of Science and Technology (KIST), Seoul (Republic of Korea)
  3. Kyung Hee Univ., Seoul (Republic of Korea)
  4. KIST, Wanju-gun (Republic of Korea)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1409643
Report Number(s):
BNL-114698-2017-JA
Journal ID: ISSN 1948-7185; R&D Project: 16060; 16060; TRN: US1703200
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
29 ENERGY PLANNING, POLICY, AND ECONOMY; lithium ion batteries; high rate; cathode; structural evolution; transmission electron microscopy; Center for Functional Nanomaterials

Citation Formats

Hwang, Sooyeon, Jo, Eunmi, Chung, Kyung Yoon, Hwang, Kyo Seon, Kim, Seung Min, and Chang, Wonyoung. Structural Evolution of LixNiyMnzCo1-y-zO2 Cathode Materials during High-Rate Charge and Discharge. United States: N. p., 2017. Web. doi:10.1021/acs.jpclett.7b02579.
Hwang, Sooyeon, Jo, Eunmi, Chung, Kyung Yoon, Hwang, Kyo Seon, Kim, Seung Min, & Chang, Wonyoung. Structural Evolution of LixNiyMnzCo1-y-zO2 Cathode Materials during High-Rate Charge and Discharge. United States. https://doi.org/10.1021/acs.jpclett.7b02579
Hwang, Sooyeon, Jo, Eunmi, Chung, Kyung Yoon, Hwang, Kyo Seon, Kim, Seung Min, and Chang, Wonyoung. Wed . "Structural Evolution of LixNiyMnzCo1-y-zO2 Cathode Materials during High-Rate Charge and Discharge". United States. https://doi.org/10.1021/acs.jpclett.7b02579. https://www.osti.gov/servlets/purl/1409643.
@article{osti_1409643,
title = {Structural Evolution of LixNiyMnzCo1-y-zO2 Cathode Materials during High-Rate Charge and Discharge},
author = {Hwang, Sooyeon and Jo, Eunmi and Chung, Kyung Yoon and Hwang, Kyo Seon and Kim, Seung Min and Chang, Wonyoung},
abstractNote = {Ni-rich lithium transition metal oxides have received significant attention due to their high capacities and rate capabilities determined via theoretical calculations. Although the structural properties of these materials are strongly correlated with the electrochemical performance, their structural stability during the high-rate electrochemical reactions has not been fully evaluated yet. In this work, transmission electron microscopy is used to investigate the crystallographic and electronic structural modifications of Ni-based cathode materials at a high charge/discharge rate of 10 C. It is found that the high-rate electrochemical reactions induce structural inhomogeneity near the surface of Ni-rich cathode materials, which limits Li transport and reduces their capacities. Furthermore, this study establishes a correlation between the high-rate electrochemical performance of the Ni-based materials and their structural evolution, which can provide profound insights for designing novel cathode materials having both high energy and power densities.},
doi = {10.1021/acs.jpclett.7b02579},
journal = {Journal of Physical Chemistry Letters},
number = ,
volume = 8,
place = {United States},
year = {Wed Nov 08 00:00:00 EST 2017},
month = {Wed Nov 08 00:00:00 EST 2017}
}

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Works referenced in this record:

Building better batteries
journal, February 2008

  • Armand, M.; Tarascon, J.-M.
  • Nature, Vol. 451, Issue 7179, p. 652-657
  • DOI: 10.1038/451652a

Electrical Energy Storage for the Grid: A Battery of Choices
journal, November 2011


Nickel-Rich Layered Lithium Transition-Metal Oxide for High-Energy Lithium-Ion Batteries
journal, March 2015

  • Liu, Wen; Oh, Pilgun; Liu, Xien
  • Angewandte Chemie International Edition, Vol. 54, Issue 15
  • DOI: 10.1002/anie.201409262

Electrodes with High Power and High Capacity for Rechargeable Lithium Batteries
journal, February 2006

  • Kang, Kisuk; Shirley Meng, Ying; Breger, Julien
  • Science, Vol. 311, Issue 5763, p. 977-980
  • DOI: 10.1126/science.1122152

Kinetics Tuning of Li-Ion Diffusion in Layered Li(Ni x Mn y Co z )O 2
journal, June 2015

  • Wei, Yi; Zheng, Jiaxin; Cui, Suihan
  • Journal of the American Chemical Society, Vol. 137, Issue 26
  • DOI: 10.1021/jacs.5b04040

Factors that affect Li mobility in layered lithium transition metal oxides
journal, September 2006


Microstructural Changes in LiNi0.8Co0.15Al0.05O2 Positive Electrode Material during the First Cycle
journal, January 2011

  • Zheng, Shijian; Huang, Rong; Makimura, Yoshinari
  • Journal of The Electrochemical Society, Vol. 158, Issue 4
  • DOI: 10.1149/1.3544843

Structural Changes and Thermal Stability of Charged LiNi x Mn y Co z O 2 Cathode Materials Studied by Combined In Situ Time-Resolved XRD and Mass Spectroscopy
journal, December 2014

  • Bak, Seong-Min; Hu, Enyuan; Zhou, Yongning
  • ACS Applied Materials & Interfaces, Vol. 6, Issue 24
  • DOI: 10.1021/am506712c

Understanding the Degradation Mechanisms of LiNi 0.5 Co 0.2 Mn 0.3 O 2 Cathode Material in Lithium Ion Batteries
journal, August 2013

  • Jung, Sung-Kyun; Gwon, Hyeokjo; Hong, Jihyun
  • Advanced Energy Materials, Vol. 4, Issue 1
  • DOI: 10.1002/aenm.201300787

High-Rate Charging Induced Intermediate Phases and Structural Changes of Layer-Structured Cathode for Lithium-Ion Batteries
journal, August 2016

  • Zhou, Yong-Ning; Yue, Ji-Li; Hu, Enyuan
  • Advanced Energy Materials, Vol. 6, Issue 21
  • DOI: 10.1002/aenm.201600597

Electron energy-loss near-edge structure - a tool for the investigation of electronic structure on the nanometre scale
journal, August 2001


Investigation of the Charge Compensation Mechanism on the Electrochemically Li-Ion Deintercalated Li 1 - x Co 1/3 Ni 1/3 Mn 1/3 O 2 Electrode System by Combination of Soft and Hard X-ray Absorption Spectroscopy
journal, December 2005

  • Yoon, Won-Sub; Balasubramanian, Mahalingam; Chung, Kyung Yoon
  • Journal of the American Chemical Society, Vol. 127, Issue 49
  • DOI: 10.1021/ja0530568

Understanding local degradation of cycled Ni-rich cathode materials at high operating temperature for Li-ion batteries
journal, September 2014

  • Hwang, Sooyeon; Kim, Dong Hyun; Chung, Kyung Yoon
  • Applied Physics Letters, Vol. 105, Issue 10
  • DOI: 10.1063/1.4895336

An Electron Energy-Loss Spectrometry Study of Charge Compensation in LiNi 0.8 Co 0.2 O 2
journal, April 2003

  • Graetz, J.; Ahn, C. C.; Yazami, R.
  • The Journal of Physical Chemistry B, Vol. 107, Issue 13
  • DOI: 10.1021/jp026484y

White lines and d -band occupancy for the 3 d transition-metal oxides and lithium transition-metal oxides
journal, June 2004


EELS analysis of cation valence states and oxygen vacancies in magnetic oxides
journal, October 2000


Electronic Structure of Lithium Nickel Oxides by Electron Energy Loss Spectroscopy
journal, June 2005

  • Koyama, Yukinori; Mizoguchi, Teruyasu; Ikeno, Hidekazu
  • The Journal of Physical Chemistry B, Vol. 109, Issue 21
  • DOI: 10.1021/jp050486b

Extraction of EELS white-line intensities of manganese compounds: Methods, accuracy, and valence sensitivity
journal, March 2006


In situ electron energy loss spectroscopy study of metallic Co and Co oxides
journal, September 2010

  • Zhao, Yuan; Feltes, Theresa E.; Regalbuto, John R.
  • Journal of Applied Physics, Vol. 108, Issue 6
  • DOI: 10.1063/1.3482013

Capacity-Fading Mechanisms of LiNiO[sub 2]-Based Lithium-Ion Batteries
journal, January 2009

  • Muto, Shunsuke; Sasano, Yusuke; Tatsumi, Kazuyoshi
  • Journal of The Electrochemical Society, Vol. 156, Issue 5
  • DOI: 10.1149/1.3076137

Determination of the mechanism and extent of surface degradation in Ni-based cathode materials after repeated electrochemical cycling
journal, September 2016

  • Hwang, Sooyeon; Kim, Se Young; Chung, Kyung Yoon
  • APL Materials, Vol. 4, Issue 9
  • DOI: 10.1063/1.4963723

Works referencing / citing this record:

Surface/Interface Structure Degradation of Ni‐Rich Layered Oxide Cathodes toward Lithium‐Ion Batteries: Fundamental Mechanisms and Remedying Strategies
journal, December 2019

  • Liang, Longwei; Zhang, Wenheng; Zhao, Fei
  • Advanced Materials Interfaces, Vol. 7, Issue 3
  • DOI: 10.1002/admi.201901749

Boron-doped single crystal LiNi0.6Mn0.2Co0.2O2 with improved electrochemical performance for lithium-ion batteries
journal, July 2019


In‐Depth TEM Investigation on Structural Inhomogeneity within a Primary Li x Ni 0.835 Co 0.15 Al 0.015 O 2 Particle: Origin of Capacity Decay during High‐Rate Discharge
journal, February 2020

  • Lee, Hyesu; Jo, Eunmi; Chung, Kyung Yoon
  • Angewandte Chemie International Edition, Vol. 59, Issue 6
  • DOI: 10.1002/anie.201910670

Cooling Induced Surface Reconstruction during Synthesis of High‐Ni Layered Oxides
journal, October 2019

  • Zhang, Ming‐Jian; Hu, Xiaobing; Li, Maofan
  • Advanced Energy Materials, Vol. 9, Issue 43
  • DOI: 10.1002/aenm.201901915

Honeycomb-Like Nitrogen-Doped Carbon 3D Nanoweb@Li 2 S Cathode Material for Use in Lithium Sulfur Batteries
journal, January 2019