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Title: Consequences of long-term water exposure for bulk crystal structure and surface composition/chemistry of nickel-rich layered oxide materials for Li-ion batteries

Abstract

Water exposure of layered nickel-rich transition metal oxide electrodes, widely used in high-energy lithium-ion batteries, has detrimental effects on the electrochemical performance, which complicates electrode handling and prevents implementation of environmentally benign aqueous processing procedures. Elucidating the degradation mechanisms in play may help rationally mitigate/circumvent key challenges. Here, the bulk structural consequences of long-term (>2.5 years) deuterated water (D2O) exposure of intercalation materials with compositions LixNi0.5Co0.2Mn0.3O2 (NCM523) and LixNi0.8Co0.1Mn0.1O2 (NCM811) are studied by neutron powder diffraction (NPD). Detailed inspection of the NPD data reveals gradual formation of a secondary crystalline phase in all exposed samples, not previously reported for this system. This unknown phase forms faster in liquid- compared to vapor-exposed compounds. Structural modelling of the NPD data shows a stable level of Li/Ni anti-site defects and does not indicate any significant changes in lattice parameters or hydrogen-lithium (D+/Li+) exchange in the structure. Consequently, the secondary phase formation must take place via transformation rather than modification of the parent material. X-ray photoelectron spectroscopy data indicate formation of LiHCO3/Li2CO3 at the surface and a Li-deficient oxide in the sub-surface region of the pristine compounds, and the presence of adsorbed water and transition metal hydroxides at the exposed sample surfaces.

Authors:
 [1];  [1];  [2];  [3];  [4];  [1]
  1. Univ. of New South Wales, Sydney, NSW (Australia)
  2. Univ. of New South Wales, Sydney, NSW (Australia) ; Australian Nuclear Science and Technology Organisation (ANSTO), Lucas Heights, NSW (Australia)
  3. Australian Nuclear Science and Technology Organisation (ANSTO), Lucas Heights, NSW (Australia)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE) - Office of Vehicle Technologies (VTO)
OSTI Identifier:
1635537
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Power Sources
Additional Journal Information:
Journal Volume: 470; Journal ID: ISSN 0378-7753
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; NMC; XPS; layered-oxide; moisture exposure; neutron diffraction; Layered nickel-rich oxides, deuterated water (D2O) exposure, neutron powder diffraction, Rietveld refinement

Citation Formats

Andersen, Henrik L., Cheung, Emily A., Avdeev, Maxim, Maynard-Casely, Helen E., Abraham, Daniel P., and Sharma, Neeraj. Consequences of long-term water exposure for bulk crystal structure and surface composition/chemistry of nickel-rich layered oxide materials for Li-ion batteries. United States: N. p., 2020. Web. https://doi.org/10.1016/j.jpowsour.2020.228370.
Andersen, Henrik L., Cheung, Emily A., Avdeev, Maxim, Maynard-Casely, Helen E., Abraham, Daniel P., & Sharma, Neeraj. Consequences of long-term water exposure for bulk crystal structure and surface composition/chemistry of nickel-rich layered oxide materials for Li-ion batteries. United States. https://doi.org/10.1016/j.jpowsour.2020.228370
Andersen, Henrik L., Cheung, Emily A., Avdeev, Maxim, Maynard-Casely, Helen E., Abraham, Daniel P., and Sharma, Neeraj. Tue . "Consequences of long-term water exposure for bulk crystal structure and surface composition/chemistry of nickel-rich layered oxide materials for Li-ion batteries". United States. https://doi.org/10.1016/j.jpowsour.2020.228370.
@article{osti_1635537,
title = {Consequences of long-term water exposure for bulk crystal structure and surface composition/chemistry of nickel-rich layered oxide materials for Li-ion batteries},
author = {Andersen, Henrik L. and Cheung, Emily A. and Avdeev, Maxim and Maynard-Casely, Helen E. and Abraham, Daniel P. and Sharma, Neeraj},
abstractNote = {Water exposure of layered nickel-rich transition metal oxide electrodes, widely used in high-energy lithium-ion batteries, has detrimental effects on the electrochemical performance, which complicates electrode handling and prevents implementation of environmentally benign aqueous processing procedures. Elucidating the degradation mechanisms in play may help rationally mitigate/circumvent key challenges. Here, the bulk structural consequences of long-term (>2.5 years) deuterated water (D2O) exposure of intercalation materials with compositions LixNi0.5Co0.2Mn0.3O2 (NCM523) and LixNi0.8Co0.1Mn0.1O2 (NCM811) are studied by neutron powder diffraction (NPD). Detailed inspection of the NPD data reveals gradual formation of a secondary crystalline phase in all exposed samples, not previously reported for this system. This unknown phase forms faster in liquid- compared to vapor-exposed compounds. Structural modelling of the NPD data shows a stable level of Li/Ni anti-site defects and does not indicate any significant changes in lattice parameters or hydrogen-lithium (D+/Li+) exchange in the structure. Consequently, the secondary phase formation must take place via transformation rather than modification of the parent material. X-ray photoelectron spectroscopy data indicate formation of LiHCO3/Li2CO3 at the surface and a Li-deficient oxide in the sub-surface region of the pristine compounds, and the presence of adsorbed water and transition metal hydroxides at the exposed sample surfaces.},
doi = {10.1016/j.jpowsour.2020.228370},
journal = {Journal of Power Sources},
number = ,
volume = 470,
place = {United States},
year = {2020},
month = {9}
}

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This content will become publicly available on September 15, 2021
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