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Title: Nonuniform Growth of Sub-2 Nanometer Atomic Layer Deposited Alumina Films on Lithium Nickel Manganese Cobalt Oxide Cathode Battery Materials

Abstract

The deposition of alumina ALD films on Li ion battery cathode particles is known to enhance the cycling stability of lithium ion batteries fabricated from those coated particles. It is commonly assumed that the film on the particles is of uniform thickness and is optimally thin enough to facilitate lithium diffusion while blocking side reactions of the electrolyte with the cathode substrate. Here, we elucidate the nature of thin alumina films deposited with between 2 and 15 ALD cycles on lithium nickel manganese cobalt oxide cathode precursor particles. Low energy ion scattering (LEIS) and secondary ion mass spectroscopy (SIMS) methods were used to characterize thin (<2 nm) films that were deposited by ALD. Surface analysis showed that low-cycle number ALD films were not uniform nor uniformly thick over the surface of the cathode particles and that alumina ALD preferentially deposited on transition metal bound sites on the cathode particle surface and coated Li on the surface to a lesser extent. Lithium was found to still be present on the cathode powder surface, even after 10 ALD cycles. Contrary to current supposition, low-cycle ALD appeared to improve the cycling stability of battery cathode active materials through this preferential growth that stabilizedmore » the transition metal oxides in the presence of electrolyte without blocking lithium intercalation pathways. This is the first study to determine that Li remains exposed on the as-synthesized surface of ALD coated cathode particles and that the ALD film is nonuniform and nonuniformly thick when less than 10 ALD cycles are used.« less

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1];  [1];  [1];  [2]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]
  1. Univ. of Colorado, Boulder, CO (United States)
  2. Missouri Univ. of Science and Technology, Rolla, MO (United States)
  3. Univ. of Colorado, Boulder, CO (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1578263
Report Number(s):
NREL/JA-5K00-75593
Journal ID: ISSN 2574-0970; MainId:22734;UUID:d69d408a-6d18-ea11-9c2a-ac162d87dfe5;MainAdminID:11210
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Nano Materials
Additional Journal Information:
Journal Volume: 2; Journal Issue: 11; Journal ID: ISSN 2574-0970
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; cathode materials; surface modification; atomic layer deposition; nanostructured films; lithium ion batteries; nonuniform particle

Citation Formats

Hoskins, Amanda L., McNeary, W. Wilson, Millican, Samantha L., Gossett, Tyler A., Lai, Annika, Gao, Yan, Liang, Xinhua, Musgrave, Charles B., and Weimer, Alan W. Nonuniform Growth of Sub-2 Nanometer Atomic Layer Deposited Alumina Films on Lithium Nickel Manganese Cobalt Oxide Cathode Battery Materials. United States: N. p., 2019. Web. doi:10.1021/acsanm.9b01490.
Hoskins, Amanda L., McNeary, W. Wilson, Millican, Samantha L., Gossett, Tyler A., Lai, Annika, Gao, Yan, Liang, Xinhua, Musgrave, Charles B., & Weimer, Alan W. Nonuniform Growth of Sub-2 Nanometer Atomic Layer Deposited Alumina Films on Lithium Nickel Manganese Cobalt Oxide Cathode Battery Materials. United States. https://doi.org/10.1021/acsanm.9b01490
Hoskins, Amanda L., McNeary, W. Wilson, Millican, Samantha L., Gossett, Tyler A., Lai, Annika, Gao, Yan, Liang, Xinhua, Musgrave, Charles B., and Weimer, Alan W. Thu . "Nonuniform Growth of Sub-2 Nanometer Atomic Layer Deposited Alumina Films on Lithium Nickel Manganese Cobalt Oxide Cathode Battery Materials". United States. https://doi.org/10.1021/acsanm.9b01490. https://www.osti.gov/servlets/purl/1578263.
@article{osti_1578263,
title = {Nonuniform Growth of Sub-2 Nanometer Atomic Layer Deposited Alumina Films on Lithium Nickel Manganese Cobalt Oxide Cathode Battery Materials},
author = {Hoskins, Amanda L. and McNeary, W. Wilson and Millican, Samantha L. and Gossett, Tyler A. and Lai, Annika and Gao, Yan and Liang, Xinhua and Musgrave, Charles B. and Weimer, Alan W.},
abstractNote = {The deposition of alumina ALD films on Li ion battery cathode particles is known to enhance the cycling stability of lithium ion batteries fabricated from those coated particles. It is commonly assumed that the film on the particles is of uniform thickness and is optimally thin enough to facilitate lithium diffusion while blocking side reactions of the electrolyte with the cathode substrate. Here, we elucidate the nature of thin alumina films deposited with between 2 and 15 ALD cycles on lithium nickel manganese cobalt oxide cathode precursor particles. Low energy ion scattering (LEIS) and secondary ion mass spectroscopy (SIMS) methods were used to characterize thin (<2 nm) films that were deposited by ALD. Surface analysis showed that low-cycle number ALD films were not uniform nor uniformly thick over the surface of the cathode particles and that alumina ALD preferentially deposited on transition metal bound sites on the cathode particle surface and coated Li on the surface to a lesser extent. Lithium was found to still be present on the cathode powder surface, even after 10 ALD cycles. Contrary to current supposition, low-cycle ALD appeared to improve the cycling stability of battery cathode active materials through this preferential growth that stabilized the transition metal oxides in the presence of electrolyte without blocking lithium intercalation pathways. This is the first study to determine that Li remains exposed on the as-synthesized surface of ALD coated cathode particles and that the ALD film is nonuniform and nonuniformly thick when less than 10 ALD cycles are used.},
doi = {10.1021/acsanm.9b01490},
journal = {ACS Applied Nano Materials},
number = 11,
volume = 2,
place = {United States},
year = {2019},
month = {10}
}

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Figures / Tables:

Figure 1 Figure 1: LEIS spectra of the (a) Al and (b) Mn and Co+Ni characteristic peaks. As the cycle number increases the Al signal increases with a corresponding decrease in both the Mn and Co+Ni signals, indicating that the film is coating on the substrate surface. The Mn and Co+Ni peaksmore » are completely suppressed by 10 cycles of Al2O3 ALD.« less

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