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Title: Understanding the Role of Temperature and Cathode Composition on Interface and Bulk: Optimizing Aluminum Oxide Coatings for Li-Ion Cathodes

Abstract

Here, surface coating of cathode materials with Al2O3 has been shown to be a promising method for cathode stabilization and improved cycling performance at high operating voltages. However, a detailed understanding on how coating process and cathode composition changes the chemical composition, morphology and distribution of coating within cathode interface and bulk lattice, is still missing. In this study, we use a wet-chemical method to synthesize a series of Al2O3-coated LiNi0.5Co0.2Mn0.3O2 and LiCoO2 cathodes treated under various annealing temperatures and a combination of structural characterization techniques to understand the composition, homogeneity and morphology of coating layer and the bulk cathode. Nuclear magnetic resonance and electron microscopy results reveal that the nature of the interface is highly depended on the annealing temperature and cathode composition. For Al2O3-coated LiNi0.5Co0.2Mn0.3O2, higher annealing temperature leads to more homogeneous and more closely attached coating on cathode materials, corresponding to better electrochemical performance. Lower Al2O3 coating content is found to be helpful to further improve the initial capacity and cyclability, which can greatly outperform the pristine cathode material. For Al2O3-coated LiCoO2, the incorporation of Al into the cathode lattice is observed after annealing at high temperatures, implying the transformation from “surface coatings” to “dopants”, which ismore » not observed for LiNi0.5Co0.2Mn0.3O2. As a result, Al2O3-coated LiCoO2 annealed at higher temperature shows similar initial capacity but lower retention compared to that annealed at a lower temperature, due to the intercalation of surface alumina into the bulk layered structure forming a solid solution.« less

Authors:
 [1];  [2];  [1];  [1];  [1];  [2]; ORCiD logo [1]; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Univ. of Illinois, Chicago, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1374597
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 9; Journal Issue: 17; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 25 ENERGY STORAGE; 27Al MAS NMR; Al2O3 coating; coating vs doping; LCO; NMC; TEM

Citation Formats

Han, Binghong, Paulauskas, Tadas, Key, Baris, Peebles, Cameron, Park, Joong Sun, Klie, Robert F., Vaughey, John T., and Dogan, Fulya. Understanding the Role of Temperature and Cathode Composition on Interface and Bulk: Optimizing Aluminum Oxide Coatings for Li-Ion Cathodes. United States: N. p., 2017. Web. https://doi.org/10.1021/acsami.7b00595.
Han, Binghong, Paulauskas, Tadas, Key, Baris, Peebles, Cameron, Park, Joong Sun, Klie, Robert F., Vaughey, John T., & Dogan, Fulya. Understanding the Role of Temperature and Cathode Composition on Interface and Bulk: Optimizing Aluminum Oxide Coatings for Li-Ion Cathodes. United States. https://doi.org/10.1021/acsami.7b00595
Han, Binghong, Paulauskas, Tadas, Key, Baris, Peebles, Cameron, Park, Joong Sun, Klie, Robert F., Vaughey, John T., and Dogan, Fulya. Fri . "Understanding the Role of Temperature and Cathode Composition on Interface and Bulk: Optimizing Aluminum Oxide Coatings for Li-Ion Cathodes". United States. https://doi.org/10.1021/acsami.7b00595. https://www.osti.gov/servlets/purl/1374597.
@article{osti_1374597,
title = {Understanding the Role of Temperature and Cathode Composition on Interface and Bulk: Optimizing Aluminum Oxide Coatings for Li-Ion Cathodes},
author = {Han, Binghong and Paulauskas, Tadas and Key, Baris and Peebles, Cameron and Park, Joong Sun and Klie, Robert F. and Vaughey, John T. and Dogan, Fulya},
abstractNote = {Here, surface coating of cathode materials with Al2O3 has been shown to be a promising method for cathode stabilization and improved cycling performance at high operating voltages. However, a detailed understanding on how coating process and cathode composition changes the chemical composition, morphology and distribution of coating within cathode interface and bulk lattice, is still missing. In this study, we use a wet-chemical method to synthesize a series of Al2O3-coated LiNi0.5Co0.2Mn0.3O2 and LiCoO2 cathodes treated under various annealing temperatures and a combination of structural characterization techniques to understand the composition, homogeneity and morphology of coating layer and the bulk cathode. Nuclear magnetic resonance and electron microscopy results reveal that the nature of the interface is highly depended on the annealing temperature and cathode composition. For Al2O3-coated LiNi0.5Co0.2Mn0.3O2, higher annealing temperature leads to more homogeneous and more closely attached coating on cathode materials, corresponding to better electrochemical performance. Lower Al2O3 coating content is found to be helpful to further improve the initial capacity and cyclability, which can greatly outperform the pristine cathode material. For Al2O3-coated LiCoO2, the incorporation of Al into the cathode lattice is observed after annealing at high temperatures, implying the transformation from “surface coatings” to “dopants”, which is not observed for LiNi0.5Co0.2Mn0.3O2. As a result, Al2O3-coated LiCoO2 annealed at higher temperature shows similar initial capacity but lower retention compared to that annealed at a lower temperature, due to the intercalation of surface alumina into the bulk layered structure forming a solid solution.},
doi = {10.1021/acsami.7b00595},
journal = {ACS Applied Materials and Interfaces},
number = 17,
volume = 9,
place = {United States},
year = {2017},
month = {4}
}

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