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Title: Surface Modification for Suppressing Interfacial Parasitic Reactions of a Nickel-Rich Lithium-Ion Cathode

Abstract

Ni-rich lithium nickel manganese cobalt oxides (Li-NixMnyCo1-x-yO2, x >= 0.5, NMCs) are high-capacity cathode materials for Li-ion batteries, but they exhibit limited cycling stability under high cutoff potentials. Various aspects, including transition metal dissolution, structural disordering, particle cracking, surface film thickening, etc., have already been investigated in terms of their performance degradation in the battery research community. Interestingly, these phenomena were primarily observed at the surface layer of the cathode material, implying that they may also be facilitated by some interfacial parasitic reactions between the delithiated NMC electrode and the non-aqueous electrolyte. Here in this study, LiNi0.6Mn0.2Co0.2O2 (NMC 622) electrodes chemically modified with TiO2 via atomic layer deposition were used as a model system to demonstrate the criticalness of the interfacial parasitic reactions. The suppression of the interfacial parasitic reactions effectively reduced. the hike of the cathodic surface film resistance, decreased the level of dissolution of transition metals, decreased the level of particle fragmentation, and mitigated the cation mixing of NMC 622. Finally, all of these results demonstrated that careful design of the interfacial layer by surface modifications is a key approach for improving the durability of Ni-rich NMCs under high-voltage cycling.

Authors:
 [1];  [2];  [1];  [3]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [4]; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  2. Univ. of Arkansas, Fayetteville, AR (United States). Dept. of Mechanical Engineering
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division; Stanford Univ., CA (United States). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1531345
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 8; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Gao, Han, Cai, Jiyu, Xu, Gui-Liang, Li, Luxi, Ren, Yang, Meng, Xiangbo, Amine, Khalil, and Chen, Zonghai. Surface Modification for Suppressing Interfacial Parasitic Reactions of a Nickel-Rich Lithium-Ion Cathode. United States: N. p., 2019. Web. doi:10.1021/acs.chemmater.8b04200.
Gao, Han, Cai, Jiyu, Xu, Gui-Liang, Li, Luxi, Ren, Yang, Meng, Xiangbo, Amine, Khalil, & Chen, Zonghai. Surface Modification for Suppressing Interfacial Parasitic Reactions of a Nickel-Rich Lithium-Ion Cathode. United States. https://doi.org/10.1021/acs.chemmater.8b04200
Gao, Han, Cai, Jiyu, Xu, Gui-Liang, Li, Luxi, Ren, Yang, Meng, Xiangbo, Amine, Khalil, and Chen, Zonghai. Fri . "Surface Modification for Suppressing Interfacial Parasitic Reactions of a Nickel-Rich Lithium-Ion Cathode". United States. https://doi.org/10.1021/acs.chemmater.8b04200. https://www.osti.gov/servlets/purl/1531345.
@article{osti_1531345,
title = {Surface Modification for Suppressing Interfacial Parasitic Reactions of a Nickel-Rich Lithium-Ion Cathode},
author = {Gao, Han and Cai, Jiyu and Xu, Gui-Liang and Li, Luxi and Ren, Yang and Meng, Xiangbo and Amine, Khalil and Chen, Zonghai},
abstractNote = {Ni-rich lithium nickel manganese cobalt oxides (Li-NixMnyCo1-x-yO2, x >= 0.5, NMCs) are high-capacity cathode materials for Li-ion batteries, but they exhibit limited cycling stability under high cutoff potentials. Various aspects, including transition metal dissolution, structural disordering, particle cracking, surface film thickening, etc., have already been investigated in terms of their performance degradation in the battery research community. Interestingly, these phenomena were primarily observed at the surface layer of the cathode material, implying that they may also be facilitated by some interfacial parasitic reactions between the delithiated NMC electrode and the non-aqueous electrolyte. Here in this study, LiNi0.6Mn0.2Co0.2O2 (NMC 622) electrodes chemically modified with TiO2 via atomic layer deposition were used as a model system to demonstrate the criticalness of the interfacial parasitic reactions. The suppression of the interfacial parasitic reactions effectively reduced. the hike of the cathodic surface film resistance, decreased the level of dissolution of transition metals, decreased the level of particle fragmentation, and mitigated the cation mixing of NMC 622. Finally, all of these results demonstrated that careful design of the interfacial layer by surface modifications is a key approach for improving the durability of Ni-rich NMCs under high-voltage cycling.},
doi = {10.1021/acs.chemmater.8b04200},
journal = {Chemistry of Materials},
number = 8,
volume = 31,
place = {United States},
year = {2019},
month = {3}
}

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