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Title: Synthesis and Characterization of Core-Shell Nanocrystals of Co-Rich Cathodes

Abstract

Interfacial stability between the cathode and the electrolyte in Li-ion batteries directly determines durability upon cycling. Core-shell nanoscale heterostructures offer high precision when replacing redox-active ions on the surface with inactive species such as Al ions to suppress these deleterious reactions. However, the level of compositional complexity of leading cathodes for high-energy devices, while showing increased stability, remains to be demonstrated for these heterostructures. A combination of colloidal synthesis and subsequent post-annealing process was used to produce cores of LiCo0.5Ni0.25Mn0.25O2, a layered oxide with a high theoretical capacity, with epitaxial and conformal shells with increasing concentration of Al from the interior to surface. Thorough insight at high chemical and spatial resolution was obtained by a combination of characterization techniques. The gradient of Al was controlled by the initial content and the temperature of synthesis. The passivation layers play a critical role in notably increasing the retention of capacity, which was particularly considerable under harsh conditions such as wide potential window and, especially, elevated temperature, which accelerate side reactions. Spectroscopic analysis revealed that the tailored surface layers mainly stabilized the electronic environment at the surface, suggesting a possible explanation to the improved battery performance.

Authors:
; ; ; ; ; ; ; ; ORCiD logo
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; National Science Foundation (NSF)
OSTI Identifier:
1567929
Alternate Identifier(s):
OSTI ID: 1670149
Grant/Contract Number:  
AC02-06CH11357; CBET-1605126; DMR-0959470; DMR-1626065
Resource Type:
Published Article
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Name: Journal of the Electrochemical Society Journal Volume: 167 Journal Issue: 5; Journal ID: ISSN 0013-4651
Publisher:
IOP Publishing - The Electrochemical Society
Country of Publication:
United States
Language:
English

Citation Formats

Kwon, Bob Jin, Dogan, Fulya, Jokisaari, Jacob R., Key, Baris, Bolotin, Igor L., Paulauskas, Tadas, Kim, Chunjoong, Klie, Robert F., and Cabana, Jordi. Synthesis and Characterization of Core-Shell Nanocrystals of Co-Rich Cathodes. United States: N. p., 2019. Web. doi:10.1149/2.0012005jes.
Kwon, Bob Jin, Dogan, Fulya, Jokisaari, Jacob R., Key, Baris, Bolotin, Igor L., Paulauskas, Tadas, Kim, Chunjoong, Klie, Robert F., & Cabana, Jordi. Synthesis and Characterization of Core-Shell Nanocrystals of Co-Rich Cathodes. United States. doi:10.1149/2.0012005jes.
Kwon, Bob Jin, Dogan, Fulya, Jokisaari, Jacob R., Key, Baris, Bolotin, Igor L., Paulauskas, Tadas, Kim, Chunjoong, Klie, Robert F., and Cabana, Jordi. Tue . "Synthesis and Characterization of Core-Shell Nanocrystals of Co-Rich Cathodes". United States. doi:10.1149/2.0012005jes.
@article{osti_1567929,
title = {Synthesis and Characterization of Core-Shell Nanocrystals of Co-Rich Cathodes},
author = {Kwon, Bob Jin and Dogan, Fulya and Jokisaari, Jacob R. and Key, Baris and Bolotin, Igor L. and Paulauskas, Tadas and Kim, Chunjoong and Klie, Robert F. and Cabana, Jordi},
abstractNote = {Interfacial stability between the cathode and the electrolyte in Li-ion batteries directly determines durability upon cycling. Core-shell nanoscale heterostructures offer high precision when replacing redox-active ions on the surface with inactive species such as Al ions to suppress these deleterious reactions. However, the level of compositional complexity of leading cathodes for high-energy devices, while showing increased stability, remains to be demonstrated for these heterostructures. A combination of colloidal synthesis and subsequent post-annealing process was used to produce cores of LiCo0.5Ni0.25Mn0.25O2, a layered oxide with a high theoretical capacity, with epitaxial and conformal shells with increasing concentration of Al from the interior to surface. Thorough insight at high chemical and spatial resolution was obtained by a combination of characterization techniques. The gradient of Al was controlled by the initial content and the temperature of synthesis. The passivation layers play a critical role in notably increasing the retention of capacity, which was particularly considerable under harsh conditions such as wide potential window and, especially, elevated temperature, which accelerate side reactions. Spectroscopic analysis revealed that the tailored surface layers mainly stabilized the electronic environment at the surface, suggesting a possible explanation to the improved battery performance.},
doi = {10.1149/2.0012005jes},
journal = {Journal of the Electrochemical Society},
number = 5,
volume = 167,
place = {United States},
year = {2019},
month = {10}
}

Journal Article:
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DOI: 10.1149/2.0012005jes

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