Multifunctional Effect of Fe Substitution in Na Layered Cathode Materials for Enhanced Storage Stability

Jehee Park; Kyojin Ku; Jihyeon Gim; Seoung Bum Son; Heonjae Jeong; Lei Cheng; Hakim Iddir; Dewen Hou; Hui Xiong; Yuzi Liu; Eungje Lee; Christopher Johnson

doi:10.1021/acsami.3c07068

Multifunctional Effect of Fe Substitution in Na Layered Cathode Materials for Enhanced Storage Stability

Jehee Park
, Kyojin Ku
, Jihyeon Gim
, Seoung Bum Son
, Heonjae Jeong
, Lei Cheng
, Hakim Iddir
, Dewen Hou
, Hui Xiong
, Yuzi Liu
, Eungje Lee
, Christopher Johnson

Research output: Contribution to journal › Article › peer-review

6 Scopus citations

Abstract

Developing stable cathode materials that are resistant to storage degradation is essential for practical development and industrial processing of Na-ion batteries as many sodium layered oxide materials are susceptible to hygroscopicity and instability upon exposure to ambient air. Among the various layered compounds, Fe-substituted O3-type Na(Ni_1/2Mn_1/2)_1-xFe_xO₂ materials have emerged as a promising option for high-performance and low-cost cathodes. While previous reports have noted the decent air-storage stability of these materials, the role and origin of Fe substitution in improving storage stability remain unclear. In this study, we investigate the air-resistant effect of Fe substitution in O3-Na(Ni_1/2Mn_1/2)_1-xFe_xO₂ cathode materials by performing systematic surface and structural characterizations. We find that the improved storage stability can be attributed to the multifunctional effect of Fe substitution, which forms a surface protective layer containing an Fe-incorporated spinel phase and decreases the thermodynamical driving force for bulk chemical sodium extraction. With these mechanisms, Fe-containing cathodes can suppress the cascades of cathode degradation processes and better retain the electrochemical performance after air storage.

Original language	English
Pages (from-to)	38454-38462
Number of pages	9
Journal	ACS Applied Materials and Interfaces
Volume	15
Issue number	32
DOIs	https://doi.org/10.1021/acsami.3c07068
State	Published - Aug 16 2023
Externally published	Yes

Funding

Support from the Advanced Battery Materials Research (BMR) Program, in particular Tien Duong, of the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, is gratefully acknowledged. The work by K.K. was supported by the research fund of Hanbat National University in 2021 and “Regional Innovation Strategy (RIS)” through the National Research Foundation of Korea (NRF) funded by the Ministry of Education (MOE) (2021RIS-004). This research used resources of the of the Advanced Photon Source and Center for Nanoscale Materials, a DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract DE-AC02-06CH11357. The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory (“Argonne”). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract DE-AC02-06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up, nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government.

Keywords

Fe substitution
air storage
iron (Fe) cathode
layered cathode
sodium-ion batteries

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10.1021/acsami.3c07068

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title = "Multifunctional Effect of Fe Substitution in Na Layered Cathode Materials for Enhanced Storage Stability",

abstract = "Developing stable cathode materials that are resistant to storage degradation is essential for practical development and industrial processing of Na-ion batteries as many sodium layered oxide materials are susceptible to hygroscopicity and instability upon exposure to ambient air. Among the various layered compounds, Fe-substituted O3-type Na(Ni1/2Mn1/2)1-xFexO2 materials have emerged as a promising option for high-performance and low-cost cathodes. While previous reports have noted the decent air-storage stability of these materials, the role and origin of Fe substitution in improving storage stability remain unclear. In this study, we investigate the air-resistant effect of Fe substitution in O3-Na(Ni1/2Mn1/2)1-xFexO2 cathode materials by performing systematic surface and structural characterizations. We find that the improved storage stability can be attributed to the multifunctional effect of Fe substitution, which forms a surface protective layer containing an Fe-incorporated spinel phase and decreases the thermodynamical driving force for bulk chemical sodium extraction. With these mechanisms, Fe-containing cathodes can suppress the cascades of cathode degradation processes and better retain the electrochemical performance after air storage.",

keywords = "Fe substitution, air storage, iron (Fe) cathode, layered cathode, sodium-ion batteries",

author = "Jehee Park and Kyojin Ku and Jihyeon Gim and Son, \{Seoung Bum\} and Heonjae Jeong and Lei Cheng and Hakim Iddir and Dewen Hou and Hui Xiong and Yuzi Liu and Eungje Lee and Christopher Johnson",

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doi = "10.1021/acsami.3c07068",

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T1 - Multifunctional Effect of Fe Substitution in Na Layered Cathode Materials for Enhanced Storage Stability

AU - Park, Jehee

AU - Ku, Kyojin

AU - Gim, Jihyeon

AU - Son, Seoung Bum

AU - Jeong, Heonjae

AU - Cheng, Lei

AU - Iddir, Hakim

AU - Hou, Dewen

AU - Xiong, Hui

AU - Liu, Yuzi

AU - Lee, Eungje

AU - Johnson, Christopher

PY - 2023/8/16

Y1 - 2023/8/16

N2 - Developing stable cathode materials that are resistant to storage degradation is essential for practical development and industrial processing of Na-ion batteries as many sodium layered oxide materials are susceptible to hygroscopicity and instability upon exposure to ambient air. Among the various layered compounds, Fe-substituted O3-type Na(Ni1/2Mn1/2)1-xFexO2 materials have emerged as a promising option for high-performance and low-cost cathodes. While previous reports have noted the decent air-storage stability of these materials, the role and origin of Fe substitution in improving storage stability remain unclear. In this study, we investigate the air-resistant effect of Fe substitution in O3-Na(Ni1/2Mn1/2)1-xFexO2 cathode materials by performing systematic surface and structural characterizations. We find that the improved storage stability can be attributed to the multifunctional effect of Fe substitution, which forms a surface protective layer containing an Fe-incorporated spinel phase and decreases the thermodynamical driving force for bulk chemical sodium extraction. With these mechanisms, Fe-containing cathodes can suppress the cascades of cathode degradation processes and better retain the electrochemical performance after air storage.

AB - Developing stable cathode materials that are resistant to storage degradation is essential for practical development and industrial processing of Na-ion batteries as many sodium layered oxide materials are susceptible to hygroscopicity and instability upon exposure to ambient air. Among the various layered compounds, Fe-substituted O3-type Na(Ni1/2Mn1/2)1-xFexO2 materials have emerged as a promising option for high-performance and low-cost cathodes. While previous reports have noted the decent air-storage stability of these materials, the role and origin of Fe substitution in improving storage stability remain unclear. In this study, we investigate the air-resistant effect of Fe substitution in O3-Na(Ni1/2Mn1/2)1-xFexO2 cathode materials by performing systematic surface and structural characterizations. We find that the improved storage stability can be attributed to the multifunctional effect of Fe substitution, which forms a surface protective layer containing an Fe-incorporated spinel phase and decreases the thermodynamical driving force for bulk chemical sodium extraction. With these mechanisms, Fe-containing cathodes can suppress the cascades of cathode degradation processes and better retain the electrochemical performance after air storage.

KW - Fe substitution

KW - air storage

KW - iron (Fe) cathode

KW - layered cathode

KW - sodium-ion batteries

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ER -

Multifunctional Effect of Fe Substitution in Na Layered Cathode Materials for Enhanced Storage Stability

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