Interfacial Design for a 4.6 V High-Voltage Single-Crystalline LiCoO2 Cathode

Jiaxun Zhang; Peng-Fei Wang; Panxing Bai; Hongli Wan; Sufu Liu; Singyuk Hou; Xiangjun Pu; Jiale Xia; Weiran Zhang; Zeyi Wang; Bo Nan; Xiyue Zhang; Jijian Xu; Chunsheng Wang

doi:10.1002/adma.202108353

Interfacial Design for a 4.6 V High-Voltage Single-Crystalline LiCoO₂ Cathode

Jiaxun Zhang, Peng-Fei Wang, Panxing Bai, Hongli Wan, Sufu Liu, Singyuk Hou, Xiangjun Pu, Jiale Xia, Weiran Zhang, Zeyi Wang, Bo Nan, Xiyue Zhang, Jijian Xu^*, Chunsheng Wang^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

211 Citations (Scopus)

Abstract

Single-crystalline cathode materials have attracted intensive interest in offering greater capacity retention than their polycrystalline counterparts by reducing material surfaces and phase boundaries. However, the single-crystalline LiCoO₂ suffers severe structural instability and capacity fading when charged to high voltages (4.6 V) due to Co element dissolution and O loss, crack formation, and subsequent electrolyte penetration. Herein, by forming a robust cathode electrolyte interphase (CEI) in an all-fluorinated electrolyte, reversible planar gliding along the (003) plane in a single-crystalline LiCoO₂ cathode is protected due to the prevention of element dissolution and electrolyte penetration. The robust CEI effectively controls the performance fading issue of the single-crystalline cathode at a high operating voltage of 4.6 V, providing new insights for improved electrolyte design of high-energy-density battery cathode materials. © 2022 Wiley-VCH GmbH

Original language	English
Article number	2108353
Journal	Advanced Materials
Volume	34
Issue number	8
Online published	8 Dec 2021
DOIs	https://doi.org/10.1002/adma.202108353
Publication status	Published - 24 Feb 2022
Externally published	Yes

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Research Keywords

high-voltage LiCoO 2 cathodes
inorganic-rich cathode electrolyte interphase
nonflammable electrolytes
single-crystalline cathodes

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Cite this

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title = "Interfacial Design for a 4.6 V High-Voltage Single-Crystalline LiCoO2 Cathode",

abstract = "Single-crystalline cathode materials have attracted intensive interest in offering greater capacity retention than their polycrystalline counterparts by reducing material surfaces and phase boundaries. However, the single-crystalline LiCoO2 suffers severe structural instability and capacity fading when charged to high voltages (4.6 V) due to Co element dissolution and O loss, crack formation, and subsequent electrolyte penetration. Herein, by forming a robust cathode electrolyte interphase (CEI) in an all-fluorinated electrolyte, reversible planar gliding along the (003) plane in a single-crystalline LiCoO2 cathode is protected due to the prevention of element dissolution and electrolyte penetration. The robust CEI effectively controls the performance fading issue of the single-crystalline cathode at a high operating voltage of 4.6 V, providing new insights for improved electrolyte design of high-energy-density battery cathode materials. {\textcopyright} 2022 Wiley-VCH GmbH",

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author = "Jiaxun Zhang and Peng-Fei Wang and Panxing Bai and Hongli Wan and Sufu Liu and Singyuk Hou and Xiangjun Pu and Jiale Xia and Weiran Zhang and Zeyi Wang and Bo Nan and Xiyue Zhang and Jijian Xu and Chunsheng Wang",

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T1 - Interfacial Design for a 4.6 V High-Voltage Single-Crystalline LiCoO2 Cathode

AU - Zhang, Jiaxun

AU - Wang, Peng-Fei

AU - Bai, Panxing

AU - Wan, Hongli

AU - Liu, Sufu

AU - Hou, Singyuk

AU - Pu, Xiangjun

AU - Xia, Jiale

AU - Zhang, Weiran

AU - Wang, Zeyi

AU - Nan, Bo

AU - Zhang, Xiyue

AU - Xu, Jijian

AU - Wang, Chunsheng

PY - 2022/2/24

Y1 - 2022/2/24

N2 - Single-crystalline cathode materials have attracted intensive interest in offering greater capacity retention than their polycrystalline counterparts by reducing material surfaces and phase boundaries. However, the single-crystalline LiCoO2 suffers severe structural instability and capacity fading when charged to high voltages (4.6 V) due to Co element dissolution and O loss, crack formation, and subsequent electrolyte penetration. Herein, by forming a robust cathode electrolyte interphase (CEI) in an all-fluorinated electrolyte, reversible planar gliding along the (003) plane in a single-crystalline LiCoO2 cathode is protected due to the prevention of element dissolution and electrolyte penetration. The robust CEI effectively controls the performance fading issue of the single-crystalline cathode at a high operating voltage of 4.6 V, providing new insights for improved electrolyte design of high-energy-density battery cathode materials. © 2022 Wiley-VCH GmbH

AB - Single-crystalline cathode materials have attracted intensive interest in offering greater capacity retention than their polycrystalline counterparts by reducing material surfaces and phase boundaries. However, the single-crystalline LiCoO2 suffers severe structural instability and capacity fading when charged to high voltages (4.6 V) due to Co element dissolution and O loss, crack formation, and subsequent electrolyte penetration. Herein, by forming a robust cathode electrolyte interphase (CEI) in an all-fluorinated electrolyte, reversible planar gliding along the (003) plane in a single-crystalline LiCoO2 cathode is protected due to the prevention of element dissolution and electrolyte penetration. The robust CEI effectively controls the performance fading issue of the single-crystalline cathode at a high operating voltage of 4.6 V, providing new insights for improved electrolyte design of high-energy-density battery cathode materials. © 2022 Wiley-VCH GmbH

KW - high-voltage LiCoO 2 cathodes

KW - inorganic-rich cathode electrolyte interphase

KW - nonflammable electrolytes

KW - single-crystalline cathodes

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DO - 10.1002/adma.202108353

M3 - RGC 21 - Publication in refereed journal

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