Origin and regulation of oxygen redox instability in high-voltage battery cathodes

Xiang Liu; Gui Liang Xu; Venkata Surya Chaitanya Kolluru; Chen Zhao; Qingtian Li; Xinwei Zhou; Yuzi Liu; Liang Yin; Zengqing Zhuo; Amine Daali; Jing Jing Fan; Wenjun Liu; Yang Ren; Wenqian Xu; Junjing Deng; Inhui Hwang; Dongsheng Ren; Xuning Feng; Chengjun Sun; Ling Huang; Tao Zhou; Ming Du; Zonghai Chen; Shi Gang Sun; Maria K.Y. Chan; Wanli Yang; Minggao Ouyang; Khalil Amine

doi:10.1038/s41560-022-01036-3

Origin and regulation of oxygen redox instability in high-voltage battery cathodes

Xiang Liu, Gui Liang Xu^*, Venkata Surya Chaitanya Kolluru, Chen Zhao, Qingtian Li, Xinwei Zhou, Yuzi Liu, Liang Yin, Zengqing Zhuo, Amine Daali, Jing Jing Fan, Wenjun Liu, Yang Ren, Wenqian Xu, Junjing Deng, Inhui Hwang, Dongsheng Ren, Xuning Feng, Chengjun Sun, Ling HuangTao Zhou, Ming Du, Zonghai Chen, Shi Gang Sun, Maria K.Y. Chan, Wanli Yang^*, Minggao Ouyang^*, Khalil Amine^*

^*Corresponding author for this work

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

15 Scopus citations

Abstract

Oxygen redox at high voltage has emerged as a transformative paradigm for high-energy battery cathodes such as layered transition-metal oxides by offering extra capacity beyond conventional transition-metal redox. However, these cathodes suffer from voltage hysteresis, voltage fade and capacity drop upon cycling. Single-crystalline cathodes have recently shown some improvements, but these challenges remain. Here we reveal the fundamental origin of oxygen redox instability to be from the domain boundaries that are present in single-crystalline cathode particles. By investigating single-crystalline cathodes with different domain boundaries structures, we show that the elimination of domain boundaries enhances the reversible lattice oxygen redox while inhibiting the irreversible oxygen release. This leads to significantly suppressed structural degradation and improved mechanical integrity during battery cycling and abuse heating. The robust oxygen redox enabled through domain boundary control provides practical opportunities towards high-energy, long-cycling, safe batteries.

Original language	English (US)
Pages (from-to)	808-817
Number of pages	10
Journal	Nature Energy
Volume	7
Issue number	9
DOIs	https://doi.org/10.1038/s41560-022-01036-3
State	Published - Sep 2022
Externally published	Yes

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
Renewable Energy, Sustainability and the Environment
Fuel Technology
Energy Engineering and Power Technology

UN SDGs

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

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10.1038/s41560-022-01036-3

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Liu, X., Xu, G. L., Kolluru, V. S. C., Zhao, C., Li, Q., Zhou, X., Liu, Y., Yin, L., Zhuo, Z., Daali, A., Fan, J. J., Liu, W., Ren, Y., Xu, W., Deng, J., Hwang, I., Ren, D., Feng, X., Sun, C., ... Amine, K. (2022). Origin and regulation of oxygen redox instability in high-voltage battery cathodes. Nature Energy, 7(9), 808-817. https://doi.org/10.1038/s41560-022-01036-3

@article{1cabce3c02a1400784003a3d5f9e67ce,

title = "Origin and regulation of oxygen redox instability in high-voltage battery cathodes",

abstract = "Oxygen redox at high voltage has emerged as a transformative paradigm for high-energy battery cathodes such as layered transition-metal oxides by offering extra capacity beyond conventional transition-metal redox. However, these cathodes suffer from voltage hysteresis, voltage fade and capacity drop upon cycling. Single-crystalline cathodes have recently shown some improvements, but these challenges remain. Here we reveal the fundamental origin of oxygen redox instability to be from the domain boundaries that are present in single-crystalline cathode particles. By investigating single-crystalline cathodes with different domain boundaries structures, we show that the elimination of domain boundaries enhances the reversible lattice oxygen redox while inhibiting the irreversible oxygen release. This leads to significantly suppressed structural degradation and improved mechanical integrity during battery cycling and abuse heating. The robust oxygen redox enabled through domain boundary control provides practical opportunities towards high-energy, long-cycling, safe batteries.",

author = "Xiang Liu and Xu, {Gui Liang} and Kolluru, {Venkata Surya Chaitanya} and Chen Zhao and Qingtian Li and Xinwei Zhou and Yuzi Liu and Liang Yin and Zengqing Zhuo and Amine Daali and Fan, {Jing Jing} and Wenjun Liu and Yang Ren and Wenqian Xu and Junjing Deng and Inhui Hwang and Dongsheng Ren and Xuning Feng and Chengjun Sun and Ling Huang and Tao Zhou and Ming Du and Zonghai Chen and Sun, {Shi Gang} and Chan, {Maria K.Y.} and Wanli Yang and Minggao Ouyang and Khalil Amine",

note = "Funding Information: Research at the Argonne National Laboratory was funded by the US Department of Energy (DOE), Vehicle Technologies Office. Support from Tien Duong of the US DOE{\textquoteright}s Office of Vehicle Technologies Program is gratefully acknowledged. Use of the Advanced Photon Source (APS) and the Centre for Nanoscale Materials, both Office of Science user facilities, was supported by the US Department of Energy, Office of Science and Office of Basic Energy Sciences, under contract no. DE-AC02-06CH11357. Soft X-ray spectroscopy experiments were performed at the Advanced Light Source of the Lawrence Berkeley National Laboratory, a U.S. DOE Office of Science User Facility under contract no. DE-AC02-05CH11231. X.L., G.-L.X., M.O. and K.A. thank the Clean Vehicle Consortium, US–China Clean Energy Research Centre (CERC-CVC2) for support. The authors thank G. Ceder for helpful discussion of DFT simulation on the OR behaviour of boundary-tailored layered cathodes, and B. Lai for technical support with ptychography characterization. Funding Information: Research at the Argonne National Laboratory was funded by the US Department of Energy (DOE), Vehicle Technologies Office. Support from Tien Duong of the US DOE{\textquoteright}s Office of Vehicle Technologies Program is gratefully acknowledged. Use of the Advanced Photon Source (APS) and the Centre for Nanoscale Materials, both Office of Science user facilities, was supported by the US Department of Energy, Office of Science and Office of Basic Energy Sciences, under contract no. DE-AC02-06CH11357. Soft X-ray spectroscopy experiments were performed at the Advanced Light Source of the Lawrence Berkeley National Laboratory, a U.S. DOE Office of Science User Facility under contract no. DE-AC02-05CH11231. X.L., G.-L.X., M.O. and K.A. thank the Clean Vehicle Consortium, US–China Clean Energy Research Centre (CERC-CVC2) for support. The authors thank G. Ceder for helpful discussion of DFT simulation on the OR behaviour of boundary-tailored layered cathodes, and B. Lai for technical support with ptychography characterization. Publisher Copyright: {\textcopyright} 2022, The Author(s), under exclusive licence to Springer Nature Limited.",

year = "2022",

month = sep,

doi = "10.1038/s41560-022-01036-3",

language = "English (US)",

volume = "7",

pages = "808--817",

journal = "Nature Energy",

issn = "2058-7546",

publisher = "Springer Nature",

number = "9",

}

Liu, X, Xu, GL, Kolluru, VSC, Zhao, C, Li, Q, Zhou, X, Liu, Y, Yin, L, Zhuo, Z, Daali, A, Fan, JJ, Liu, W, Ren, Y, Xu, W, Deng, J, Hwang, I, Ren, D, Feng, X, Sun, C, Huang, L, Zhou, T, Du, M, Chen, Z, Sun, SG, Chan, MKY, Yang, W, Ouyang, M & Amine, K 2022, 'Origin and regulation of oxygen redox instability in high-voltage battery cathodes', Nature Energy, vol. 7, no. 9, pp. 808-817. https://doi.org/10.1038/s41560-022-01036-3

TY - JOUR

T1 - Origin and regulation of oxygen redox instability in high-voltage battery cathodes

AU - Liu, Xiang

AU - Xu, Gui Liang

AU - Kolluru, Venkata Surya Chaitanya

AU - Zhao, Chen

AU - Li, Qingtian

AU - Zhou, Xinwei

AU - Liu, Yuzi

AU - Yin, Liang

AU - Zhuo, Zengqing

AU - Daali, Amine

AU - Fan, Jing Jing

AU - Liu, Wenjun

AU - Ren, Yang

AU - Xu, Wenqian

AU - Deng, Junjing

AU - Hwang, Inhui

AU - Ren, Dongsheng

AU - Feng, Xuning

AU - Sun, Chengjun

AU - Huang, Ling

AU - Zhou, Tao

AU - Du, Ming

AU - Chen, Zonghai

AU - Sun, Shi Gang

AU - Chan, Maria K.Y.

AU - Yang, Wanli

AU - Ouyang, Minggao

AU - Amine, Khalil

N1 - Funding Information: Research at the Argonne National Laboratory was funded by the US Department of Energy (DOE), Vehicle Technologies Office. Support from Tien Duong of the US DOE’s Office of Vehicle Technologies Program is gratefully acknowledged. Use of the Advanced Photon Source (APS) and the Centre for Nanoscale Materials, both Office of Science user facilities, was supported by the US Department of Energy, Office of Science and Office of Basic Energy Sciences, under contract no. DE-AC02-06CH11357. Soft X-ray spectroscopy experiments were performed at the Advanced Light Source of the Lawrence Berkeley National Laboratory, a U.S. DOE Office of Science User Facility under contract no. DE-AC02-05CH11231. X.L., G.-L.X., M.O. and K.A. thank the Clean Vehicle Consortium, US–China Clean Energy Research Centre (CERC-CVC2) for support. The authors thank G. Ceder for helpful discussion of DFT simulation on the OR behaviour of boundary-tailored layered cathodes, and B. Lai for technical support with ptychography characterization. Funding Information: Research at the Argonne National Laboratory was funded by the US Department of Energy (DOE), Vehicle Technologies Office. Support from Tien Duong of the US DOE’s Office of Vehicle Technologies Program is gratefully acknowledged. Use of the Advanced Photon Source (APS) and the Centre for Nanoscale Materials, both Office of Science user facilities, was supported by the US Department of Energy, Office of Science and Office of Basic Energy Sciences, under contract no. DE-AC02-06CH11357. Soft X-ray spectroscopy experiments were performed at the Advanced Light Source of the Lawrence Berkeley National Laboratory, a U.S. DOE Office of Science User Facility under contract no. DE-AC02-05CH11231. X.L., G.-L.X., M.O. and K.A. thank the Clean Vehicle Consortium, US–China Clean Energy Research Centre (CERC-CVC2) for support. The authors thank G. Ceder for helpful discussion of DFT simulation on the OR behaviour of boundary-tailored layered cathodes, and B. Lai for technical support with ptychography characterization. Publisher Copyright: © 2022, The Author(s), under exclusive licence to Springer Nature Limited.

PY - 2022/9

Y1 - 2022/9

N2 - Oxygen redox at high voltage has emerged as a transformative paradigm for high-energy battery cathodes such as layered transition-metal oxides by offering extra capacity beyond conventional transition-metal redox. However, these cathodes suffer from voltage hysteresis, voltage fade and capacity drop upon cycling. Single-crystalline cathodes have recently shown some improvements, but these challenges remain. Here we reveal the fundamental origin of oxygen redox instability to be from the domain boundaries that are present in single-crystalline cathode particles. By investigating single-crystalline cathodes with different domain boundaries structures, we show that the elimination of domain boundaries enhances the reversible lattice oxygen redox while inhibiting the irreversible oxygen release. This leads to significantly suppressed structural degradation and improved mechanical integrity during battery cycling and abuse heating. The robust oxygen redox enabled through domain boundary control provides practical opportunities towards high-energy, long-cycling, safe batteries.

AB - Oxygen redox at high voltage has emerged as a transformative paradigm for high-energy battery cathodes such as layered transition-metal oxides by offering extra capacity beyond conventional transition-metal redox. However, these cathodes suffer from voltage hysteresis, voltage fade and capacity drop upon cycling. Single-crystalline cathodes have recently shown some improvements, but these challenges remain. Here we reveal the fundamental origin of oxygen redox instability to be from the domain boundaries that are present in single-crystalline cathode particles. By investigating single-crystalline cathodes with different domain boundaries structures, we show that the elimination of domain boundaries enhances the reversible lattice oxygen redox while inhibiting the irreversible oxygen release. This leads to significantly suppressed structural degradation and improved mechanical integrity during battery cycling and abuse heating. The robust oxygen redox enabled through domain boundary control provides practical opportunities towards high-energy, long-cycling, safe batteries.

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U2 - 10.1038/s41560-022-01036-3

DO - 10.1038/s41560-022-01036-3

M3 - Article

AN - SCOPUS:85131319722

SN - 2058-7546

VL - 7

SP - 808

EP - 817

JO - Nature Energy

JF - Nature Energy

IS - 9

ER -

Origin and regulation of oxygen redox instability in high-voltage battery cathodes

Abstract

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