Ultra-high-voltage Ni-rich layered cathodes in practical Li metal batteries enabled by a sulfonamide-based electrolyte

Weijiang Xue; Mingjun Huang; Yutao Li; Yun Guang Zhu; Rui Gao; Xianghui Xiao; Wenxu Zhang; Sipei Li; Guiyin Xu; Yang Yu; Peng Li; Jeffrey Lopez; Daiwei Yu; Yanhao Dong; Weiwei Fan; Zhe Shi; Rui Xiong; Cheng Jun Sun; Inhui Hwang; Wah Keat Lee; Yang Shao-Horn; Jeremiah A. Johnson; Ju Li

doi:10.1038/s41560-021-00792-y

Ultra-high-voltage Ni-rich layered cathodes in practical Li metal batteries enabled by a sulfonamide-based electrolyte

Weijiang Xue, Mingjun Huang, Yutao Li, Yun Guang Zhu, Rui Gao, Xianghui Xiao, Wenxu Zhang, Sipei Li, Guiyin Xu, Yang Yu, Peng Li, Jeffrey Lopez, Daiwei Yu, Yanhao Dong^*, Weiwei Fan, Zhe Shi, Rui Xiong, Cheng Jun Sun, Inhui Hwang, Wah Keat LeeYang Shao-Horn^*, Jeremiah A. Johnson^*, Ju Li^*

^*Corresponding author for this work

School of Mechanical Engineering

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

456 Citations (Scopus)

Abstract

By increasing the charging voltage, a cell specific energy of >400 W h kg⁻¹ is achievable with LiNi_0.8Mn_0.1Co_0.1O₂ in Li metal batteries. However, stable cycling of high-nickel cathodes at ultra-high voltages is extremely challenging. Here we report that a rationally designed sulfonamide-based electrolyte enables stable cycling of commercial LiNi_0.8Co_0.1Mn_0.1O₂ with a cut-off voltage up to 4.7 V in Li metal batteries. In contrast to commercial carbonate electrolytes, the electrolyte not only suppresses side reactions, stress-corrosion cracking, transition-metal dissolution and impedance growth on the cathode side, but also enables highly reversible Li metal stripping and plating leading to a compact morphology and low pulverization. Our lithium-metal battery delivers a specific capacity >230 mA h g⁻¹ and an average Coulombic efficiency >99.65% over 100 cycles. Even under harsh testing conditions, the 4.7 V lithium-metal battery can retain >88% capacity for 90 cycles, advancing practical lithium-metal batteries.

Original language	English
Pages (from-to)	495-505
Number of pages	11
Journal	Nature Energy
Volume	6
Issue number	5
DOIs	https://doi.org/10.1038/s41560-021-00792-y
Publication status	Published - May 2021

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Xue, W., Huang, M., Li, Y., Zhu, Y. G., Gao, R., Xiao, X., Zhang, W., Li, S., Xu, G., Yu, Y., Li, P., Lopez, J., Yu, D., Dong, Y., Fan, W., Shi, Z., Xiong, R., Sun, C. J., Hwang, I., ... Li, J. (2021). Ultra-high-voltage Ni-rich layered cathodes in practical Li metal batteries enabled by a sulfonamide-based electrolyte. Nature Energy, 6(5), 495-505. https://doi.org/10.1038/s41560-021-00792-y

@article{bcaa61b3407942248ba9377a6b652f7e,

title = "Ultra-high-voltage Ni-rich layered cathodes in practical Li metal batteries enabled by a sulfonamide-based electrolyte",

abstract = "By increasing the charging voltage, a cell specific energy of >400 W h kg−1 is achievable with LiNi0.8Mn0.1Co0.1O2 in Li metal batteries. However, stable cycling of high-nickel cathodes at ultra-high voltages is extremely challenging. Here we report that a rationally designed sulfonamide-based electrolyte enables stable cycling of commercial LiNi0.8Co0.1Mn0.1O2 with a cut-off voltage up to 4.7 V in Li metal batteries. In contrast to commercial carbonate electrolytes, the electrolyte not only suppresses side reactions, stress-corrosion cracking, transition-metal dissolution and impedance growth on the cathode side, but also enables highly reversible Li metal stripping and plating leading to a compact morphology and low pulverization. Our lithium-metal battery delivers a specific capacity >230 mA h g−1 and an average Coulombic efficiency >99.65% over 100 cycles. Even under harsh testing conditions, the 4.7 V lithium-metal battery can retain >88% capacity for 90 cycles, advancing practical lithium-metal batteries.",

author = "Weijiang Xue and Mingjun Huang and Yutao Li and Zhu, {Yun Guang} and Rui Gao and Xianghui Xiao and Wenxu Zhang and Sipei Li and Guiyin Xu and Yang Yu and Peng Li and Jeffrey Lopez and Daiwei Yu and Yanhao Dong and Weiwei Fan and Zhe Shi and Rui Xiong and Sun, {Cheng Jun} and Inhui Hwang and Lee, {Wah Keat} and Yang Shao-Horn and Johnson, {Jeremiah A.} and Ju Li",

note = "Publisher Copyright: {\textcopyright} 2021, The Author(s), under exclusive licence to Springer Nature Limited.",

year = "2021",

month = may,

doi = "10.1038/s41560-021-00792-y",

language = "English",

volume = "6",

pages = "495--505",

journal = "Nature Energy",

issn = "2058-7546",

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number = "5",

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Xue, W, Huang, M, Li, Y, Zhu, YG, Gao, R, Xiao, X, Zhang, W, Li, S, Xu, G, Yu, Y, Li, P, Lopez, J, Yu, D, Dong, Y, Fan, W, Shi, Z, Xiong, R, Sun, CJ, Hwang, I, Lee, WK, Shao-Horn, Y, Johnson, JA & Li, J 2021, 'Ultra-high-voltage Ni-rich layered cathodes in practical Li metal batteries enabled by a sulfonamide-based electrolyte', Nature Energy, vol. 6, no. 5, pp. 495-505. https://doi.org/10.1038/s41560-021-00792-y

TY - JOUR

T1 - Ultra-high-voltage Ni-rich layered cathodes in practical Li metal batteries enabled by a sulfonamide-based electrolyte

AU - Xue, Weijiang

AU - Huang, Mingjun

AU - Li, Yutao

AU - Zhu, Yun Guang

AU - Gao, Rui

AU - Xiao, Xianghui

AU - Zhang, Wenxu

AU - Li, Sipei

AU - Xu, Guiyin

AU - Yu, Yang

AU - Li, Peng

AU - Lopez, Jeffrey

AU - Yu, Daiwei

AU - Dong, Yanhao

AU - Fan, Weiwei

AU - Shi, Zhe

AU - Xiong, Rui

AU - Sun, Cheng Jun

AU - Hwang, Inhui

AU - Lee, Wah Keat

AU - Shao-Horn, Yang

AU - Johnson, Jeremiah A.

AU - Li, Ju

PY - 2021/5

Y1 - 2021/5

N2 - By increasing the charging voltage, a cell specific energy of >400 W h kg−1 is achievable with LiNi0.8Mn0.1Co0.1O2 in Li metal batteries. However, stable cycling of high-nickel cathodes at ultra-high voltages is extremely challenging. Here we report that a rationally designed sulfonamide-based electrolyte enables stable cycling of commercial LiNi0.8Co0.1Mn0.1O2 with a cut-off voltage up to 4.7 V in Li metal batteries. In contrast to commercial carbonate electrolytes, the electrolyte not only suppresses side reactions, stress-corrosion cracking, transition-metal dissolution and impedance growth on the cathode side, but also enables highly reversible Li metal stripping and plating leading to a compact morphology and low pulverization. Our lithium-metal battery delivers a specific capacity >230 mA h g−1 and an average Coulombic efficiency >99.65% over 100 cycles. Even under harsh testing conditions, the 4.7 V lithium-metal battery can retain >88% capacity for 90 cycles, advancing practical lithium-metal batteries.

AB - By increasing the charging voltage, a cell specific energy of >400 W h kg−1 is achievable with LiNi0.8Mn0.1Co0.1O2 in Li metal batteries. However, stable cycling of high-nickel cathodes at ultra-high voltages is extremely challenging. Here we report that a rationally designed sulfonamide-based electrolyte enables stable cycling of commercial LiNi0.8Co0.1Mn0.1O2 with a cut-off voltage up to 4.7 V in Li metal batteries. In contrast to commercial carbonate electrolytes, the electrolyte not only suppresses side reactions, stress-corrosion cracking, transition-metal dissolution and impedance growth on the cathode side, but also enables highly reversible Li metal stripping and plating leading to a compact morphology and low pulverization. Our lithium-metal battery delivers a specific capacity >230 mA h g−1 and an average Coulombic efficiency >99.65% over 100 cycles. Even under harsh testing conditions, the 4.7 V lithium-metal battery can retain >88% capacity for 90 cycles, advancing practical lithium-metal batteries.

UR - http://www.scopus.com/inward/record.url?scp=85103198421&partnerID=8YFLogxK

U2 - 10.1038/s41560-021-00792-y

DO - 10.1038/s41560-021-00792-y

M3 - Article

AN - SCOPUS:85103198421

SN - 2058-7546

VL - 6

SP - 495

EP - 505

JO - Nature Energy

JF - Nature Energy

IS - 5

ER -

Ultra-high-voltage Ni-rich layered cathodes in practical Li metal batteries enabled by a sulfonamide-based electrolyte

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