Reviving the rock-salt phases in Ni-rich layered cathodes by mechano-electrochemistry in all-solid-state batteries

Zaifa Wang; Zhenyu Wang; Dingchuan Xue; Jun Zhao; Xuedong Zhang; Lin Geng; Yanshuai Li; Congcong Du; Marnix Wagemaker; null More Authors

doi:10.1016/j.nanoen.2022.108016

Reviving the rock-salt phases in Ni-rich layered cathodes by mechano-electrochemistry in all-solid-state batteries

Zaifa Wang, Zhenyu Wang, Dingchuan Xue, Jun Zhao, Xuedong Zhang, Lin Geng, Yanshuai Li, Congcong Du, Marnix Wagemaker, More Authors

RST/Storage of Electrochemical Energy

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

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Abstract

The rock-salt phase (RSP) formed on the surface of Ni-rich layered cathodes in liquid-electrolyte lithium-ion batteries is conceived to be electrochemically "dead". Here we show massive RSP forms in the interior of LiNi_xMn_yCo_(1−x-y)O₂ (NMC) crystals in sulfide based all solid state batteries (ASSBs), but the RSP remains electrochemically active even after long cycles. The RSP and the layered structure constitute a two-phase mixture, a material architecture that is distinctly different from the RSP in liquid electrolytes. The tensioned layered phase affords an effective percolation channel into which lithium is squeezed out of the RSPs by compressive stress, rendering the RSPs electrochemically active. Consequently, the ASSBs with predominant RSP in the NMC cathode deliver remarkable long cycle life of 4000 cycles at high areal capacity of 4.3 mAh/cm². Our study unveils distinct mechano-electrochemistry of RSPs in ASSBs that can be harnessed to enable high energy density and durable ASSBs.

Original language	English
Article number	108016
Number of pages	10
Journal	Nano Energy
Volume	105
DOIs	https://doi.org/10.1016/j.nanoen.2022.108016
Publication status	Published - 2023

Bibliographical note

Green Open Access added to TU Delft Institutional Repository ‘You share, we take care!’ – Taverne project https://www.openaccess.nl/en/you-share-we-take-care Otherwise as indicated in the copyright section: the publisher is the copyright holder of this work and the author uses the Dutch legislation to make this work public.

Keywords

All-solid-state batteries
Mechano-electrochemistry
Ni-rich cathodes
Rock-salt phases

UN SDGs

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

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10.1016/j.nanoen.2022.108016

1-s2.0-S2211285522010941-mainFinal published version, 9.51 MB

Cite this

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title = "Reviving the rock-salt phases in Ni-rich layered cathodes by mechano-electrochemistry in all-solid-state batteries",

abstract = "The rock-salt phase (RSP) formed on the surface of Ni-rich layered cathodes in liquid-electrolyte lithium-ion batteries is conceived to be electrochemically {"}dead{"}. Here we show massive RSP forms in the interior of LiNixMnyCo(1−x-y)O2 (NMC) crystals in sulfide based all solid state batteries (ASSBs), but the RSP remains electrochemically active even after long cycles. The RSP and the layered structure constitute a two-phase mixture, a material architecture that is distinctly different from the RSP in liquid electrolytes. The tensioned layered phase affords an effective percolation channel into which lithium is squeezed out of the RSPs by compressive stress, rendering the RSPs electrochemically active. Consequently, the ASSBs with predominant RSP in the NMC cathode deliver remarkable long cycle life of 4000 cycles at high areal capacity of 4.3 mAh/cm2. Our study unveils distinct mechano-electrochemistry of RSPs in ASSBs that can be harnessed to enable high energy density and durable ASSBs.",

keywords = "All-solid-state batteries, Mechano-electrochemistry, Ni-rich cathodes, Rock-salt phases",

author = "Zaifa Wang and Zhenyu Wang and Dingchuan Xue and Jun Zhao and Xuedong Zhang and Lin Geng and Yanshuai Li and Congcong Du and Marnix Wagemaker and {More Authors}",

note = "Green Open Access added to TU Delft Institutional Repository {\textquoteleft}You share, we take care!{\textquoteright} – Taverne project https://www.openaccess.nl/en/you-share-we-take-care Otherwise as indicated in the copyright section: the publisher is the copyright holder of this work and the author uses the Dutch legislation to make this work public. ",

year = "2023",

doi = "10.1016/j.nanoen.2022.108016",

language = "English",

volume = "105",

journal = "Nano Energy",

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TY - JOUR

T1 - Reviving the rock-salt phases in Ni-rich layered cathodes by mechano-electrochemistry in all-solid-state batteries

AU - Wang, Zaifa

AU - Wang, Zhenyu

AU - Xue, Dingchuan

AU - Zhao, Jun

AU - Zhang, Xuedong

AU - Geng, Lin

AU - Li, Yanshuai

AU - Du, Congcong

AU - Wagemaker, Marnix

AU - More Authors, null

N1 - Green Open Access added to TU Delft Institutional Repository ‘You share, we take care!’ – Taverne project https://www.openaccess.nl/en/you-share-we-take-care Otherwise as indicated in the copyright section: the publisher is the copyright holder of this work and the author uses the Dutch legislation to make this work public.

PY - 2023

Y1 - 2023

N2 - The rock-salt phase (RSP) formed on the surface of Ni-rich layered cathodes in liquid-electrolyte lithium-ion batteries is conceived to be electrochemically "dead". Here we show massive RSP forms in the interior of LiNixMnyCo(1−x-y)O2 (NMC) crystals in sulfide based all solid state batteries (ASSBs), but the RSP remains electrochemically active even after long cycles. The RSP and the layered structure constitute a two-phase mixture, a material architecture that is distinctly different from the RSP in liquid electrolytes. The tensioned layered phase affords an effective percolation channel into which lithium is squeezed out of the RSPs by compressive stress, rendering the RSPs electrochemically active. Consequently, the ASSBs with predominant RSP in the NMC cathode deliver remarkable long cycle life of 4000 cycles at high areal capacity of 4.3 mAh/cm2. Our study unveils distinct mechano-electrochemistry of RSPs in ASSBs that can be harnessed to enable high energy density and durable ASSBs.

AB - The rock-salt phase (RSP) formed on the surface of Ni-rich layered cathodes in liquid-electrolyte lithium-ion batteries is conceived to be electrochemically "dead". Here we show massive RSP forms in the interior of LiNixMnyCo(1−x-y)O2 (NMC) crystals in sulfide based all solid state batteries (ASSBs), but the RSP remains electrochemically active even after long cycles. The RSP and the layered structure constitute a two-phase mixture, a material architecture that is distinctly different from the RSP in liquid electrolytes. The tensioned layered phase affords an effective percolation channel into which lithium is squeezed out of the RSPs by compressive stress, rendering the RSPs electrochemically active. Consequently, the ASSBs with predominant RSP in the NMC cathode deliver remarkable long cycle life of 4000 cycles at high areal capacity of 4.3 mAh/cm2. Our study unveils distinct mechano-electrochemistry of RSPs in ASSBs that can be harnessed to enable high energy density and durable ASSBs.

KW - All-solid-state batteries

KW - Mechano-electrochemistry

KW - Ni-rich cathodes

KW - Rock-salt phases

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VL - 105

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ER -

Reviving the rock-salt phases in Ni-rich layered cathodes by mechano-electrochemistry in all-solid-state batteries

Abstract

Bibliographical note

Keywords

UN SDGs

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