Conformal PEDOT Coating Enables Ultra-High-Voltage and High-Temperature Operation for Single-Crystal Ni-Rich Cathodes

Qiang Liu; Yutong Liu; Chen Zhao; Qingsong Weng; Junjing Deng; Inhui Hwang; Yi Jiang; Chengjun Sun; Tianyi Li; Wenqian Xu; Ke Du; Amine Daali; Gui Liang Xu; Khalil Amine; Guohua Chen

doi:10.1021/acsnano.2c04959

Conformal PEDOT Coating Enables Ultra-High-Voltage and High-Temperature Operation for Single-Crystal Ni-Rich Cathodes

Qiang Liu, Yutong Liu, Chen Zhao, Qingsong Weng, Junjing Deng, Inhui Hwang, Yi Jiang, Chengjun Sun, Tianyi Li, Wenqian Xu, Ke Du, Amine Daali, Gui Liang Xu, Khalil Amine, Guohua Chen

Research output: Journal article publication › Journal article › Academic research › peer-review

33 Citations (Scopus)

Abstract

Single-crystal Ni-rich Li[Ni _xMn _yCo _1-x-y]O ₂(SC-NMC) cathodes represent a promising approach to mitigate the cracking issue of conventional polycrystalline cathodes. However, many reported SC-NMC cathodes still suffer from unsatisfactory cycling stability, particularly under high charge cutoff voltage and/or elevated temperature. Herein, we report an ultraconformal and durable poly(3,4-ethylenedioxythiophene) (PEDOT) coating for SC-NMC cathodes using an oxidative chemical vapor deposition (oCVD) technique, which significantly improves their high-voltage (4.6 V) and high-temperature operation resiliency. The PEDOT coated SC LiNi _0.83Mn _0.1Co _0.07O ₂(SC-NMC83) delivers an impressive capacity retention rate of 96.7% and 89.5% after 100 and 200 cycles, respectively. Significantly, even after calendar aging at 45 °C and 4.6 V, the coated cathode can still retain 85.3% (in comparison with 59.6% for the bare one) of the initial capacity after 100 cycles at a 0.5 C rate. Synchrotron X-ray experiments and interface characterization collectively reveal that the conformal PEDOT coating not only effectively stabilizes the crystallographic structure and maintains the integrity of the particles but also significantly suppresses the electrolyte's corrosion, resulting in improved electrochemical/thermal stability. Our findings highlight the promise of an oCVD PEDOT coating for single-crystal Ni-rich cathodes to meet the grand challenge of high-energy batteries under extreme conditions.

Original language	English
Pages (from-to)	14527-14538
Number of pages	12
Journal	ACS Nano
Volume	16
Issue number	9
DOIs	https://doi.org/10.1021/acsnano.2c04959
Publication status	Published - 27 Sept 2022

Keywords

Ni-rich NMC
conformal PEDOT coating
high-temperature
high-voltage
oCVD
single-crystal

ASJC Scopus subject areas

General Engineering
General Physics and Astronomy
General Materials Science

More information

10.1021/acsnano.2c04959

Cite this

@article{54db92b1f8e94d9f828684d939c0aa25,

title = "Conformal PEDOT Coating Enables Ultra-High-Voltage and High-Temperature Operation for Single-Crystal Ni-Rich Cathodes",

abstract = "Single-crystal Ni-rich Li[Ni xMn yCo 1-x-y]O 2(SC-NMC) cathodes represent a promising approach to mitigate the cracking issue of conventional polycrystalline cathodes. However, many reported SC-NMC cathodes still suffer from unsatisfactory cycling stability, particularly under high charge cutoff voltage and/or elevated temperature. Herein, we report an ultraconformal and durable poly(3,4-ethylenedioxythiophene) (PEDOT) coating for SC-NMC cathodes using an oxidative chemical vapor deposition (oCVD) technique, which significantly improves their high-voltage (4.6 V) and high-temperature operation resiliency. The PEDOT coated SC LiNi 0.83Mn 0.1Co 0.07O 2(SC-NMC83) delivers an impressive capacity retention rate of 96.7% and 89.5% after 100 and 200 cycles, respectively. Significantly, even after calendar aging at 45 °C and 4.6 V, the coated cathode can still retain 85.3% (in comparison with 59.6% for the bare one) of the initial capacity after 100 cycles at a 0.5 C rate. Synchrotron X-ray experiments and interface characterization collectively reveal that the conformal PEDOT coating not only effectively stabilizes the crystallographic structure and maintains the integrity of the particles but also significantly suppresses the electrolyte's corrosion, resulting in improved electrochemical/thermal stability. Our findings highlight the promise of an oCVD PEDOT coating for single-crystal Ni-rich cathodes to meet the grand challenge of high-energy batteries under extreme conditions.",

keywords = "Ni-rich NMC, conformal PEDOT coating, high-temperature, high-voltage, oCVD, single-crystal",

author = "Qiang Liu and Yutong Liu and Chen Zhao and Qingsong Weng and Junjing Deng and Inhui Hwang and Yi Jiang and Chengjun Sun and Tianyi Li and Wenqian Xu and Ke Du and Amine Daali and Xu, {Gui Liang} and Khalil Amine and Guohua Chen",

note = "Funding Information: Research at the Hong Kong Polytechnic University (HK PolyU) was funded by the Hong Kong Research Grants Council (GRF 15221719), Otto Poon Charitable Foundation (847W), The Hong Kong Polytechnic University (Start-up Fund for New Recruits of Mechanical Engineering, P0034050), and the Research Institute for Smart Energy (RISE project, P0034521). The financial support from Shenzhen Science and Technology Program (Grant RCBS20200714114920129 and Grant 201908163000519) and GDSTC-Guangdong-HK-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices (GDSTC 2019B121205001) is gratefully acknowledged. Research at Argonne National Laboratory was funded by the U.S. Department of Energy (DOE) Vehicle Technologies Office. Use of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the U.S. DOE under Contract DE-AC02-06CH11357. G.-L.X. and K.A. acknowledge the support of the U.S. China Clean Energy Research Center (CERC-CVC2). K.A. acknowledges the support from Army Research Laboratory under Cooperative Agreement W911NF-20-2-0284 and W911NF-22-2-0021. Publisher Copyright: {\textcopyright} 2022 American Chemical Society. All rights reserved.",

year = "2022",

month = sep,

day = "27",

doi = "10.1021/acsnano.2c04959",

language = "English",

volume = "16",

pages = "14527--14538",

journal = "ACS Nano",

issn = "1936-0851",

publisher = "American Chemical Society",

number = "9",

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TY - JOUR

T1 - Conformal PEDOT Coating Enables Ultra-High-Voltage and High-Temperature Operation for Single-Crystal Ni-Rich Cathodes

AU - Liu, Qiang

AU - Liu, Yutong

AU - Zhao, Chen

AU - Weng, Qingsong

AU - Deng, Junjing

AU - Hwang, Inhui

AU - Jiang, Yi

AU - Sun, Chengjun

AU - Li, Tianyi

AU - Xu, Wenqian

AU - Du, Ke

AU - Daali, Amine

AU - Xu, Gui Liang

AU - Amine, Khalil

AU - Chen, Guohua

N1 - Funding Information: Research at the Hong Kong Polytechnic University (HK PolyU) was funded by the Hong Kong Research Grants Council (GRF 15221719), Otto Poon Charitable Foundation (847W), The Hong Kong Polytechnic University (Start-up Fund for New Recruits of Mechanical Engineering, P0034050), and the Research Institute for Smart Energy (RISE project, P0034521). The financial support from Shenzhen Science and Technology Program (Grant RCBS20200714114920129 and Grant 201908163000519) and GDSTC-Guangdong-HK-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices (GDSTC 2019B121205001) is gratefully acknowledged. Research at Argonne National Laboratory was funded by the U.S. Department of Energy (DOE) Vehicle Technologies Office. Use of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the U.S. DOE under Contract DE-AC02-06CH11357. G.-L.X. and K.A. acknowledge the support of the U.S. China Clean Energy Research Center (CERC-CVC2). K.A. acknowledges the support from Army Research Laboratory under Cooperative Agreement W911NF-20-2-0284 and W911NF-22-2-0021. Publisher Copyright: © 2022 American Chemical Society. All rights reserved.

PY - 2022/9/27

Y1 - 2022/9/27

N2 - Single-crystal Ni-rich Li[Ni xMn yCo 1-x-y]O 2(SC-NMC) cathodes represent a promising approach to mitigate the cracking issue of conventional polycrystalline cathodes. However, many reported SC-NMC cathodes still suffer from unsatisfactory cycling stability, particularly under high charge cutoff voltage and/or elevated temperature. Herein, we report an ultraconformal and durable poly(3,4-ethylenedioxythiophene) (PEDOT) coating for SC-NMC cathodes using an oxidative chemical vapor deposition (oCVD) technique, which significantly improves their high-voltage (4.6 V) and high-temperature operation resiliency. The PEDOT coated SC LiNi 0.83Mn 0.1Co 0.07O 2(SC-NMC83) delivers an impressive capacity retention rate of 96.7% and 89.5% after 100 and 200 cycles, respectively. Significantly, even after calendar aging at 45 °C and 4.6 V, the coated cathode can still retain 85.3% (in comparison with 59.6% for the bare one) of the initial capacity after 100 cycles at a 0.5 C rate. Synchrotron X-ray experiments and interface characterization collectively reveal that the conformal PEDOT coating not only effectively stabilizes the crystallographic structure and maintains the integrity of the particles but also significantly suppresses the electrolyte's corrosion, resulting in improved electrochemical/thermal stability. Our findings highlight the promise of an oCVD PEDOT coating for single-crystal Ni-rich cathodes to meet the grand challenge of high-energy batteries under extreme conditions.

AB - Single-crystal Ni-rich Li[Ni xMn yCo 1-x-y]O 2(SC-NMC) cathodes represent a promising approach to mitigate the cracking issue of conventional polycrystalline cathodes. However, many reported SC-NMC cathodes still suffer from unsatisfactory cycling stability, particularly under high charge cutoff voltage and/or elevated temperature. Herein, we report an ultraconformal and durable poly(3,4-ethylenedioxythiophene) (PEDOT) coating for SC-NMC cathodes using an oxidative chemical vapor deposition (oCVD) technique, which significantly improves their high-voltage (4.6 V) and high-temperature operation resiliency. The PEDOT coated SC LiNi 0.83Mn 0.1Co 0.07O 2(SC-NMC83) delivers an impressive capacity retention rate of 96.7% and 89.5% after 100 and 200 cycles, respectively. Significantly, even after calendar aging at 45 °C and 4.6 V, the coated cathode can still retain 85.3% (in comparison with 59.6% for the bare one) of the initial capacity after 100 cycles at a 0.5 C rate. Synchrotron X-ray experiments and interface characterization collectively reveal that the conformal PEDOT coating not only effectively stabilizes the crystallographic structure and maintains the integrity of the particles but also significantly suppresses the electrolyte's corrosion, resulting in improved electrochemical/thermal stability. Our findings highlight the promise of an oCVD PEDOT coating for single-crystal Ni-rich cathodes to meet the grand challenge of high-energy batteries under extreme conditions.

KW - Ni-rich NMC

KW - conformal PEDOT coating

KW - high-temperature

KW - high-voltage

KW - oCVD

KW - single-crystal

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U2 - 10.1021/acsnano.2c04959

DO - 10.1021/acsnano.2c04959

M3 - Journal article

SN - 1936-0851

VL - 16

SP - 14527

EP - 14538

JO - ACS Nano

JF - ACS Nano

IS - 9

ER -

Conformal PEDOT Coating Enables Ultra-High-Voltage and High-Temperature Operation for Single-Crystal Ni-Rich Cathodes

Abstract

Keywords

ASJC Scopus subject areas

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