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

Qiang Liu; Yu-Tong Liu; Chen Zhao; Qing-Song 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^*, Yu-Tong Liu, Chen Zhao, Qing-Song Weng, Junjing Deng, Inhui Hwang, Yi Jiang, Chengjun Sun, Tianyi Li, Wenqian Xu, Ke Du, Amine Daali, Gui-Liang Xu^*, Khalil Amine^*, Guohua Chen^*

^*Corresponding author for this work

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

46 Citations (Scopus)

Abstract

Single-crystal Ni-rich Li[Ni_xMn_yCo_1-x-y]O₂(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_0.07O₂(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
Journal	ACS Nano
Volume	16
Issue number	9
Online published	13 Sept 2022
DOIs	https://doi.org/10.1021/acsnano.2c04959
Publication status	Published - 27 Sept 2022
Externally published	Yes

Funding

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.

Research Keywords

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

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@article{0d56b9432fcb4510adde52dd628792e3,

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

abstract = "Single-crystal Ni-rich Li[NixMnyCo1-x-y]O2 (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 LiNi0.83Mn0.1Co0.07O2 (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 = "conformal PEDOT coating, high-temperature, high-voltage, Ni-rich NMC, oCVD, single-crystal",

author = "Qiang Liu and Yu-Tong Liu and Chen Zhao and Qing-Song 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 Gui-Liang Xu and Khalil Amine and Guohua Chen",

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doi = "10.1021/acsnano.2c04959",

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

AU - Liu, Qiang

AU - Liu, Yu-Tong

AU - Zhao, Chen

AU - Weng, Qing-Song

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

PY - 2022/9/27

Y1 - 2022/9/27

N2 - Single-crystal Ni-rich Li[NixMnyCo1-x-y]O2 (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 LiNi0.83Mn0.1Co0.07O2 (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[NixMnyCo1-x-y]O2 (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 LiNi0.83Mn0.1Co0.07O2 (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 - conformal PEDOT coating

KW - high-temperature

KW - high-voltage

KW - Ni-rich NMC

KW - oCVD

KW - single-crystal

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U2 - 10.1021/acsnano.2c04959

DO - 10.1021/acsnano.2c04959

M3 - RGC 21 - Publication in refereed journal

C2 - 36098636

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

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GRF: Conformal Coating of Elastomeric Conducting Polymer with Ionic Conductivity on Ni-rich Layered Cathodes for Enhanced Redox Cycle Stability of Lithium-ion Batteries

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

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GRF: Conformal Coating of Elastomeric Conducting Polymer with Ionic Conductivity on Ni-rich Layered Cathodes for Enhanced Redox Cycle Stability of Lithium-ion Batteries

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