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 publicationJournal articleAcademic researchpeer-review

17 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 languageEnglish
Pages (from-to)14527-14538
Number of pages12
JournalACS Nano
Volume16
Issue number9
DOIs
Publication statusPublished - 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

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