Skip to main content

Lund University Publications

LUND UNIVERSITY LIBRARIES

Study of degradation mechanisms in aqueous-processed Ni-rich cathodes for enhanced sustainability of batteries

Chen, Heyin ; Mattsson, Agnes Matilda ; King, Laura ; Liu, Haidong ; Nielsen, Ida ; Ericson, Tove ; Preobrajenski, Alexei LU ; Brant, William R. and Hahlin, Maria (2024) In Journal of Materials Chemistry A 12(37). p.25393-25406
Abstract

Traditionally, Ni-rich-layered oxide cathodes for lithium-ion batteries are produced utilizing N-methyl-2-pyrrolidone (NMP)-processed casting. However, to avoid using the reprotoxic solvent NMP, aqueous processing becomes one of the options. In this study, H2O-processed LiNi0.8Mn0.1Co0.1O2 (NMC811) electrodes have been prepared to compare with the NMP-processed counterparts to investigate the degradation mechanism. The thick cathode-electrolyte interphase (CEI), NiO-like phase formation, and the growth of electrochemically inactive NMC particles after long-term cycling lead to capacity decay. In addition, phosphoric acid (H3PO4) was utilized to lower the pH... (More)

Traditionally, Ni-rich-layered oxide cathodes for lithium-ion batteries are produced utilizing N-methyl-2-pyrrolidone (NMP)-processed casting. However, to avoid using the reprotoxic solvent NMP, aqueous processing becomes one of the options. In this study, H2O-processed LiNi0.8Mn0.1Co0.1O2 (NMC811) electrodes have been prepared to compare with the NMP-processed counterparts to investigate the degradation mechanism. The thick cathode-electrolyte interphase (CEI), NiO-like phase formation, and the growth of electrochemically inactive NMC particles after long-term cycling lead to capacity decay. In addition, phosphoric acid (H3PO4) was utilized to lower the pH value during the water-processed electrode preparation, to avoid corrosion of the aluminium current collector. The use of H3PO4 enhanced the capacity retention of NMC811 electrodes, likely owing to the formation of a LiF-rich CEI layer in the initial cycle(s) and the alleviated formation of electrochemically inactive NMC particles. Additionally, reaction inhomogeneity is present in H3PO4-modified electrodes, which is attributed to various Li-ion reinsertion resistances throughout the porous electrode during long-term cycling. Although the performance of the water-processed NMC811 electrode is not reaching the level of NMP-processed electrodes, this study provides key insights into the involved degradation mechanisms and demonstrates a viable pathway for the development of sustainable battery manufacturing processes.

(Less)
Please use this url to cite or link to this publication:
author
; ; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Journal of Materials Chemistry A
volume
12
issue
37
pages
14 pages
publisher
Royal Society of Chemistry
external identifiers
  • scopus:85203199968
ISSN
2050-7488
DOI
10.1039/d4ta03592e
language
English
LU publication?
yes
id
cbd7490d-7606-40d8-ac85-76894dc01a94
date added to LUP
2024-12-13 12:38:33
date last changed
2025-04-04 15:13:33
@article{cbd7490d-7606-40d8-ac85-76894dc01a94,
  abstract     = {{<p>Traditionally, Ni-rich-layered oxide cathodes for lithium-ion batteries are produced utilizing N-methyl-2-pyrrolidone (NMP)-processed casting. However, to avoid using the reprotoxic solvent NMP, aqueous processing becomes one of the options. In this study, H<sub>2</sub>O-processed LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> (NMC811) electrodes have been prepared to compare with the NMP-processed counterparts to investigate the degradation mechanism. The thick cathode-electrolyte interphase (CEI), NiO-like phase formation, and the growth of electrochemically inactive NMC particles after long-term cycling lead to capacity decay. In addition, phosphoric acid (H<sub>3</sub>PO<sub>4</sub>) was utilized to lower the pH value during the water-processed electrode preparation, to avoid corrosion of the aluminium current collector. The use of H<sub>3</sub>PO<sub>4</sub> enhanced the capacity retention of NMC811 electrodes, likely owing to the formation of a LiF-rich CEI layer in the initial cycle(s) and the alleviated formation of electrochemically inactive NMC particles. Additionally, reaction inhomogeneity is present in H<sub>3</sub>PO<sub>4</sub>-modified electrodes, which is attributed to various Li-ion reinsertion resistances throughout the porous electrode during long-term cycling. Although the performance of the water-processed NMC811 electrode is not reaching the level of NMP-processed electrodes, this study provides key insights into the involved degradation mechanisms and demonstrates a viable pathway for the development of sustainable battery manufacturing processes.</p>}},
  author       = {{Chen, Heyin and Mattsson, Agnes Matilda and King, Laura and Liu, Haidong and Nielsen, Ida and Ericson, Tove and Preobrajenski, Alexei and Brant, William R. and Hahlin, Maria}},
  issn         = {{2050-7488}},
  language     = {{eng}},
  number       = {{37}},
  pages        = {{25393--25406}},
  publisher    = {{Royal Society of Chemistry}},
  series       = {{Journal of Materials Chemistry A}},
  title        = {{Study of degradation mechanisms in aqueous-processed Ni-rich cathodes for enhanced sustainability of batteries}},
  url          = {{http://dx.doi.org/10.1039/d4ta03592e}},
  doi          = {{10.1039/d4ta03592e}},
  volume       = {{12}},
  year         = {{2024}},
}