DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Influence of Binder Coverage on Interfacial Chemistry of Thin Film LiNi0.6Mn 0.2Co0.2O2 Cathodes

Abstract

In this work, we explore the influence of binder coverage and chemistry on the interfacial properties of the textured Ni-rich cathode LiNi0.6Mn0.2Co0.2O2. We find that the formation of the cathode/electrolyte interphase (CEI) composition varies significantly for cathodes coated with either poly(vinylene fluoride) (PVDF), carboxymethyl cellulose (CMC), or lithium polyacrylate (LiPAA) after cycling to high upper cutoff voltages (4.5 V vs Li/Li). The PVDF-coated samples had a thinner CEI and twice the relative concentration of LiF and Li2CO3 to LixPOyFz species in the CEI compared to the uncoated sample. This correlated with significantly lower interfacial impedance (285 vs ~1700 Ohm-cm2) and improved capacity retention between cycles of the PVDF-coated samples compared to the other binder compositions and the uncoated sample. CMC-coated samples performed worst, with a CEI comprised of greater amounts of LixPOyFz. In addition, we find the choice of binder results in the selective protection or promotion of electrolyte reactions at the (104) surface of the 622 cathode. This suggests that the choice of binder can impact the surface chemistry and performance of high voltage cathodes and supports an avenue for interest in multifunctional binders for stabilizing the CEI.

Authors:
ORCiD logo; ; ORCiD logo
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1602334
Alternate Identifier(s):
OSTI ID: 1607055
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Published Article
Journal Name:
Journal of the Electrochemical Society (Online)
Additional Journal Information:
Journal Name: Journal of the Electrochemical Society (Online) Journal Volume: 167 Journal Issue: 4; Journal ID: ISSN 1945-7111
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Phillip, Nathan D., Daniel, Claus, and Veith, Gabriel M. Influence of Binder Coverage on Interfacial Chemistry of Thin Film LiNi0.6Mn 0.2Co0.2O2 Cathodes. United States: N. p., 2020. Web. doi:10.1149/1945-7111/ab78fc.
Phillip, Nathan D., Daniel, Claus, & Veith, Gabriel M. Influence of Binder Coverage on Interfacial Chemistry of Thin Film LiNi0.6Mn 0.2Co0.2O2 Cathodes. United States. https://doi.org/10.1149/1945-7111/ab78fc
Phillip, Nathan D., Daniel, Claus, and Veith, Gabriel M. Mon . "Influence of Binder Coverage on Interfacial Chemistry of Thin Film LiNi0.6Mn 0.2Co0.2O2 Cathodes". United States. https://doi.org/10.1149/1945-7111/ab78fc.
@article{osti_1602334,
title = {Influence of Binder Coverage on Interfacial Chemistry of Thin Film LiNi0.6Mn 0.2Co0.2O2 Cathodes},
author = {Phillip, Nathan D. and Daniel, Claus and Veith, Gabriel M.},
abstractNote = {In this work, we explore the influence of binder coverage and chemistry on the interfacial properties of the textured Ni-rich cathode LiNi0.6Mn0.2Co0.2O2. We find that the formation of the cathode/electrolyte interphase (CEI) composition varies significantly for cathodes coated with either poly(vinylene fluoride) (PVDF), carboxymethyl cellulose (CMC), or lithium polyacrylate (LiPAA) after cycling to high upper cutoff voltages (4.5 V vs Li/Li). The PVDF-coated samples had a thinner CEI and twice the relative concentration of LiF and Li2CO3 to LixPOyFz species in the CEI compared to the uncoated sample. This correlated with significantly lower interfacial impedance (285 vs ~1700 Ohm-cm2) and improved capacity retention between cycles of the PVDF-coated samples compared to the other binder compositions and the uncoated sample. CMC-coated samples performed worst, with a CEI comprised of greater amounts of LixPOyFz. In addition, we find the choice of binder results in the selective protection or promotion of electrolyte reactions at the (104) surface of the 622 cathode. This suggests that the choice of binder can impact the surface chemistry and performance of high voltage cathodes and supports an avenue for interest in multifunctional binders for stabilizing the CEI.},
doi = {10.1149/1945-7111/ab78fc},
journal = {Journal of the Electrochemical Society (Online)},
number = 4,
volume = 167,
place = {United States},
year = {Mon Mar 02 00:00:00 EST 2020},
month = {Mon Mar 02 00:00:00 EST 2020}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1149/1945-7111/ab78fc

Citation Metrics:
Cited by: 16 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Theoretical Investigations on Oxidative Stability of Solvents and Oxidative Decomposition Mechanism of Ethylene Carbonate for Lithium Ion Battery Use
journal, December 2009

  • Xing, Lidan; Li, Weishan; Wang, Chaoyang
  • The Journal of Physical Chemistry B, Vol. 113, Issue 52
  • DOI: 10.1021/jp9074064

Optimization of Acetylene Black Conductive Additive and PVDF Composition for High-Power Rechargeable Lithium-Ion Cells
journal, January 2007

  • Liu, G.; Zheng, H.; Simens, A. S.
  • Journal of The Electrochemical Society, Vol. 154, Issue 12
  • DOI: 10.1149/1.2792293

Nickel-Rich Layered Lithium Transition-Metal Oxide for High-Energy Lithium-Ion Batteries
journal, March 2015

  • Liu, Wen; Oh, Pilgun; Liu, Xien
  • Angewandte Chemie International Edition, Vol. 54, Issue 15
  • DOI: 10.1002/anie.201409262

Quantitative electron spectroscopy of surfaces: A standard data base for electron inelastic mean free paths in solids
journal, February 1979


Synthesis of Ni-Rich Thin-Film Cathode as Model System for Lithium Ion Batteries
journal, January 2019

  • Phillip, Nathan D.; Ruther, Rose E.; Sang, Xiahan
  • ACS Applied Energy Materials, Vol. 2, Issue 2
  • DOI: 10.1021/acsaem.8b01982

Charge Heterogeneity and Surface Chemistry in Polycrystalline Cathode Materials
journal, March 2018


Surface Modification for Suppressing Interfacial Parasitic Reactions of a Nickel-Rich Lithium-Ion Cathode
journal, March 2019


Processing of water-based LiNi1/3Mn1/3Co1/3O2 pastes for manufacturing lithium ion battery cathodes
journal, December 2014


Singlet oxygen evolution from layered transition metal oxide cathode materials and its implications for lithium-ion batteries
journal, October 2018


Ab Initio Modeling of Electrolyte Molecule Ethylene Carbonate Decomposition Reaction on Li(Ni,Mn,Co)O 2 Cathode Surface
journal, June 2017

  • Xu, Shenzhen; Luo, Guangfu; Jacobs, Ryan
  • ACS Applied Materials & Interfaces, Vol. 9, Issue 24
  • DOI: 10.1021/acsami.7b03435

Particles and Polymer Binder Interaction: A Controlling Factor in Lithium-Ion Electrode Performance
journal, January 2012

  • Liu, G.; Zheng, H.; Song, X.
  • Journal of The Electrochemical Society, Vol. 159, Issue 3
  • DOI: 10.1149/2.024203jes

The effect of different binders on electrochemical properties of LiNi1/3Mn1/3Co1/3O2 cathode material in lithium ion batteries
journal, March 2013


In Situ Determination of the Liquid/Solid Interface Thickness and Composition for the Li Ion Cathode LiMn 1.5 Ni 0.5 O 4
journal, October 2014

  • Browning, James F.; Baggetto, Loïc; Jungjohann, Katherine L.
  • ACS Applied Materials & Interfaces, Vol. 6, Issue 21
  • DOI: 10.1021/am5032055

Temperature Dependence of Oxygen Release from LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622) Cathode Materials for Li-Ion Batteries
journal, January 2018

  • Jung, Roland; Strobl, Philipp; Maglia, Filippo
  • Journal of The Electrochemical Society, Vol. 165, Issue 11
  • DOI: 10.1149/2.1261811jes

Lithium Polyacrylate (LiPAA) as an Advanced Binder and a Passivating Agent for High-Voltage Li-Ion Batteries
journal, September 2015

  • Pieczonka, Nicholas P. W.; Borgel, Valentina; Ziv, Baruch
  • Advanced Energy Materials, Vol. 5, Issue 23
  • DOI: 10.1002/aenm.201501008

Aging of LiNi1/3Mn1/3Co1/3O2 cathode material upon exposure to H2O
journal, June 2011


A carbonate-free, sulfone-based electrolyte for high-voltage Li-ion batteries
journal, May 2018


Ion chromatographic determination of hydrolysis products of hexafluorophosphate salts in aqueous solution
journal, February 2012


Singlet Oxygen Reactivity with Carbonate Solvents Used for Li-Ion Battery Electrolytes
journal, October 2018

  • Freiberg, Anna T. S.; Roos, Matthias K.; Wandt, Johannes
  • The Journal of Physical Chemistry A, Vol. 122, Issue 45
  • DOI: 10.1021/acs.jpca.8b08079

Probing Surface Chemistry Changes Using LiCoO 2 -only Electrodes in Li-Ion Batteries
journal, January 2018

  • Gauthier, Magali; Karayaylali, Pinar; Giordano, Livia
  • Journal of The Electrochemical Society, Vol. 165, Issue 7
  • DOI: 10.1149/2.0431807jes

Chemical versus Electrochemical Electrolyte Oxidation on NMC111, NMC622, NMC811, LNMO, and Conductive Carbon
journal, September 2017

  • Jung, Roland; Metzger, Michael; Maglia, Filippo
  • The Journal of Physical Chemistry Letters, Vol. 8, Issue 19
  • DOI: 10.1021/acs.jpclett.7b01927

Structural Degradation of High Voltage Lithium Nickel Manganese Cobalt Oxide (NMC) Cathodes in Solid-State Batteries and Implications for Next Generation Energy Storage
journal, January 2020

  • Phillip, Nathan D.; Westover, Andrew S.; Daniel, Claus
  • ACS Applied Energy Materials, Vol. 3, Issue 2
  • DOI: 10.1021/acsaem.9b02230

What makes lithium substituted polyacrylic acid a better binder than polyacrylic acid for silicon-graphite composite anodes?
journal, April 2018


Depth-Dependent Redox Behavior of LiNi 0.6 Mn 0.2 Co 0.2 O 2
journal, January 2018

  • Tian, Chixia; Nordlund, Dennis; Xin, Huolin L.
  • Journal of The Electrochemical Society, Vol. 165, Issue 3
  • DOI: 10.1149/2.1021803jes

Perspective—Fluorinating Interphases
journal, December 2018

  • Wang, Chunsheng; Meng, Ying Shirley; Xu, Kang
  • Journal of The Electrochemical Society, Vol. 166, Issue 3
  • DOI: 10.1149/2.0281903jes

Solid‐State Electrochemical Kinetics of Li‐Ion Intercalation into Li1 − xCoO2: Simultaneous Application of Electroanalytical Techniques SSCV, PITT, and EIS
journal, January 1999

  • Levi, M. D.; Salitra, G.; Markovsky, B.
  • Journal of The Electrochemical Society, Vol. 146, Issue 4, p. 1279-1289
  • DOI: 10.1149/1.1391759

Nickel, Manganese, and Cobalt Dissolution from Ni-Rich NMC and Their Effects on NMC622-Graphite Cells
journal, January 2019

  • Jung, Roland; Linsenmann, Fabian; Thomas, Rowena
  • Journal of The Electrochemical Society, Vol. 166, Issue 2
  • DOI: 10.1149/2.1151902jes

Oxygen Release and Its Effect on the Cycling Stability of LiNi x Mn y Co z O 2 (NMC) Cathode Materials for Li-Ion Batteries
journal, January 2017

  • Jung, Roland; Metzger, Michael; Maglia, Filippo
  • Journal of The Electrochemical Society, Vol. 164, Issue 7
  • DOI: 10.1149/2.0021707jes

Thermal Decomposition of LiPF[sub 6]-Based Electrolytes for Lithium-Ion Batteries
journal, January 2005

  • Campion, Christopher L.; Li, Wentao; Lucht, Brett L.
  • Journal of The Electrochemical Society, Vol. 152, Issue 12
  • DOI: 10.1149/1.2083267

Decomposition of LiPF 6 in High Energy Lithium-Ion Batteries Studied with Online Electrochemical Mass Spectrometry
journal, January 2016

  • Guéguen, Aurélie; Streich, Daniel; He, Minglong
  • Journal of The Electrochemical Society, Vol. 163, Issue 6
  • DOI: 10.1149/2.0981606jes

NiO as a peculiar support for metal nanoparticles in polyols oxidation
journal, January 2013

  • Villa, Alberto; Veith, Gabriel M.; Ferri, Davide
  • Catal. Sci. Technol., Vol. 3, Issue 2
  • DOI: 10.1039/C2CY20370G