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

Title: Role of conductive binder to direct solid–electrolyte interphase formation over silicon anodes

Journal Article · · Physical Chemistry Chemical Physics. PCCP
DOI: https://doi.org/10.1039/c9cp02610j · OSTI ID:1617806

In this study, with the use of in situ neutron reflectometry (NR) we show how the addition of an electronically conductive polymeric binder, PEFM, mediates the solid–electrolyte interphase (SEI) formation and composition on an amorphous Si (a-Si) electrode as a function of the state-of-charge. Upon initial contact with the electrolyte a Li rich, 41 Å thick, layer forms on the surface of the anode below the polymer layer. At 0.8 V (vs. Li/Li+), a distinct SEI layer forms from the incorporation of electrolyte decomposition products in the reaction layer that is organic in nature. In addition, solvent uptake in the PEFM layer occurs resulting in the layer swelling to ~200 Å. Upon further polarization to 0.4 and 0.15 V (vs. Li/Li+) a thick layer (800 Å) on the surface of the Si is evident where a diffuse interface between the PEFM and SEI occurs resulting in a matrix between the two layers, as the binder has taken up a large amount of electrolyte. The two layers appear to be interchanging solvent molecules from the PEFM to the SEI to the Si surface preventing the lithiation of the a-Si. By 0.05 V (vs. Li/Li+) a Li rich, 72 Å thick, SEI layer condenses on the surface of the anode, and a 121 Å intermixed layer on top of the SEI with LiF and Li–C–O species is present with the rest blended into the electrolyte.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1617806
Alternate ID(s):
OSTI ID: 1545403
Journal Information:
Physical Chemistry Chemical Physics. PCCP, Vol. 21, Issue 31; ISSN 1463-9076
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 12 works
Citation information provided by
Web of Science

References (23)

Colossal Reversible Volume Changes in Lithium Alloys journal January 2001
Reversible Cycling of Crystalline Silicon Powder journal January 2007
Toward Efficient Binders for Li-Ion Battery Si-Based Anodes: Polyacrylic Acid journal October 2010
Enhanced Cycle Life of Si Anode for Li-Ion Batteries by Using Modified Elastomeric Binder journal January 2005
Sodium Carboxymethyl Cellulose journal January 2007
Lithium polyacrylate as a binder for tin–cobalt–carbon negative electrodes in lithium-ion batteries journal March 2010
Toward an Ideal Polymer Binder Design for High-Capacity Battery Anodes journal July 2013
Systematic Investigation of Binders for Silicon Anodes: Interactions of Binder with Silicon Particles and Electrolytes and Effects of Binders on Solid Electrolyte Interphase Formation journal May 2016
Direct measurement of the chemical reactivity of silicon electrodes with LiPF6-based battery electrolytes journal January 2014
Direct Determination of Solid-Electrolyte Interphase Thickness and Composition as a Function of State of Charge on a Silicon Anode journal August 2015
The Atomic Scale Electrochemical Lithiation and Delithiation Process of Silicon journal September 2017
Determination of the Solid Electrolyte Interphase Structure Grown on a Silicon Electrode Using a Fluoroethylene Carbonate Additive journal July 2017
Design and performance of horizontal-type neutron reflectometer SOFIA at J-PARC/MLF journal November 2011
Novel neutron reflectometer SOFIA at J-PARC/MLF for in-situ soft-interface characterization journal September 2012
Co-refinement of multiple-contrast neutron/X-ray reflectivity data using MOTOFIT journal March 2006
First Principles Model of Amorphous Silicon Lithiation journal January 2009
Evaluating the solid electrolyte interphase formed on silicon electrodes: a comparison of ex situ X-ray photoelectron spectroscopy and in situ neutron reflectometry journal January 2016
Manipulating the polarity of conductive polymer binders for Si-based anodes in lithium-ion batteries journal January 2015
The electrochemical behavior of poly 1-pyrenemethyl methacrylate binder and its effect on the interfacial chemistry of a silicon electrode journal February 2018
Advanced Model for Solid Electrolyte Interphase Electrodes in Liquid and Polymer Electrolytes journal January 1997
Comparison of PVDF and PVDF-TFE-P as Binders for Electrode Materials Showing Large Volume Changes in Lithium-Ion Batteries journal January 2003
Study on Polymer Binders for High-Capacity SiO Negative Electrode of Li-Ion Batteries journal June 2011
Sodium Carboxymethyl Cellulose journal January 1985

Figures / Tables (16)