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Title: The Study of the Binder Poly(acrylic acid) and Its Role in Concomitant Solid–Electrolyte Interphase Formation on Si Anodes

Abstract

In this work we use neutron reflectometry to study how the polymeric binder, poly(acrylic acid) (PAA), affects the in situ formation and chemical composition of the solid–electrolyte interphase (SEI) formation on a silicon anode at various states of charge. The reflectivity is correlated with electrochemical quartz crystal microbalance to better understand the viscoelastic effects of the polymer during cycling. The use of model thin films allows for a well-controlled interface between the amorphous Si surface and the PAA layer. If the PAA perfectly coats the Si surface and standard processing conditions are used, the binder will prevent the lithiation of the anode. The PAA suppresses the growth of a new layer formed at early states of discharge (open circuit voltage to 0.8 V vs Li/Li+), protecting the surface of the anode. At 0.15 V, the SEI layer underneath the PAA changes in chemical composition as indicated by an increase in the scattering length density and thickness as the layer incorporates components from the electrolyte, most likely the salt. At lithiated and delithiated states, the SEI layer changes in chemical composition and grows in thickness with delithiation and shrinks during lithiation.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]
  1. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1606640
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 12; Journal Issue: 8; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; poly(acrylic acid) binder; Si anodes; solid-electrolyte interphase; neutron reflectometry; quartz crystal microbalance

Citation Formats

Browning, Katie L., Sacci, Robert L., Doucet, Mathieu, Browning, James F., Kim, Joshua R., and Veith, Gabriel M. The Study of the Binder Poly(acrylic acid) and Its Role in Concomitant Solid–Electrolyte Interphase Formation on Si Anodes. United States: N. p., 2020. Web. https://doi.org/10.1021/acsami.9b22382.
Browning, Katie L., Sacci, Robert L., Doucet, Mathieu, Browning, James F., Kim, Joshua R., & Veith, Gabriel M. The Study of the Binder Poly(acrylic acid) and Its Role in Concomitant Solid–Electrolyte Interphase Formation on Si Anodes. United States. https://doi.org/10.1021/acsami.9b22382
Browning, Katie L., Sacci, Robert L., Doucet, Mathieu, Browning, James F., Kim, Joshua R., and Veith, Gabriel M. Sat . "The Study of the Binder Poly(acrylic acid) and Its Role in Concomitant Solid–Electrolyte Interphase Formation on Si Anodes". United States. https://doi.org/10.1021/acsami.9b22382. https://www.osti.gov/servlets/purl/1606640.
@article{osti_1606640,
title = {The Study of the Binder Poly(acrylic acid) and Its Role in Concomitant Solid–Electrolyte Interphase Formation on Si Anodes},
author = {Browning, Katie L. and Sacci, Robert L. and Doucet, Mathieu and Browning, James F. and Kim, Joshua R. and Veith, Gabriel M.},
abstractNote = {In this work we use neutron reflectometry to study how the polymeric binder, poly(acrylic acid) (PAA), affects the in situ formation and chemical composition of the solid–electrolyte interphase (SEI) formation on a silicon anode at various states of charge. The reflectivity is correlated with electrochemical quartz crystal microbalance to better understand the viscoelastic effects of the polymer during cycling. The use of model thin films allows for a well-controlled interface between the amorphous Si surface and the PAA layer. If the PAA perfectly coats the Si surface and standard processing conditions are used, the binder will prevent the lithiation of the anode. The PAA suppresses the growth of a new layer formed at early states of discharge (open circuit voltage to 0.8 V vs Li/Li+), protecting the surface of the anode. At 0.15 V, the SEI layer underneath the PAA changes in chemical composition as indicated by an increase in the scattering length density and thickness as the layer incorporates components from the electrolyte, most likely the salt. At lithiated and delithiated states, the SEI layer changes in chemical composition and grows in thickness with delithiation and shrinks during lithiation.},
doi = {10.1021/acsami.9b22382},
journal = {ACS Applied Materials and Interfaces},
number = 8,
volume = 12,
place = {United States},
year = {2020},
month = {1}
}

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