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Title: Intrinsic chemical reactivity of solid-electrolyte interphase components in silicon–lithium alloy anode batteries probed by FTIR spectroscopy

Abstract

The chemical reactivity of silicon surface species with LiPF6/carbonate electrolyte are detailed via FTIR spectroscopy and verified by MD/DFPD simulations.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [4];  [5]; ORCiD logo [6]; ORCiD logo [6]; ORCiD logo [4]; ORCiD logo [7]; ORCiD logo [8]; ORCiD logo [5]; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Tennessee, Knoxville, TN (United States)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States); Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  5. Univ. of California, Berkeley, CA (United States)
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  7. Argonne National Lab. (ANL), Lemont, IL (United States)
  8. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS); National Renewable Energy Lab. (NREL), Golden, CO (United States); Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Argonne National Lab. (ANL), Argonne, IL (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Science (SC); USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office
OSTI Identifier:
1617794
Alternate Identifier(s):
OSTI ID: 1616360; OSTI ID: 1659889; OSTI ID: 1756168; OSTI ID: 1766489
Report Number(s):
NREL/JA-5900-75298
Journal ID: ISSN 2050-7488; JMCAET
Grant/Contract Number:  
AC05-00OR22725; AC36-08GO28308; NA0003525; AC02-06CH11357; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 8; Journal Issue: 16; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; silicon; Li-ion; electrochemical

Citation Formats

Pekarek, Ryan T., Affolter, Alec, Baranowski, Lauryn L., Coyle, Jaclyn, Hou, Tingzheng, Sivonxay, Eric, Smith, Brenda A., McAuliffe, Rebecca D., Persson, Kristin A., Key, Baris, Apblett, Christopher, Veith, Gabriel M., and Neale, Nathan R. Intrinsic chemical reactivity of solid-electrolyte interphase components in silicon–lithium alloy anode batteries probed by FTIR spectroscopy. United States: N. p., 2020. Web. doi:10.1039/C9TA13535A.
Pekarek, Ryan T., Affolter, Alec, Baranowski, Lauryn L., Coyle, Jaclyn, Hou, Tingzheng, Sivonxay, Eric, Smith, Brenda A., McAuliffe, Rebecca D., Persson, Kristin A., Key, Baris, Apblett, Christopher, Veith, Gabriel M., & Neale, Nathan R. Intrinsic chemical reactivity of solid-electrolyte interphase components in silicon–lithium alloy anode batteries probed by FTIR spectroscopy. United States. doi:https://doi.org/10.1039/C9TA13535A
Pekarek, Ryan T., Affolter, Alec, Baranowski, Lauryn L., Coyle, Jaclyn, Hou, Tingzheng, Sivonxay, Eric, Smith, Brenda A., McAuliffe, Rebecca D., Persson, Kristin A., Key, Baris, Apblett, Christopher, Veith, Gabriel M., and Neale, Nathan R. Tue . "Intrinsic chemical reactivity of solid-electrolyte interphase components in silicon–lithium alloy anode batteries probed by FTIR spectroscopy". United States. doi:https://doi.org/10.1039/C9TA13535A. https://www.osti.gov/servlets/purl/1617794.
@article{osti_1617794,
title = {Intrinsic chemical reactivity of solid-electrolyte interphase components in silicon–lithium alloy anode batteries probed by FTIR spectroscopy},
author = {Pekarek, Ryan T. and Affolter, Alec and Baranowski, Lauryn L. and Coyle, Jaclyn and Hou, Tingzheng and Sivonxay, Eric and Smith, Brenda A. and McAuliffe, Rebecca D. and Persson, Kristin A. and Key, Baris and Apblett, Christopher and Veith, Gabriel M. and Neale, Nathan R.},
abstractNote = {The chemical reactivity of silicon surface species with LiPF6/carbonate electrolyte are detailed via FTIR spectroscopy and verified by MD/DFPD simulations.},
doi = {10.1039/C9TA13535A},
journal = {Journal of Materials Chemistry. A},
number = 16,
volume = 8,
place = {United States},
year = {2020},
month = {3}
}

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Works referenced in this record:

Chemistry of Electrolyte Reduction on Lithium Silicide
journal, May 2019

  • Xu, Yun; Wood, Kevin; Coyle, Jaclyn
  • The Journal of Physical Chemistry C, Vol. 123, Issue 21
  • DOI: 10.1021/acs.jpcc.9b02611

Nonthermal Plasma Synthesis of Nanocrystals: Fundamental Principles, Materials, and Applications
journal, August 2016


Three-dimensional electronic resistivity mapping of solid electrolyte interphase on Si anode materials
journal, January 2019


The infra-red spectra and structure of ethylene carbonate
journal, January 1956


Mechanism of Interactions between CMC Binder and Si Single Crystal Facets
journal, August 2014

  • Vogl, U. S.; Das, P. K.; Weber, A. Z.
  • Langmuir, Vol. 30, Issue 34
  • DOI: 10.1021/la501791q

Decomposition Reactions of Anode Solid Electrolyte Interphase (SEI) Components with LiPF 6
journal, October 2017

  • Parimalam, Bharathy S.; MacIntosh, Alex D.; Kadam, Rahul
  • The Journal of Physical Chemistry C, Vol. 121, Issue 41
  • DOI: 10.1021/acs.jpcc.7b08433

In Situ Potentiodynamic Analysis of the Electrolyte/Silicon Electrodes Interface Reactions - A Sum Frequency Generation Vibrational Spectroscopy Study
journal, January 2016

  • Horowitz, Yonatan; Han, Hui-Ling; Ross, Philip N.
  • Journal of the American Chemical Society, Vol. 138, Issue 3
  • DOI: 10.1021/jacs.5b10333

Shear Thickening Electrolytes for High Impact Resistant Batteries
journal, August 2017


Role of Mixed Solvation and Ion Pairing in the Solution Structure of Lithium Ion Battery Electrolytes
journal, June 2015

  • Seo, Daniel M.; Reininger, Stefanie; Kutcher, Mary
  • The Journal of Physical Chemistry C, Vol. 119, Issue 25
  • DOI: 10.1021/acs.jpcc.5b03694

In situ FTIR study of the Cu electrode/ethylene carbonate+dimethyl carbonate solution interface
journal, April 2008


Plasmonic Properties of Silicon Nanocrystals Doped with Boron and Phosphorus
journal, July 2015


Hypervalent surface interactions for colloidal stability and doping of silicon nanocrystals
journal, July 2013

  • Wheeler, Lance M.; Neale, Nathan R.; Chen, Ting
  • Nature Communications, Vol. 4, Article No. 2197
  • DOI: 10.1038/ncomms3197

Si-Based Anode Materials for Li-Ion Batteries: A Mini Review
journal, September 2014


Probing Electrolyte Solvents at Solid/Liquid Interface Using Gap-Mode Surface-Enhanced Raman Spectroscopy
journal, January 2019

  • Yang, Guang; Sacci, Robert L.; Ivanov, Ilia N.
  • Journal of The Electrochemical Society, Vol. 166, Issue 2
  • DOI: 10.1149/2.0391902jes

Unraveling the Nanoscale Heterogeneity of Solid Electrolyte Interphase Using Tip-Enhanced Raman Spectroscopy
journal, August 2019


Direct measurement of the chemical reactivity of silicon electrodes with LiPF6-based battery electrolytes
journal, January 2014

  • Veith, Gabriel M.; Baggetto, Loïc; Sacci, Robert L.
  • Chemical Communications, Vol. 50, Issue 23
  • DOI: 10.1039/c3cc49269a

In-Situ Spectro-electrochemical Insight Revealing Distinctive Silicon Anode Solid Electrolyte Interphase Formation in a Lithium-ion Battery
journal, March 2016

  • Yang , Junfeng; Solomatin, Nickolay; Kraytsberg, Alexander
  • ChemistrySelect, Vol. 1, Issue 3
  • DOI: 10.1002/slct.201600119

Tuning Confinement in Colloidal Silicon Nanocrystals with Saturated Surface Ligands
journal, April 2018


Competitive lithium solvation of linear and cyclic carbonates from quantum chemistry
journal, January 2016

  • Borodin, Oleg; Olguin, Marco; Ganesh, P.
  • Physical Chemistry Chemical Physics, Vol. 18, Issue 1
  • DOI: 10.1039/C5CP05121E

Alloy Negative Electrodes for Li-Ion Batteries
journal, October 2014

  • Obrovac, M. N.; Chevrier, V. L.
  • Chemical Reviews, Vol. 114, Issue 23
  • DOI: 10.1021/cr500207g

Temperature-Dependent Solubility of Solid Electrolyte Interphase on Silicon Electrodes
journal, October 2019


Characterization of Silicon Nanocrystal Surfaces by Multidimensional Solid-State NMR Spectroscopy
journal, November 2017


Free-Energy and Structural Analysis of Ion Solvation and Contact Ion-Pair Formation of Li + with BF 4 and PF 6 in Water and Carbonate Solvents
journal, May 2012

  • Takeuchi, Munetaka; Matubayasi, Nobuyuki; Kameda, Yasuo
  • The Journal of Physical Chemistry B, Vol. 116, Issue 22
  • DOI: 10.1021/jp3011487

Tailoring the Surface of Silicon Nanoparticles for Enhanced Chemical and Electrochemical Stability for Li-Ion Batteries
journal, August 2019

  • Jiang, Sisi; Hu, Bin; Sahore, Ritu
  • ACS Applied Energy Materials, Vol. 2, Issue 9
  • DOI: 10.1021/acsaem.9b01601

Structural and compositional characterization of RF magnetron cosputtered lithium silicate films: From Li 2 Si 2 O 5 to lithium-rich Li 8 SiO 6
journal, November 2017

  • Coyle, Jaclyn; Apblett, Christopher; Brumbach, Michael
  • Journal of Vacuum Science & Technology A, Vol. 35, Issue 6
  • DOI: 10.1116/1.4998726

Role of Solution Structure in Solid Electrolyte Interphase Formation on Graphite with LiPF 6 in Propylene Carbonate
journal, November 2013

  • Nie, Mengyun; Abraham, Daniel P.; Seo, Daniel M.
  • The Journal of Physical Chemistry C, Vol. 117, Issue 48
  • DOI: 10.1021/jp409765w

XPS on Li-Battery-Related Compounds: Analysis of Inorganic SEI Phases and a Methodology for Charge Correction
journal, August 2018


Raman and Infrared Spectral Studies of Anhydrous Li 2 CO 3 and Na 2 CO 3
journal, June 1971

  • Brooker, M. H.; Bates, John B.
  • The Journal of Chemical Physics, Vol. 54, Issue 11
  • DOI: 10.1063/1.1674754

The Formation Mechanism of Fluorescent Metal Complexes at the Li x Ni 0.5 Mn 1.5 O 4−δ /Carbonate Ester Electrolyte Interface
journal, March 2015

  • Jarry, Angélique; Gottis, Sébastien; Yu, Young-Sang
  • Journal of the American Chemical Society, Vol. 137, Issue 10
  • DOI: 10.1021/ja5116698

Determination of the Solid Electrolyte Interphase Structure Grown on a Silicon Electrode Using a Fluoroethylene Carbonate Additive
journal, July 2017


Mechanical Properties and Chemical Reactivity of Li x SiO y Thin Films
journal, October 2018

  • Xu, Yun; Stetson, Caleb; Wood, Kevin
  • ACS Applied Materials & Interfaces, Vol. 10, Issue 44
  • DOI: 10.1021/acsami.8b10895

The Role of Silanols in the Interactions between Methyl tert -Butyl Ether and High-Silica Faujasite Y: An Infrared Spectroscopy and Computational Model Study
journal, March 2012

  • Braschi, Ilaria; Gatti, Giorgio; Bisio, Chiara
  • The Journal of Physical Chemistry C, Vol. 116, Issue 12
  • DOI: 10.1021/jp210605t

Probing the Surface Structure of Semiconductor Nanoparticles by DNP SENS with Dielectric Support Materials
journal, August 2019

  • Hanrahan, Michael P.; Chen, Yunhua; Blome-Fernández, Rafael
  • Journal of the American Chemical Society, Vol. 141, Issue 39
  • DOI: 10.1021/jacs.9b05509

Infrared and Raman spectra of the silicon-hydrogen bonds in amorphous silicon prepared by glow discharge and sputtering
journal, October 1977


Co-ordinating tendencies of the hexafluorophosphate ion
journal, January 1971

  • Mayfield, H. Gordon; Bull, William E.
  • Journal of the Chemical Society A: Inorganic, Physical, Theoretical
  • DOI: 10.1039/j19710002279

Si Oxidation and H 2 Gassing During Aqueous Slurry Preparation for Li-Ion Battery Anodes
journal, April 2018

  • Hays, Kevin A.; Key, Baris; Li, Jianlin
  • The Journal of Physical Chemistry C, Vol. 122, Issue 18
  • DOI: 10.1021/acs.jpcc.8b01062

The Vibrational Spectra and Structure of Dimethyl Carbonate and its Conformational Behavior
journal, May 1975

  • Katon, J. E.; Cohen, M. D.
  • Canadian Journal of Chemistry, Vol. 53, Issue 9
  • DOI: 10.1139/v75-191

Silyl Radical Abstraction in the Functionalization of Plasma-Synthesized Silicon Nanocrystals
journal, September 2015

  • Wheeler, Lance M.; Anderson, Nicholas C.; Palomaki, Peter K. B.
  • Chemistry of Materials, Vol. 27, Issue 19, p. 6869-6878
  • DOI: 10.1021/acs.chemmater.5b03309