Structure of spontaneously formed solid-electrolyte interphase on lithiated graphite determined using small-angle neutron scattering

Sacci, Robert L.; Banuelos, Jose Leobardo; Veith, Gabriel M.; Littrell, Ken C.; Cheng, Yongqiang Q.; Wildgruber, Christoph U.; Jones, Lacy L.; Ramirez-Cuesta, Anibal J.; Rother, Gernot; Dudney, Nancy J.

doi:10.1021/acs.jpcc.5b00215

Title: Structure of spontaneously formed solid-electrolyte interphase on lithiated graphite determined using small-angle neutron scattering

Journal Article · Wed Mar 25 00:00:00 EDT 2015 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.5b00215· OSTI ID:1185815

Sacci, Robert L. ^[1]; Banuelos, Jose Leobardo ^[1]; Veith, Gabriel M. ^[1]; Littrell, Ken C. ^[1]; Cheng, Yongqiang Q. ^[1]; Wildgruber, Christoph U. ^[1]; Jones, Lacy L. ^[1]; Ramirez-Cuesta, Anibal J. ^[1]; Rother, Gernot ^[1]; Dudney, Nancy J. ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

We report the first small-angle neutron scattering of a chemically formed solid-electrolyte interphase from LixC6 reacting with ethylene carbonate/dimethyl carbon solvent. This provides a different and perhaps simpler view of SEI formation than the usual electrochemically-driven reaction. We show that an organic layer coats the graphite particles filling in micro-pores and is polymeric in nature being 1-3 nm thick. We used inelastic neutron scattering to probe the chemistry, and we found that the SEI showed similar inelastic scattering to polyethylene oxide.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1185815

Journal Information:: Journal of Physical Chemistry. C, Vol. 119, Issue 18; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 24 works

Citation information provided by
Web of Science

References (25)

Building better batteries Armand, M.; Tarascon, J.-M. Nature, Vol. 451, Issue 7179, p. 652-657 https://doi.org/10.1038/451652a	journal	February 2008
Electrode–solution interactions in Li-ion batteries: a short summary and new insights Aurbach, D. Journal of Power Sources, Vol. 119-121 https://doi.org/10.1016/S0378-7753(03)00273-8	journal	June 2003
The Correlation Between the Surface Chemistry and the Performance of Li-Carbon Intercalation Anodes for Rechargeable ‘Rocking-Chair’ Type Batteries Aurbach, Doron Journal of The Electrochemical Society, Vol. 141, Issue 3 https://doi.org/10.1149/1.2054777	journal	January 1994
A short review of failure mechanisms of lithium metal and lithiated graphite anodes in liquid electrolyte solutions Aurbach, D. Solid State Ionics, Vol. 148, Issue 3-4 https://doi.org/10.1016/S0167-2738(02)00080-2	journal	June 2002
A Study of Electrochemical Reduction of Ethylene and Propylene Carbonate Electrolytes on Graphite Using ATR-FTIR Spectroscopy Zhuang, Guorong V.; Yang, Hui; Blizanac, Berislav Electrochemical and Solid-State Letters, Vol. 8, Issue 9 https://doi.org/10.1149/1.1979327	journal	January 2005
Investigation of the Electrochemical Windows of Aprotic Alkali Metal (Li, Na, K) Salt Solutions Moshkovich, M.; Gofer, Y.; Aurbach, D. Journal of The Electrochemical Society, Vol. 148, Issue 4 https://doi.org/10.1149/1.1357316	journal	January 2001
Direct visualization of initial SEI morphology and growth kinetics during lithium deposition by in situ electrochemical transmission electron microscopy Sacci, Robert L.; Dudney, Nancy J.; More, Karren L. Chemical Communications, Vol. 50, Issue 17 https://doi.org/10.1039/c3cc49029g	journal	January 2014
Nanoscale Imaging of Fundamental Li Battery Chemistry: Solid-Electrolyte Interphase Formation and Preferential Growth of Lithium Metal Nanoclusters Sacci, Robert L.; Black, Jennifer M.; Balke, Nina Nano Letters, Vol. 15, Issue 3 https://doi.org/10.1021/nl5048626	journal	February 2015
Structure Analysis by Small-Angle X-Ray and Neutron Scattering Feigin, L. A.; Svergun, D. I. https://doi.org/10.1007/978-1-4757-6624-0	book	January 1987
Vibrational Spectroscopy with Neutrons Mitchell, Philip C. H.; Parker, Stewart F.; Ramirez-Cuesta, Anibal J. https://doi.org/10.1142/5628	book	June 2005
Characterization of the neutron detector upgrade to the GP-SANS and Bio-SANS instruments at HFIR Berry, Kevin D.; Bailey, Katherine M.; Beal, Justin Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 693 https://doi.org/10.1016/j.nima.2012.06.052	journal	November 2012
The 40 m general purpose small-angle neutron scattering instrument at Oak Ridge National Laboratory Wignall, George D.; Littrell, Kenneth C.; Heller, William T. Journal of Applied Crystallography, Vol. 45, Issue 5 https://doi.org/10.1107/S0021889812027057	journal	August 2012
Resolution of VISION, a crystal-analyzer spectrometer Seeger, Philip A.; Daemen, Luke L.; Larese, John Z. Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 604, Issue 3 https://doi.org/10.1016/j.nima.2009.03.204	journal	June 2009
A comparison of electrochemical performance of natural graphite sulfurized by ball-milling and heat-treating as an anode for lithium ion batteries Lu, Mi; Tian, Yanyan; Yang, Yong Electrochimica Acta, Vol. 54, Issue 27 https://doi.org/10.1016/j.electacta.2009.06.079	journal	November 2009
Dry Synthesis of Lithium Intercalated Graphite Powder and Fiber Sacci, Robert L.; Adamczyk, Leslie A.; Veith, Gabriel M. Journal of The Electrochemical Society, Vol. 161, Issue 4 https://doi.org/10.1149/2.082404jes	journal	January 2014
Small-Angle X-Ray-Scattering Investigation of Submicroscopic Porosity with Fractal Properties Bale, Harold D.; Schmidt, Paul W. Physical Review Letters, Vol. 53, Issue 6 https://doi.org/10.1103/PhysRevLett.53.596	journal	August 1984
Small-angle scattering by fractal systems Teixeira, J. Journal of Applied Crystallography, Vol. 21, Issue 6, p. 781-785 https://doi.org/10.1107/S0021889888000263	journal	December 1988
Inelastic neutron scattering, Raman and DFT investigations of the adsorption of phenanthrenequinone on onion-like carbon Anjos, Daniela M.; Kolesnikov, Alexander I.; Wu, Zili Carbon, Vol. 52 https://doi.org/10.1016/j.carbon.2012.09.016	journal	February 2013
Infrared and Raman spectra and vibrational assignment of ethylene carbonate Fortunato, Bruno; Mirone, Paolo; Fini, Glancaelo Spectrochimica Acta Part A: Molecular Spectroscopy, Vol. 27, Issue 9 https://doi.org/10.1016/0584-8539(71)80245-3	journal	September 1971
Structure, vibrational-dynamics and first-principles study of diglyme as a model system for poly(ethyleneoxide) Kearley, G. Solid State Ionics, Vol. 147, Issue 3-4 https://doi.org/10.1016/S0167-2738(02)00022-X	journal	April 2002
Lithium Ethylene Dicarbonate Identified as the Primary Product of Chemical and Electrochemical Reduction of EC in 1.2 M LiPF ₆ /EC:EMC Electrolyte Zhuang, Guorong V.; Xu, Kang; Yang, Hui The Journal of Physical Chemistry B, Vol. 109, Issue 37 https://doi.org/10.1021/jp052474w	journal	September 2005
Electrochemical and Infrared Studies of the Reduction of Organic Carbonates Zhang, Xuerong; Kostecki, Robert; Richardson, Thomas J. Journal of The Electrochemical Society, Vol. 148, Issue 12 https://doi.org/10.1149/1.1415547	journal	January 2001
PRINSAS – a Windows-based computer program for the processing and interpretation of small-angle scattering data tailored to the analysis of sedimentary rocks Hinde, Alan L. Journal of Applied Crystallography, Vol. 37, Issue 6 https://doi.org/10.1107/S0021889804021260	journal	November 2004
Direct Visualization of Solid Electrolyte Interphase Formation in Lithium-Ion Batteries with In Situ Electrochemical Transmission Electron Microscopy Unocic, Raymond R.; Sun, Xiao-Guang; Sacci, Robert L. Microscopy and Microanalysis, Vol. 20, Issue 4 https://doi.org/10.1017/S1431927614012744	journal	July 2014
Visualization of Electrode–Electrolyte Interfaces in LiPF ₆ /EC/DEC Electrolyte for Lithium Ion Batteries via in Situ TEM Zeng, Zhiyuan; Liang, Wen-I; Liao, Hong-Gang Nano Letters, Vol. 14, Issue 4 https://doi.org/10.1021/nl403922u	journal	March 2014

Cited By (2)

Li-ion half-cells studied operando during cycling by small-angle neutron scattering Hattendorff, Johannes; Seidlmayer, Stefan; Gasteiger, Hubert A. Journal of Applied Crystallography, Vol. 53, Issue 1 https://doi.org/10.1107/s160057671901714x	journal	February 2020
Contrast Matched SANS for Observing SEI and Pore Clogging in Silicon-Graphite Anodes Paul, Neelima; Wetjen, Morten; Busch, Sebastian Journal of The Electrochemical Society, Vol. 166, Issue 6 https://doi.org/10.1149/2.0781906jes	journal	January 2019

Similar Records

In-Situ Observation of Solid Electrolyte Interphase Formation in Ordered Mesoporous Hard Carbon by Small-Angle Neutron Scattering

Journal Article · Sun Jan 01 00:00:00 EST 2012 · Journal of Physical Chemistry C · OSTI ID:1185815

Bridges, Craig A; Paranthaman, Mariappan Parans; Sun, Xiao-Guang; +2 more

Examining CO₂ as an Additive for Solid Electrolyte Interphase Formation on Silicon Anodes

Journal Article · Thu Mar 18 00:00:00 EDT 2021 · Journal of the Electrochemical Society · OSTI ID:1185815

Hopkins, Emma; Frisco, Sarah; Pekarek, Ryan; +11 more

Effect of Fluoroethylene Carbonate Additives on the Initial Formation of the Solid Electrolyte Interphase on an Oxygen-Functionalized Graphitic Anode in Lithium-Ion Batteries

Journal Article · Mon Feb 15 00:00:00 EST 2021 · ACS Applied Materials and Interfaces · OSTI ID:1185815

Intan, Nadia N.; Pfaendtner, Jim

Related Subjects

36 MATERIALS SCIENCE
solid-electrolyte interphase
small-angle neutron scattering
inelastic neutron scattering
lithiated graphite
anodes

Title: Structure of spontaneously formed solid-electrolyte interphase on lithiated graphite determined using small-angle neutron scattering

Citation Formats

References (25)

Cited By (2)

Similar Records

Related Subjects