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Direct determination of solid-electrolyte interphase thickness and composition as a function of state of charge on a silicon anode

Journal Article · · Journal of Physical Chemistry. C
 [1];  [1];  [2];  [1];  [1];  [2];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Using neutron reflectometry we have determined the thickness and chemistry of the solid-electrolyte interphase (SEI) layer grown on a silicon anode as a function of state of charge and during cycling. We show the chemistry of this SEI layer becomes more LiF like with increasing lithiation and more Li-C-O-F like with delithiation. More importantly the SEI layer thickness appears to increase (about 250 ) as the electrode becomes less lithiated and thins to 180 with increasing Li content (Li3.7Si). We attribute this breathing to the continual consumption of electrolyte with cycling.
Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1222554
Journal Information:
Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 35 Vol. 119; ISSN 1932-7447
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (40)

Silicon-Based Nanomaterials for Lithium-Ion Batteries: A Review journal October 2013
Toward High Cycle Efficiency of Silicon-Based Negative Electrodes by Designing the Solid Electrolyte Interphase journal November 2014
Electrodes: Lithium Intercalation Behavior in Multilayer Silicon Electrodes (Adv. Energy Mater. 7/2014) journal May 2014
Review of selected electrode–solution interactions which determine the performance of Li and Li ion batteries journal August 2000
Nano-morphology of lithiated thin film TiO2 anatase probed with in situ neutron reflectometry journal August 2003
Surface chemistry and morphology of the solid electrolyte interphase on silicon nanowire lithium-ion battery anodes journal April 2009
Quantifying capacity loss due to solid-electrolyte-interphase layer formation on silicon negative electrodes in lithium-ion batteries journal October 2012
Mantid—Data analysis and visualization package for neutron scattering and μ SR experiments
  • Arnold, O.; Bilheux, J. C.; Borreguero, J. M.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 764 https://doi.org/10.1016/j.nima.2014.07.029
journal November 2014
Quantitative Electrochemical Measurements Using In Situ ec-S/TEM Devices journal March 2014
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
In Situ Solid-State NMR Spectroscopy of Electrochemical Cells: Batteries, Supercapacitors, and Fuel Cells journal June 2013
Nanosilicon Electrodes for Lithium-Ion Batteries: Interfacial Mechanisms Studied by Hard and Soft X-ray Photoelectron Spectroscopy journal February 2012
Solid Electrolyte Interphase in Li-Ion Batteries: Evolving Structures Measured In situ by Neutron Reflectometry journal May 2012
Role of the LiPF 6 Salt for the Long-Term Stability of Silicon Electrodes in Li-Ion Batteries – A Photoelectron Spectroscopy Study journal January 2013
In Situ TEM on the Reversibility of Nanosized Sn Anodes during the Electrochemical Reaction journal July 2014
Nonaqueous Liquid Electrolytes for Lithium-Based Rechargeable Batteries journal October 2004
Electrolytes and Interphases in Li-Ion Batteries and Beyond journal October 2014
Improved Performances of Nanosilicon Electrodes Using the Salt LiFSI: A Photoelectron Spectroscopy Study journal June 2013
In Situ Observation of Solid Electrolyte Interphase Formation in Ordered Mesoporous Hard Carbon by Small-Angle Neutron Scattering journal March 2012
Lithium Ion Battery Graphite Solid Electrolyte Interphase Revealed by Microscopy and Spectroscopy journal January 2013
In Situ TEM Observation of the Electrochemical Process of Individual CeO 2 /Graphene Anode for Lithium Ion Battery journal February 2013
Silicon Solid Electrolyte Interphase (SEI) of Lithium Ion Battery Characterized by Microscopy and Spectroscopy journal June 2013
In Situ TEM Observation of Local Phase Transformation in a Rechargeable LiMn 2 O 4 Nanowire Battery journal November 2013
Chemistry, Impedance, and Morphology Evolution in Solid Electrolyte Interphase Films during Formation in Lithium Ion Batteries journal December 2013
Volume Expansion during Lithiation of Amorphous Silicon Thin Film Electrodes Studied by In-Operando Neutron Reflectometry journal April 2014
Impedance Analysis of Silicon Nanowire Lithium Ion Battery Anodes journal June 2009
X-ray Photoelectron Spectroscopy Studies of Lithium Surfaces Prepared in Several Important Electrolyte Solutions. A Comparison with Previous Studies by Fourier Transform Infrared Spectroscopy journal January 1996
Demonstration of an Electrochemical Liquid Cell for Operando Transmission Electron Microscopy Observation of the Lithiation/Delithiation Behavior of Si Nanowire Battery Anodes journal November 2013
In Situ and Quantitative Characterization of Solid Electrolyte Interphases journal February 2014
Nanoscale Imaging of Fundamental Li Battery Chemistry: Solid-Electrolyte Interphase Formation and Preferential Growth of Lithium Metal Nanoclusters journal February 2015
In Situ Transmission Electron Microscopy Observation of Electrochemical Sodiation of Individual Co 9 S 8 -Filled Carbon Nanotubes journal March 2014
7Li MRI of Li batteries reveals location of microstructural lithium journal February 2012
Interfacing electrolytes with electrodes in Li ion batteries journal January 2011
Direct measurement of the chemical reactivity of silicon electrodes with LiPF6-based battery electrolytes journal January 2014
Neutron reflectometry studies on the lithiation of amorphous silicon electrodes in lithium-ion batteries journal January 2013
Co-refinement of multiple-contrast neutron/X-ray reflectivity data using MOTOFIT journal March 2006
The Study of Surface Phenomena Related to Electrochemical Lithium Intercalation into Li[sub x]MO[sub y] Host Materials (M = Ni, Mn) journal January 2000
First Principles Model of Amorphous Silicon Lithiation journal January 2009
Electrode/Electrolyte Interface Studies in Lithium Batteries Using NMR journal January 2011
Surface Characterization of LiFePO4 Epitaxial Thin Films by X-ray/Neutron Reflectometry journal January 2010

Cited By (16)

Determination of the Solid Electrolyte Interphase Structure Grown on a Silicon Electrode Using a Fluoroethylene Carbonate Additive journal July 2017
The Atomic Scale Electrochemical Lithiation and Delithiation Process of Silicon journal September 2017
Mass‐Production of Electrospun Carbon Nanofiber Containing SiO x for Lithium‐Ion Batteries with Enhanced Capacity journal December 2018
Insights into solid electrolyte interphase formation on alternative anode materials in lithium-ion batteries journal December 2016
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
Dynamics and morphology of solid electrolyte interphase (SEI) journal January 2016
Electrolyte additives for lithium ion battery electrodes: progress and perspectives journal January 2016
In situ analytical techniques for battery interface analysis journal January 2018
Lithium insertion into silicon electrodes studied by cyclic voltammetry and operando neutron reflectometry journal January 2018
Role of conductive binder to direct solid–electrolyte interphase formation over silicon anodes journal January 2019
Roll-to-roll prelithiation of Sn foil anode suppresses gassing and enables stable full-cell cycling of lithium ion batteries journal January 2019
Designing superior solid electrolyte interfaces on silicon anodes for high-performance lithium-ion batteries journal January 2019
Silicon clathrates for lithium ion batteries: A perspective journal December 2016
Anodic decomposition of surface films on high voltage spinel surfaces—Density function theory and experimental study journal December 2019
Ion Diffusivity through the Solid Electrolyte Interphase in Lithium-Ion Batteries journal January 2017
Investigation of the Influence of Nanostructured LiNi 0.33 Co 0.33 Mn 0.33 O 2 Lithium-Ion Battery Electrodes on Performance and Aging journal January 2018

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