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Title: Evaluating the solid electrolyte interphase formed on silicon electrodes: A comparison of ex situ X-ray photoelectron spectroscopy and in situ neutron reflectometry

Journal Article · · Physical Chemistry Chemical Physics. PCCP
DOI:https://doi.org/10.1039/C6CP00978F· OSTI ID:1261360
 [1];  [1];  [2];  [3];  [4];  [4];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. Missouri Univ. of Science and Technology, Rolla, MO (United States)
  4. Univ. of Missouri, Columbia, MO (United States)
+ Show Author Affiliations

This work details the in situ characterization of the interface between a silicon electrode and an electrolyte using a linear fluorinated solvent molecule, 0.1 M lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) in deuterated dimethyl perfluoroglutarate (d6-PF5M2) (1.87 x 10-2 mS/cm-1). The solid electrolyte interphase (SEI) composition and thickness determined via in situ neutron reflectometry (NR) and ex situ X-ray photoelectron spectroscopy (XPS) were compared. The data show that SEI expansion and contraction (breathing) during electrochemical cycling was observed via both techniques; however, ex situ XPS suggests that the SEI thickness increases during Si lithiation and decreases during delithiation, while in situ NR suggests the opposite. The most likely cause of this discrepancy is the selective removal of SEI components (top 20 nm of the SEI) during the electrode rinse process, required to remove electrolyte residue prior to ex situ analysis, demonstrating the necessity of performing SEI characterizations in situ.

Research Organization:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS); 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:
1261360
Journal Information:
Physical Chemistry Chemical Physics. PCCP, Vol. 18, Issue 20; ISSN 1463-9076
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 60 works
Citation information provided by
Web of Science

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Cited By (10)

Review of Recent Development of In Situ/Operando Characterization Techniques for Lithium Battery Research journal May 2019
The Atomic Scale Electrochemical Lithiation and Delithiation Process of Silicon journal September 2017
Computational Insights into Materials and Interfaces for Capacitive Energy Storage journal April 2017
In Situ Mechanical Analysis of the Nanoscopic Solid Electrolyte Interphase on Anodes of Li‐Ion Batteries journal June 2019
Binary Si–Ge Alloys as High‐Capacity Anodes for Li‐Ion Batteries journal November 2019
Determination of the Solid Electrolyte Interphase Structure Grown on a Silicon Electrode Using a Fluoroethylene Carbonate Additive journal July 2017
Silicon Surface Tethered Polymer as Artificial Solid Electrolyte Interface journal August 2018
Role of conductive binder to direct solid–electrolyte interphase formation over silicon anodes journal January 2019
Improving the electrochemical performance of Si-based anodes by co-compositing LiF and double carbon layer composed of graphite and three-dimensional PM journal September 2019
Ultrathin conformal polycyclosiloxane films to improve silicon cycling stability journal July 2019

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY