4.6 Article

Direct Determination of Solid-Electrolyte Interphase Thickness and Composition as a Function of State of Charge on a Silicon Anode

Journal

JOURNAL OF PHYSICAL CHEMISTRY C
Volume 119, Issue 35, Pages 20339-20349

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.5b06817

Keywords

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Funding

  1. Materials Sciences and Engineering Division, Office of Basic Energy Sciences, U.S. Department of Energy
  2. Fluid Interface Reactions, Structures, and Transport (FIRST) Center, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences
  3. U.S. Department of Energy, Office of Science, Office of Workforce Development for Teachers and Scientists, Office of Science Graduate Student Research (SCGSR) program
  4. Oak Ridge Institute for Science and Education for the DOE [DE-AC05-06OR23100]
  5. Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy
  6. National Nuclear Security Administration of the U.S. Department of Energy [DE-AC52-06NA25396]
  7. UT-Battelle, LLC [DE-AC05-00OR22725]

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With the use of 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 LIP like with increasing lithiation and more Li-C-O-F like with delithiation. More importantly, the SET layer thickness appears to increase (about 250 angstrom) as the electrode becomes less lithiated and thins to 180 angstrom with increasing Li content (Li3.7Si). We attribute this breathing to the continual consumption of electrolyte with cycling.

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