Thermogravimetric Evolved Gas Analysis and Microscopic Elemental Mapping of the Solid Electrolyte Interphase on Silicon Incorporated in Free-Standing Porous Carbon Electrodes

George Hasegawa, Kazuyoshi Kanamori, Kazuki Nakanishi, Katsuro Hayashi

Research output: Contribution to journalArticle

Abstract

Free-standing electrodes, which are free from additives (binders and conductive agents) and even current collectors, are useful in terms of both application research and fundamental study. Here, we demonstrate the preparation of binder-free monolithic carbon electrodes embracing Si nanoparticles in their well-defined porous scaffolds via the one-pot sol-gel reaction followed by carbonization. The free-standing electrodes with a thickness of 150 μm work out as a high-areal-density anode for Li-ion batteries, delivering up to ca. 7 mA h cm-2. As the Si content increases, the capacity decay on cycling becomes pronounced, which is likely to associate with the fracturing and pulverization of Si nanoparticles even with the size smaller than 100 nm after long-term cycles. The thermogravimetry-mass spectrometry profile of the cycled electrode corroborates the successive electrolyte decomposition to grow solid electrolyte interphase (SEI) mainly composed of lithium alkylcarbonates, polymeric species, and LiF, rendering the electrode mass nearly double of its original state after 200 cycles. The elemental mapping analysis reveals that LiF is generated inhomogeneously in the monolithic electrodes unlike the other SEI components, resulting in the concentration gradient depending on the distance from a Li counter electrode.

Original languageEnglish
Pages (from-to)12680-12688
Number of pages9
JournalLangmuir
Volume35
Issue number39
DOIs
Publication statusPublished - Oct 1 2019

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Gas fuel analysis
gas analysis
Solid electrolytes
solid electrolytes
Silicon
Carbon
Electrodes
electrodes
carbon
silicon
cycles
Binders
Nanoparticles
nanoparticles
carbonization
fracturing
Carbonization
thermogravimetry
Lithium
Scaffolds

All Science Journal Classification (ASJC) codes

  • Materials Science(all)
  • Condensed Matter Physics
  • Surfaces and Interfaces
  • Spectroscopy
  • Electrochemistry

Cite this

Thermogravimetric Evolved Gas Analysis and Microscopic Elemental Mapping of the Solid Electrolyte Interphase on Silicon Incorporated in Free-Standing Porous Carbon Electrodes. / Hasegawa, George; Kanamori, Kazuyoshi; Nakanishi, Kazuki; Hayashi, Katsuro.

In: Langmuir, Vol. 35, No. 39, 01.10.2019, p. 12680-12688.

Research output: Contribution to journalArticle

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