Intrinsic Chemical Reactivity of Silicon Electrode Materials: Gas Evolution

Claire Seitzinger, Robert Sacci, Jaclyn Coyle, Christopher Apblett, Kevin Hays, Ryan Armstrong, Alexander Rogers, Beth Armstrong, Taylor Bennet, Nathan Neale, Gabriel Veith

Research output: Contribution to journalArticlepeer-review

26 Scopus Citations

Abstract

In this work, we explore how the chemical reactivity toward an aprotic battery electrolyte changes as a function of lithium salt and silicon surface termination chemistry. The reactions are highly correlated, where one decomposition reaction leads to a subsequent decomposition reaction. The data show that the presence of silicon hydrides (SiHx) promotes the formation of CO gas, while surface oxides SiOx drive the formation of CO2. The extent and rate of oxidation depend on the surface basicity of the SiO2 surface species. The most acidic surfaces seem to hinder CO2 generation but not the decomposition of the salt. Indeed, the presence of F-containing salts (LiPF6 and LiTFSI) promotes the reactions between carbonate electrolyte and silicon surfaces. Surfaces with high Li content seem to be the most passivating to gassing reactions, pointing to a pathway to stabilize the interfaces during cell formation and assembly.

Original languageAmerican English
Pages (from-to)3199-3210
Number of pages12
JournalChemistry of Materials
Volume32
Issue number7
DOIs
StatePublished - 14 Apr 2020

Bibliographical note

Publisher Copyright:
Copyright © 2020 American Chemical Society.

NREL Publication Number

  • NREL/JA-5900-75872

Keywords

  • batteries
  • chemical reactivity
  • electrode materials

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