Evaluating the roles of electrolyte components on the passivation of silicon anodes

Thomas F. Malkowski, Zhenzhen Yang, Robert L. Sacci, Stephen E. Trask, Marco Tulio F. Rodrigues, Ira D. Bloom, Gabriel M. Veith

Research output: Contribution to journalArticlepeer-review

14 Scopus citations

Abstract

A protocol was recently developed to compare calendar life using a constant potential while monitoring the electrical current required to maintain the potential. Here, this calendar life protocol is used with electrolyte formulations containing various mole fractions of ethylene carbonate (EC), ethyl methyl carbonate (EMC), and LiPF6 to elucidate the role each component plays in passivation for high silicon anodes. Together, EC and LiPF6 lead to higher currents, and thus poorer passivation, whereas EMC acts as a spectator. The variation of the components’ mole fraction also changes the solid-electrolyte interphase (SEI) composition, as measured by x-ray photoelectron spectroscopy. Importantly, higher LiPF6 content leads to increased LiF as well as increased current, indicating that higher LiF content does not enhance the passivation of the silicon surface. Finding that EC did not yield a passivating SEI, instead ethylene sulfite, sulfolane, and propylene carbonate (PC) were used in place of EC. Using ethylene sulfite and sulfolane resulted in poorer passivation compared to EC, whereas PC resulted in superior passivation. The superior passivation may be related to more stable lithium-solvent complexes.

Original languageEnglish
Article number231021
JournalJournal of Power Sources
Volume523
DOIs
StatePublished - Mar 1 2022

Funding

This research was supported by the US Department of Energy's (DOE's) Vehicle Technologies Office under the Silicon Consortium Project, directed by Brian Cunningham and managed by Anthony Burrell. This manuscript has been authored by UT-Battelle LLC under Contract No. DE-AC05-00OR22725 with DOE. Argonne is operated for the DOE Office of Science by UChicago Argonne LLC under contract number DE-AC02-06CH11357. The electrodes used in this article were made by Argonne's CAMP Facility, which was supported by the Applied Battery Research for Transportation Program directed by David Howell. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). This research was supported by the US Department of Energy's (DOE's) Vehicle Technologies Office under the Silicon Consortium Project, directed by Brian Cunningham and managed by Anthony Burrell. This manuscript has been authored by UT-Battelle LLC under Contract No. DE-AC05-00OR22725 with DOE. Argonne is operated for the DOE Office of Science by UChicago Argonne LLC under contract number DE-AC02-06CH11357. The electrodes used in this article were made by Argonne's CAMP Facility, which was supported by the Applied Battery Research for Transportation Program directed by David Howell. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ).

Keywords

  • Anode
  • Lithium
  • Silicon
  • Solid-electrolyte interphase

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