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

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

doi:10.1016/j.jpowsour.2022.231021

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

Journal Article · Fri Jan 21 23:00:00 EST 2022 · Journal of Power Sources

DOI:https://doi.org/10.1016/j.jpowsour.2022.231021· OSTI ID:1878604

^[1]; Yang, Zhenzhen ^[2]; ^[1]; Trask, Stephen E. ^[2]; Rodrigues, Marco-Tulio F. ^[2]; ^[2]; Veith, Gabriel M. ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)

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. As a result, the superior passivation may be related to more stable lithium-solvent complexes.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: AC02-06CH11357; AC05-00OR22725

OSTI ID:: 1878604

Journal Information:: Journal of Power Sources, Journal Name: Journal of Power Sources Vol. 523; ISSN 0378-7753

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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