Compositions and Formation Mechanisms of Solid-Electrolyte Interphase on Microporous Carbon/Sulfur Cathodes

Wang, Luning; Lin, Yuxiao; DeCarlo, Samantha; Wang, Yi; Leung, Kevin; Qi, Yue; Xu, Kang; Wang, Chunsheng; Eichhorn, Bryan W.

doi:10.1021/acs.chemmater.9b05027

Compositions and Formation Mechanisms of Solid-Electrolyte Interphase on Microporous Carbon/Sulfur Cathodes

Journal Article · Thu Apr 02 00:00:00 EDT 2020 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.9b05027· OSTI ID:1634803

^[1]; Lin, Yuxiao ^[2]; DeCarlo, Samantha ^[1]; ^[1]; ^[3]; ^[2]; ^[4]; ^[1]; ^[5]

Univ. of Maryland, College Park, MD (United States). Dept. of Chemistry and Biochemistry
Michigan State Univ., East Lansing, MI (United States). Dept. of Chemical Engineering and Materials Science
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Army Research Lab., Adelphi, MD (United States). Electrochemistry Branch, Power and Energy Division Sensor and Electron Devices Directorate
Univ. of Maryland, College Park, MD (United States). Dept. of Chemistry and Biochemistry and Dept. of Chemical and Biomolecular Engineering

We report the formation mechanism and compositions of a solid-electrolyte interphase (SEI) on a microporous carbon/sulfur (MC/S) cathode in Li–S batteries using a carbonate-based electrolyte (1 M LiPF₆ in ethylene carbonate (EC)/dimethyl carbonate, v:v = 1:1). Through characterizations using 1D and 2D solution-phase nuclear magnetic resonance spectroscopy, coupled with model chemical reactions and DFT calculations, we have identified two critical roles of Li⁺ in steering the SEI formation. First, the preferential solvation of Li⁺ by EC in the mixed carbonate electrolyte renders EC as the dominant participant in the SEI formation, and second, Li⁺ coordination to the EC carbonyl alters activation barriers and changes the reaction pathways relative to Na⁺. The main organic components in the SEI are identified as lithium ethylene monocarbonate and lithium methyl carbonate, which are virtually identical to those formed on Li and graphite anodes of lithium-ion batteries but via a different pathway.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000; SC0001160; NA0003525

OSTI ID:: 1634803

Report Number(s):: SAND--2020-5284J; 686230

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 9 Vol. 32; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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