In Situ Chemical Imaging of Solid-Electrolyte Interphase Layer Evolution in Li–S Batteries

Nandasiri, Manjula I.; Camacho-Forero, Luis E.; Schwarz, Ashleigh M.; Shutthanandan, Vaithiyalingam; Thevuthasan, Suntharampillai; Balbuena, Perla B.; Mueller, Karl T.; Murugesan, Vijayakumar

doi:10.1021/acs.chemmater.7b00374

Title: In Situ Chemical Imaging of Solid-Electrolyte Interphase Layer Evolution in Li–S Batteries

Journal Article · 02 May 2017 · Chemistry of Materials

DOI: https://doi.org/10.1021/acs.chemmater.7b00374 · OSTI ID:1430633

Nandasiri, Manjula I. ^[1]; Camacho-Forero, Luis E. ^[2]; Schwarz, Ashleigh M. ^[3]; Shutthanandan, Vaithiyalingam ^[3]; Thevuthasan, Suntharampillai ^[3];

^[2];

^[4];

^[4]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States); TexasA&M University
Texas A & M Univ., College Station, TX (United States). Department of Chemical Engineering
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Joint Center for Energy Storage Research (JCESR)

Parasitic reactions of electrolyte and polysulfide with the Li-anode in lithium sulfur (Li-S) batteries lead to the formation of solid-electrolyte interphase (SEI) layers, which are the major reason behind severe capacity fading in these systems. Despite numerous studies, the evolution mechanism of the SEI layer and specific roles of polysulfides and other electrolyte components are still unclear. Here, we report an in-situ X-ray photoelectron spectroscopy (XPS) and chemical imaging analysis combined with ab initio molecular dynamics (AIMD) computational modeling to gain fundamental understanding regarding the evolution of SEI layers on Li-anodes within Li-S batteries. A multi-modal approach involving AIMD modeling and in-situ XPS characterization uniquely reveals the chemical identity and distribution of active participants in parasitic reactions as well as the SEI layer evolution mechanism. The SEI layer evolution has three major stages: the formation of a primary composite mixture phase involving stable lithium compounds (Li₂S, LiF, Li₂O etc); and formation of a secondary matrix type phase due to cross interaction between reaction products and electrolyte components, which is followed by a highly dynamic mono-anionic polysulfide (i.e. LiS₅) fouling process. In conclusion, these new molecular-level insights into the SEI layer evolution on Li- anodes are crucial for delineating effective strategies for the development of Li–S batteries.

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Research Organization:: Texas A&M Engineering Experiment Station, College Station, TX (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: EE0006832

OSTI ID:: 1430633

Alternate ID(s):: OSTI ID: 1371990

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 11 Vol. 29; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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