In Situ Chemical Imaging of Solid-Electrolyte Interphase Layer Evolution in Li–S Batteries
Abstract
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 strategiesmore »
- Authors:
-
[2];
[3];
[3]
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Texas A & M Univ., College Station, TX (United States). Department of Chemical Engineering
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Joint Center for Energy Storage Research (JCESR)
- Publication Date:
- Research Org.:
- Texas A & M Univ., College Station, TX (United States). Texas A & M Engineering Experiment Station
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1430633
- Grant/Contract Number:
- EE0006832
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 29; Journal Issue: 11; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Nandasiri, Manjula I., Camacho-Forero, Luis E., Schwarz, Ashleigh M., Shutthanandan, Vaithiyalingam, Thevuthasan, Suntharampillai, Balbuena, Perla B., Mueller, Karl T., and Murugesan, Vijayakumar. In Situ Chemical Imaging of Solid-Electrolyte Interphase Layer Evolution in Li–S Batteries. United States: N. p., 2017.
Web. doi:10.1021/acs.chemmater.7b00374.
Nandasiri, Manjula I., Camacho-Forero, Luis E., Schwarz, Ashleigh M., Shutthanandan, Vaithiyalingam, Thevuthasan, Suntharampillai, Balbuena, Perla B., Mueller, Karl T., & Murugesan, Vijayakumar. In Situ Chemical Imaging of Solid-Electrolyte Interphase Layer Evolution in Li–S Batteries. United States. https://doi.org/10.1021/acs.chemmater.7b00374
Nandasiri, Manjula I., Camacho-Forero, Luis E., Schwarz, Ashleigh M., Shutthanandan, Vaithiyalingam, Thevuthasan, Suntharampillai, Balbuena, Perla B., Mueller, Karl T., and Murugesan, Vijayakumar. Wed .
"In Situ Chemical Imaging of Solid-Electrolyte Interphase Layer Evolution in Li–S Batteries". United States. https://doi.org/10.1021/acs.chemmater.7b00374. https://www.osti.gov/servlets/purl/1430633.
@article{osti_1430633,
title = {In Situ Chemical Imaging of Solid-Electrolyte Interphase Layer Evolution in Li–S Batteries},
author = {Nandasiri, Manjula I. and Camacho-Forero, Luis E. and Schwarz, Ashleigh M. and Shutthanandan, Vaithiyalingam and Thevuthasan, Suntharampillai and Balbuena, Perla B. and Mueller, Karl T. and Murugesan, Vijayakumar},
abstractNote = {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.},
doi = {10.1021/acs.chemmater.7b00374},
journal = {Chemistry of Materials},
number = 11,
volume = 29,
place = {United States},
year = {Wed May 03 00:00:00 EDT 2017},
month = {Wed May 03 00:00:00 EDT 2017}
}
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