Role of Catalytic Conversions of Ethylene Carbonate, Water, and HF in Forming the Solid-Electrolyte Interphase of Li-Ion Batteries
Abstract
Compared to aqueous electrolytes, fundamental understanding of the chemical and electrochemical processes occurring in non-aqueous electrolytes is far less developed. This is no different for Li-ion battery (LiB) electrolytes, where many questions regarding the solid-electrolyte interphase (SEI) on the anode side remain unanswered, including its chemical composition, the mechanism of formation, and its impact on LiB performance. Here, we present a detailed experimental and the oreticalstudy of the electro chemistry of ethylene carbonate (EC) and its chemical relationship with trace amounts of water and HF across a vast range of electrode materials, from well-ordered single crystals to realistic graphite electrodes. We reveal the electro catalytic nature of EC,HF, and water electro reductions at all interfaces, and unveil the catalytic role of water in EC electro reduction. Moreover, we show that these reactions are connected in a closed cycle by chemical reactions that take place either at the electrode/electrolyte interface or in the bulk of the electrolyte and demonstrate that the composition of the SEI depends predominantly on the balance between the (electro)chemistry of EC, water, and HF.
- Authors:
-
[3];
[6];
[7];
[3];
[9];
[2];
[5];
[4];
[1]
- Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States, National Institute of Chemistry, SI-1000 Ljubljana, Slovenia
- Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States, Department of Chemical and Biomolecular Engineering, Horiba Institute for Mobility and Connectivity, University of California Irvine, Irvine, California 92697, United States
- Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States
- Nano-Science Center, Department of Chemistry, University of Copenhagen, DK-2100 Copenhagen, Denmark
- Department of Energy Conversion and Storage, Technical University of Denmark, DK-2800 Kgs. Lyngby, Denmark
- Faculty of Chemistry and Chemical Technology, University of Ljubljana, Vecna Pot 113, SI-1000 Ljubljana, Slovenia
- Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States, National Institute of Chemistry, SI-1000 Ljubljana, Slovenia, Faculty of Chemistry and Chemical Technology, University of Ljubljana, Vecna Pot 113, SI-1000 Ljubljana, Slovenia
- Battery Cell Technology, BMW Group, 80788 München, Germany, Institute for Advanced Study, Technical University of Munich, Lichtenbergstrasse 2a, D-85748 Garching, Germany
- Battery Cell Technology, BMW Group, 80788 München, Germany
- Publication Date:
- Research Org.:
- National Institute of Chemistry Slovenia, Ljubljana (Slovenia); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC)
- OSTI Identifier:
- 1987443
- Alternate Identifier(s):
- OSTI ID: 1988732; OSTI ID: 2337468
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Published Article
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Name: ACS Catalysis Journal Volume: 13 Journal Issue: 13; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Li-ion battery; solid-electrolyte interphase; electroreduction; ethylene carbonate; HF; water; electrodes; electrolytes; Fourier transform infrared spectroscopy; metals; surface chemistry
Citation Formats
Martins, Milena, Haering, Dominik, Connell, Justin G., Wan, Hao, Svane, Katrine L., Genorio, Bostjan, Farinazzo Bergamo Dias Martins, Pedro, Lopes, Pietro P., Gould, Brian, Maglia, Filippo, Jung, Roland, Stamenkovic, Vojislav, Castelli, Ivano E., Markovic, Nenad M., Rossmeisl, Jan, and Strmcnik, Dusan. Role of Catalytic Conversions of Ethylene Carbonate, Water, and HF in Forming the Solid-Electrolyte Interphase of Li-Ion Batteries. United States: N. p., 2023.
Web. doi:10.1021/acscatal.3c01531.
Martins, Milena, Haering, Dominik, Connell, Justin G., Wan, Hao, Svane, Katrine L., Genorio, Bostjan, Farinazzo Bergamo Dias Martins, Pedro, Lopes, Pietro P., Gould, Brian, Maglia, Filippo, Jung, Roland, Stamenkovic, Vojislav, Castelli, Ivano E., Markovic, Nenad M., Rossmeisl, Jan, & Strmcnik, Dusan. Role of Catalytic Conversions of Ethylene Carbonate, Water, and HF in Forming the Solid-Electrolyte Interphase of Li-Ion Batteries. United States. https://doi.org/10.1021/acscatal.3c01531
Martins, Milena, Haering, Dominik, Connell, Justin G., Wan, Hao, Svane, Katrine L., Genorio, Bostjan, Farinazzo Bergamo Dias Martins, Pedro, Lopes, Pietro P., Gould, Brian, Maglia, Filippo, Jung, Roland, Stamenkovic, Vojislav, Castelli, Ivano E., Markovic, Nenad M., Rossmeisl, Jan, and Strmcnik, Dusan. Tue .
"Role of Catalytic Conversions of Ethylene Carbonate, Water, and HF in Forming the Solid-Electrolyte Interphase of Li-Ion Batteries". United States. https://doi.org/10.1021/acscatal.3c01531.
@article{osti_1987443,
title = {Role of Catalytic Conversions of Ethylene Carbonate, Water, and HF in Forming the Solid-Electrolyte Interphase of Li-Ion Batteries},
author = {Martins, Milena and Haering, Dominik and Connell, Justin G. and Wan, Hao and Svane, Katrine L. and Genorio, Bostjan and Farinazzo Bergamo Dias Martins, Pedro and Lopes, Pietro P. and Gould, Brian and Maglia, Filippo and Jung, Roland and Stamenkovic, Vojislav and Castelli, Ivano E. and Markovic, Nenad M. and Rossmeisl, Jan and Strmcnik, Dusan},
abstractNote = {Compared to aqueous electrolytes, fundamental understanding of the chemical and electrochemical processes occurring in non-aqueous electrolytes is far less developed. This is no different for Li-ion battery (LiB) electrolytes, where many questions regarding the solid-electrolyte interphase (SEI) on the anode side remain unanswered, including its chemical composition, the mechanism of formation, and its impact on LiB performance. Here, we present a detailed experimental and the oreticalstudy of the electro chemistry of ethylene carbonate (EC) and its chemical relationship with trace amounts of water and HF across a vast range of electrode materials, from well-ordered single crystals to realistic graphite electrodes. We reveal the electro catalytic nature of EC,HF, and water electro reductions at all interfaces, and unveil the catalytic role of water in EC electro reduction. Moreover, we show that these reactions are connected in a closed cycle by chemical reactions that take place either at the electrode/electrolyte interface or in the bulk of the electrolyte and demonstrate that the composition of the SEI depends predominantly on the balance between the (electro)chemistry of EC, water, and HF.},
doi = {10.1021/acscatal.3c01531},
journal = {ACS Catalysis},
number = 13,
volume = 13,
place = {United States},
year = {Tue Jun 27 00:00:00 EDT 2023},
month = {Tue Jun 27 00:00:00 EDT 2023}
}
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