Role of catalytic conversions of ethylene carbonate, water, and HF in forming the solid-electrolyte interphase of Li-ion batteries

Martins, Milena (author), Haering, Dominik (author), Connell, Justin Grant (author), Wan, Hao (author), Svane, Katrine L. (author), Genorio, Boštjan (author), Farinazzo Bergamo Dias Martins, Pedro (author), Lopes, Pietro P. (author), Gould, Brian (author), Maglia, Filippo (author), Jung, Roland (author), Stamenkovic, Vojislav (author), Castelli, Ivano E. (author), Markovic, Nenad M. (author), Rossmeisl, Jan (author), Strmčnik, Dušan (author)

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 theoretical study of the electrochemistry 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 electrocatalytic nature of EC, HF, and water electroreductions at all interfaces, and unveil the catalytic role of water in EC electroreduction. 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.

• Language: English
• Keywords: Li-ion battery, solid-electrolyte interphase, electroreduction, ethylene carbonate, HF, water, electrodes, electrolytes, fourier transform infrared spectroscopy, metals, surface chemistry
• Work type: Article
• Typology: 1.01 - Original Scientific Article
• Organization: FKKT - Faculty of Chemistry and Chemical Technology
• Publication status: Published
• Publication version: Version of Record
• Year: 2023
• Number of pages: Str. 9289-9301
• Numbering: Vol. 13, iss. 13
• PID: 20.500.12556/RUL-148257
• UDC: 621.355
• ISSN on article: 2155-5435
• DOI: 10.1021/acscatal.3c01531
• COBISS.SI-ID: 160329731
• Publication date in RUL: 07.08.2023

Record is a part of a journal

• Title: ACS catalysis
• Shortened title: ACS catal.
• Publisher: American Chemical Society
• ISSN: 2155-5435
• COBISS.SI-ID: 518529817

Licences

• License: CC BY 4.0, Creative Commons Attribution 4.0 International
• Link: http://creativecommons.org/licenses/by/4.0/
• Description: This is the standard Creative Commons license that gives others maximum freedom to do what they want with the work as long as they credit the author.

Secondary language

• Language: Slovenian
• Keywords: Li-ionski akumulatorji, medfaza trdni elektrolit, elektroredukcija, etilen karbonat, HF, voda

Projects

• Funder: Other - Other funder or multiple funders
• Funding programme: BMW Technology Corporation