Role of Catalytic Conversions of Ethylene Carbonate, Water, and HF in Forming the Solid-Electrolyte Interphase of Li-Ion Batteries
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Role of Catalytic Conversions of Ethylene Carbonate, Water, and HF in Forming the Solid-Electrolyte Interphase of Li-Ion Batteries. / 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.
I: ACS Catalysis, Bind 13, Nr. 13, 2023, s. 9289-9301.Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt
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TY - JOUR
T1 - Role of Catalytic Conversions of Ethylene Carbonate, Water, and HF in Forming the Solid-Electrolyte Interphase of Li-Ion Batteries
AU - Martins, Milena
AU - Haering, Dominik
AU - Connell, Justin G.
AU - Wan, Hao
AU - Svane, Katrine L.
AU - Genorio, Bostjan
AU - Farinazzo Bergamo Dias Martins, Pedro
AU - Lopes, Pietro P.
AU - Gould, Brian
AU - Maglia, Filippo
AU - Jung, Roland
AU - Stamenkovic, Vojislav
AU - Castelli, Ivano E.
AU - Markovic, Nenad M.
AU - Rossmeisl, Jan
AU - Strmcnik, Dusan
PY - 2023
Y1 - 2023
N2 - 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.
AB - 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.
U2 - 10.1021/acscatal.3c01531
DO - 10.1021/acscatal.3c01531
M3 - Journal article
VL - 13
SP - 9289
EP - 9301
JO - ACS Catalysis
JF - ACS Catalysis
SN - 2155-5435
IS - 13
ER -
ID: 359082960