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Reaction Mechanisms of the Degradation of Fluoroethylene Carbonate, an Additive of Lithium‐Ion Batteries, Unraveled by Radiation Chemistry
Author(s) -
Puget Marin,
Shcherbakov Viacheslav,
Denisov Sergey,
Moreau Philippe,
Dog JeanPierre,
Mostafavi Mehran,
Le Caër Sophie
Publication year - 2021
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.202100562
Subject(s) - radiolysis , chemistry , oxidizing agent , electrolyte , lithium (medication) , solvation , solvated electron , photochemistry , degradation (telecommunications) , ion , carbonate , inorganic chemistry , radical , electrode , organic chemistry , medicine , telecommunications , endocrinology , computer science
Numerous additives are used in the electrolytes of lithium‐ion batteries, especially for the formation of an efficient solid electrolyte interphase at the surface of the electrodes. Understanding the degradation processes of these compounds is thus important; they can be seen through radiolysis. In the case of fluoroethylene carbonate (FEC), picosecond pulse radiolysis experiments evidenced the formation of FEC .− . This radical is stabilized in neat FEC, whereas the ring opens to form more stable radical anions when FEC is a solute in other solvents, as confirmed by quantum chemistry calculations. In neat FEC, pre‐solvated electrons primarily undergo attachment rather than solvation. On long timescales, the gases produced (H 2 , CO, and CO 2 ) were quantified. A reaction scheme for both the oxidizing and reducing pathways at stake in irradiated FEC is proposed. This work shows that the nature of the primary species formed in FEC depends on the amount of FEC in the solution.