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@ARTICLE{Kubot:1025932,
author = {Kubot, Maximilian and von Holtum, Bastian and Winter,
Martin and Wiemers-Meyer, Simon and Nowak, Sascha},
title = {{O}rganofluorophosphates as {O}xidative {D}egradation
{P}roducts in {H}igh-{V}oltage {L}ithium {I}on {B}atteries
with {NMC} or {LNMO} {C}athodes},
journal = {Journal of the Electrochemical Society},
volume = {169},
number = {11},
issn = {0013-4651},
address = {Bristol},
publisher = {IOP Publishing},
reportid = {FZJ-2024-03210},
pages = {110534 -},
year = {2022},
abstract = {Organofluorophosphates (OFPs) have been reported to pose
substantial health hazards due to their structural
similarities to pesticides and nerve agents. Formation of
OFPs in lithium ion batteries (LIBs) due to hydrolysis of
the conducting salt lithium hexafluorophosphate (LiPF6) and
the reaction with the organic carbonate solvents that make
up the electrolyte has been discussed in literature. The
oxidative formation of OFPs in electrolytes containing
fluoroethylene carbonate (FEC) and vinylene carbonate (VC)
as film-forming additives is presented in this study.
Further the impact of potentially reactive positive
electrode surfaces is investigated with the layered metal
oxide NCM622 which is ascribed to release reactive oxygen
species at high voltages and the spinel type LNMO as a
typical high-voltage material. Cycling of the self-assembled
LIB coin cells (CR2032) at cut-off voltages of 4.8 V gave
rise to a number of degradation products including
potentially highly toxic OFPs. Here, the presence of the
film-forming additive had a massive impact on the amount of
OFPs formed during electrochemical cycling experiments,
which raises further concerns for the utilization of
film-forming additives for high voltage applications. The
formation pathway of OFPs through EC-polymerization proposed
in literature is evaluated and an alternative mechanism with
FEC/VC as the carbonyl carbon-donor is presented. Structure
elucidation and separation of the formed OFPs is achieved by
utilization of reversed-phase (RP) chromatography hyphenated
to a high-resolution ion trap time-of-flight mass
spectrometer (IT-TOF-MS). The findings presented in this
study support further investigation of the formation of OFPs
in film-forming additive-containing electrolytes,
quantitative approaches and toxicological assessments due to
the highly toxic nature of OFPs.},
cin = {IEK-12},
ddc = {660},
cid = {I:(DE-Juel1)IEK-12-20141217},
pnm = {1221 - Fundamentals and Materials (POF4-122) / BMBF
03XP0311B - BatgasMod - Batteriegasungs-Modellierung
(03XP0311B)},
pid = {G:(DE-HGF)POF4-1221 / G:(BMBF)03XP0311B},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000889361400001},
doi = {10.1149/1945-7111/aca2e8},
url = {https://juser.fz-juelich.de/record/1025932},
}