TY  - JOUR
AU  - Kubot, Maximilian
AU  - Balke, Lisa
AU  - Scholz, Johannes
AU  - Wiemers-Meyer, Simon
AU  - Karst, Uwe
AU  - Hayen, Heiko
AU  - Hur, Hyuck
AU  - Winter, Martin
AU  - Kasnatscheew, Johannes
AU  - Nowak, Sascha
TI  - High‐Voltage Instability of Vinylene Carbonate (VC): Impact of Formed Poly‐VC on Interphases and Toxicity
JO  - Advanced science
VL  - 11
IS  - 1
SN  - 2198-3844
CY  - Weinheim
PB  - Wiley-VCH
M1  - FZJ-2024-02545
SP  - 2305282
PY  - 2024
N1  - Unterstützt durch BMBF Grant: “BatGasMod” (03XP0311C), BMWK Grant: "Go3” (03ETE002D)
AB  - Full exhaustion in specific energy/energy density of state-of-the-art LiNixCoyMnzO2 (NCM)-based Li-ion batteries (LIB) is currently limited for reasons of NCM stability by upper cut-off voltages (UCV) below 4.3 V. At higher UCV, structural decomposition triggers electrode crosstalk in the course of enhanced transition metal dissolution and leads to severe specific capacity/energy fade; in the worst case to a sudden death phenomenon (roll-over failure). The additive lithium difluorophosphate (LiDFP) is known to suppress this by scavenging dissolved metals, but at the cost of enhanced toxicity due to the formation of organofluorophosphates (OFPs). Addition of film-forming electrolyte additives like vinylene carbonate (VC) can intrinsically decrease OFP formation in thermally aged LiDFP-containing electrolytes, though the benefit of this dual-additive approach can be questioned at higher UCVs. In this work, VC is shown to decrease the formation of potentially toxic OFPs within the electrolyte during cycling at conventional UCVs but triggers OFP formation at higher UCVs. The electrolyte contains soluble VC-polymerization products. These products are formed at the cathode during VC oxidation (and are found within the cathode electrolyte interphase (CEI), suggesting an OFP electrode crosstalk of VC decomposition species, as the OFP-precursor molecules are shown to be formed at the anode.
LB  - PUB:(DE-HGF)16
C6  - 37939283
UR  - <Go to ISI:>//WOS:001096887600001
DO  - DOI:10.1002/advs.202305282
UR  - https://juser.fz-juelich.de/record/1024894
ER  -