%0 Journal Article %A Klein, Sven %A Wrogemann, Jens Matthies %A van Wickeren, Stefan %A Harte, Patrick %A Bärmann, Peer %A Heidrich, Bastian %A Hesper, Jakob %A Borzutzki, Kristina %A Nowak, Sascha %A Börner, Markus %A Winter, Martin %A Kasnatscheew, Johannes %A Placke, Tobias %T Understanding the Role of Commercial Separators and Their Reactivity toward LiPF 6 on the Failure Mechanism of High‐Voltage NCM523 || Graphite Lithium Ion Cells %J Advanced energy materials %V 12 %N 2 %@ 1614-6832 %C Weinheim %I Wiley-VCH %M FZJ-2021-05231 %P 2102599 - %D 2022 %X NCM523 || graphite lithium ion cells operated at 4.5 V are prone to an early “rollover” failure, due to electrode cross-talk, that is, transition metal (TM = Mn, Ni, and Co) dissolution from NCM523 and deposition at graphite, subsequent formation of Li metal dendrites, and, in the worst case, generation of (micro-)short-circuits by dendrites growing to the cathode. Here, the impact of different separators on the high-voltage performance of NCM523 || graphite cells is elucidated focusing on the separators’ structural properties (e.g., membrane vs fiber) and their reactivity toward LiPF6 (e.g., ceramic-coated separators). First, the separator architecture has a major impact on cycle life. Fiber-structured separators can prevent the “rollover” failure by a more homogeneous deposition of TMs and formation of Li metal dendrites, thus, hindering penetration of dendrites to the cathode. In contrast, porous membrane-structured separators cannot prevent the cell failure due to inhomogeneous TM deposits/Li metal dendrites. Second, it is demonstrated that different types of ceramic-coated separators (Boehmite (γ-AlO(OH)) vs α-Al2O3) exhibit different reactivities toward LiPF6. While α-Al2O3 shows a minor reactivity toward LiPF6, the γ-AlO(OH) coating leads to in situ formation of the beneficial difluorophosphate anion in high amounts due the high reactivity toward LiPF6 decomposition, which significantly improves cycle life. %F PUB:(DE-HGF)16 %9 Journal Article %U <Go to ISI:>//WOS:000725443500001 %R 10.1002/aenm.202102599 %U https://juser.fz-juelich.de/record/903576