TY - JOUR AU - Haneke, Lukas AU - Pfeiffer, Felix AU - Rudolf, Katharina AU - Sutar, Pranti AU - Baghernejad, Masoud AU - Winter, Martin AU - Placke, Tobias AU - Kasnatscheew, Johannes TI - Investigating the Existence of a Cathode Electrolyte Interphase on Graphite in Dual‐Ion Batteries with LiPF 6 ‐Based Aprotic Electrolytes and Unraveling the Origin of Capacity Fade JO - Advanced energy & sustainability research VL - 6 IS - 3 SN - 2699-9412 CY - Weinheim PB - Wiley-VCH M1 - FZJ-2025-04673 SP - 2400330 PY - 2025 AB - This study elucidates the presence of a cathode electrolyte interphase (CEI) at graphite positive electrodes (PEs) and assesses its impact on the performance of dual-ion batteries, being promising candidates for cost-efficient and sustainable stationary energy storage. Indeed, electrolyte oxidation increases during charge (5 V vs Li|Li+) for decreased C rates, that is longer duration at high state-of-charges (SOC) , but effective protection and evidence for CEI formation is missing as no increase in Coulombic efficiencies is observed, even with literature-known electrolyte additives like vinylene carbonate, fluoroethylene carbonate, or ethylene sulfite in a highly concentrated base electrolyte (4.0 m LiPF6 in dimethyl carbonate) as reference. Via studying charged and pristine PEs by X-ray photoelectron spectroscopy, PF6−-graphite intercalation compounds and cointercalated solvent molecules are identified, while indications for CEI are absent within 1000 charge/discharge cycles. Nevertheless, a high capacity retention of ≈94% (referring to 0.1C) is demonstrated. Affirmed by Raman spectroscopy and scanning electron microscopy, the active material remains structurally stable, suggesting capacity fading to be dominated by resistance rise at the PE, likely due to an electronic contact resistance from active material grain boundaries and/or from the interface between electrode particles and the current collector in course of high volume changes; as systematically derived by impedance spectroscopy. LB - PUB:(DE-HGF)16 UR - <Go to ISI:>//WOS:001373740100001 DO - DOI:10.1002/aesr.202400330 UR - https://juser.fz-juelich.de/record/1048484 ER -