Fluorine‐Free Lithium‐Ion Capacitor with Enhanced Sustainability and Safety Based on Bio‐Based ƴ‐Valerolactone and Lithium Bis(Oxalato)Borate Electrolyte

Abstract In this work, the properties of a novel electrolyte based on the combination of bio‐based ƴ‐valerolactone (GVL) solvent with lithium bis(oxalato)borate (LiBOB) salt and its use for lithium‐ion capacitors (LICs) are presented. It is shown that the 1 m LiBOB in GVL electrolyte displays good transport properties, high thermal stability, and the ability to prevent anodic dissolution. Its impact on the performance of both battery‐type and capacitive‐type electrodes is evaluated. In this regard, special attention is paid to the filming properties associated with LiBOB and GVL decomposition at the electrode surfaces. To the best of the authors’ knowledge, the full‐cell devices assembled in this study are the first example of a fluorine‐free LIC. These devices exhibit a favorable energy‐to‐power ratio, delivering 80 Wh kg⁻¹_AM at 10 000 W kg⁻¹_AM along with excellent cycling stability, retaining 80% of the initial capacitance after 25 000 cycles. Furthermore, post‐mortem analysis of the LIC electrodes is conducted to gain deeper insights into the degradation mechanisms within the device.