Batteries & Supercaps ( IF 0 ) Pub Date : 2023-07-26 , DOI:
10.1002/batt.202300226PhilippSchweigart,ObinnaEgwuEleri,Inger-EmmaNylund,SamsonYuxiuLai,FengliuLou,AnnMariSvensson
Lithium-ion capacitors (LICs) represent promising high power energy storage devices, most commonly composed of a Li-ion intercalation anode (e.g., graphite or hard carbon), a supercapacitor activated carbon (AC) cathode, and an electrolyte with 1 M LiPF6 in carbonate solvents. Here, we report on the feasibility of replacing LiPF6 with the novel salt LiFSI for use with AC electrodes. Based on voltage hold measurements in a half-cell setup, good long-term stability is achieved with an upper cut-off voltage of 3.95 V vs. Li/Li+, potentially enabling cell voltages of ~3.8 V when combined with graphite anodes (operating at ~0.1 V vs. Li/Li+) in LIC full cells. The systematic comparison of cyclic voltammetry, leakage current analysis, and capacity retention upon voltage hold highlights the importance of the latter method to provide a realistic assessment of the electrochemical stability window of LiFSI on AC. The morphological and surface-chemical post-mortem analysis of AC electrodes used with LiFSI revealed that the oxidation of the FSI anion, as evidenced by the presence of new S 2p and N 1s features in the XPS spectra, and an increasing amount of oxygenated species on the AC were the main processes causing capacity fade at positive polarization.