Water-in-Salt Electrolyte Promotes High-Capacity FeFe(CN)₆ Cathode for Aqueous Al-Ion Battery

Prussian blue analogues (PBAs) are considered to be ideal multivalent cation host materials due to their unique open-framework structure. In aqueous solution, however, the PBAs' cathodes have a low reversible capacity limited by the single electrochemical group Fe(CN)₆^3- and high crystal water content. They also suffer from fast cycle fading, resulting from significant oxygen/hydrogen evolution and cathode dissolution. In this work, a high-capacity PBA-type FeFe(CN)₆ cathode with double transition metal redox sites is successfully demonstrated in 5 m Al(CF₃SO₃)₃ Water-in-Salt electrolyte (Al-WISE). Due to Al-WISE having a wide electrochemical window (2.65 V) and low dissolution of the cathode, our PBA cathode exhibits a high discharge capacity of 116 mAh/g and the superior cycle stability >100 cycles with capacity fading of 0.39% per cycle.