Owing to its unique structure, Chevrel phase (CP) is a promising candidate for applications in rechargeable multivalent (Mg and Al) batteries. However, its wide applications are severely limited by time-consuming and complex synthesis processes, accompanied by uncontrollable growth and large particle sizes, which will magnify the charge trapping effect and lower the electrochemical performance. Here, an iodine vapor transport reaction (IVT) is proposed to obtain large-scale and highly pure Mo6S8 nanosheets, in which iodine helps to regulate the growth kinetics and induce the preferential growth of Mo6S8, as a typical three-dimensional material, to form nanosheets. When applied in rechargeable multivalent (Mg and Al) batteries, Mo6S8 nanosheets show very fast kinetics owing to the short diffusion distance, thereby exhibiting lower polarization, higher capacities, and better low-temperature performance (up to −40 °C) compared to that of microparticles obtained via the conventional method. It is anticipated that Mo6S8 nanosheets would boost the application of Chevrel phase, especially in areas of energy storage and catalysis, and the IVT reaction would be generalized to a wide range of inorganic compound nanosheets.

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.