Abstract
Rechargeable aluminum-ion batteries have attracted increasing attention owing to the advantageous multivalent ion storage mechanism thus high theoretical capacity as well as inherent safety and low cost of using aluminum. However, their development has been largely impeded by the lack of suitable positive electrodes to provide both sufficient energy density and satisfactory rate capability. Here we report a candidate positive electrode based on ternary metal oxides, Fe(2)(MoO(4))(3), which was assembled by cross-stacking of porous nanosheets, featuring superior rate performance and cycle stability, and most importantly a well-defined discharge voltage plateau near 1.9 V. Specifically, the positive electrode is able to deliver reversible capacities of 239.3 mA h g(-1) at 0.2 A g(-1) and 73.4 mA h g(-1) at 8.0 A g(-1), and retains 126.5 mA h g(-1) at 1.0 A g(-1) impressively, after 2000 cycles. Furthermore, the aluminum-storage mechanism operating on Al(3+) intercalation in this positive electrode is demonstrated for the first time via combined in situ and ex situ characterization studies and density functional theory calculations. This work not only explores potential positive electrodes for aluminum-based batteries but also sheds light on the fundamental charge storage mechanism within the electrode.