Rechargeable magnesium batteries have attracted considerable attention because of their potential high energy density and low cost. However, their development has been severely hindered because of the lack of appropriate cathode materials. Here we report a rechargeable magnesium/iodine battery, in which the soluble iodine reacts with Mg²⁺ to form a soluble intermediate and then an insoluble final product magnesium iodide. The liquid–solid two-phase reaction pathway circumvents solid-state Mg²⁺ diffusion and ensures a large interfacial reaction area, leading to fast reaction kinetics and high reaction reversibility. As a result, the rechargeable magnesium/iodine battery shows a better rate capability (180 mAh g⁻¹ at 0.5 C and 140 mAh g⁻¹ at 1 C) and a higher energy density (∼400 Wh kg⁻¹) than all other reported rechargeable magnesium batteries using intercalation cathodes. This study demonstrates that the liquid–solid two-phase reaction mechanism is promising in addressing the kinetic limitation of rechargeable magnesium batteries.

Aqueous zinc-ion batteries, in terms of integration with high safety, environmental benignity, and low cost, have attracted much attention for powering electronic devices and storage systems. However, the interface instability issues at the Zn anode caused by detrimental side reactions such as dendrite growth, hydrogen evolution, and metal corrosion at the solid (anode)/liquid (electrolyte) interface impede their practical applications in the fields requiring long-term performance persistence. Despite the rapid progress in suppressing the side reactions at the materials interface, the mechanism of ion storage and dendrite formation in practical aqueous zinc-ion batteries with dual-cation aqueous electrolytes is still unclear. Herein, we design an interface material consisting of forest-like three-dimensional zinc-copper alloy with engineered surfaces to explore the Zn plating/stripping mode in dual-cation electrolytes. The three-dimensional nanostructured surface of zinc-copper alloy is demonstrated to be in favor of effectively regulating the reaction kinetics of Zn plating/stripping processes. The developed interface materials suppress the dendrite growth on the anode surface towards high-performance persistent aqueous zinc-ion batteries in the aqueous electrolytes containing single and dual cations. This work remarkably enhances the fundamental understanding of dual-cation intercalation chemistry in aqueous electrochemical systems and provides a guide for exploring high-performance aqueous zinc-ion batteries and beyond.

Tremendous efforts have been devoted to replace commercial graphite anode (372 mAh g−1) by group IV elements (Si, Ge, Sn) based-materials with high capacities in lithium-ion batteries (LIBs). The use of these materials is hampered by the pulverization of these particles due to the high volumetric change during lithiation and delithiation cycles, which leads to particles pulverization and destabilization of solid electrolyte interphase (SEI) films. These problems result in fast capacity fading and low Coulombic efficiency. Nanostructured materials show significant improvements in rate capability and cyclability due to their high surface-to-volume ratio, reduced Li+ diffusion length, and increased freedom associated with the volume change during cycling. However, the nanostructured active materials with high ratio of surface-to-volume increase the irreversible capacity due to the formation of more SEI films. Although the nanostructured materials active materials keep relatively stable during repeated cycles of lithiation/delithiation process, the SEI film continually breaks/reforms, lowing the Coulombic efficiency. Meanwhile, the high-cost, low Coulombic efficiency and low tapping density limit the commercialization of the nanostructured electrode materials. Therefore, it is urgent to find solutions which could take advantage of both long cycle life of nanomaterials within the group IV elements (Si, Ge, Sn) and high volumetric/gravimetric capacity of micro-materials in the group IV as well as elements (Si, Ge, Sn). This report presents an overview of the recently developed strategies for improving the group IV elements (Si, Ge, Sn)-based anodes performances in LIBs to provide a further insight understanding in designing novel anodes