Utilization of Interfacial Charge Storage toward Ultra-high Capacity: Li₂SO₄ Sealed Micron Sized Iron Oxides as Anode for Lithium Batteries

The interfacial charge storage is derived from spin-polarized electrons stored on the surface of iron metal nanoparticles, and reasonable utilization can achieve a capacity far beyond the traditional conversion mechanism. Generally, iron oxide is easy to crack, pulverize, and fall off due to its poor conductivity and large volume change during cycling, and causes serious side reactions with the electrolyte. Herein, this pulverization phenomenon was intentionally utilized to in situ form nano-sized iron particles and create a large number of Fe/Li2O interfaces. Specifically, a Li+ conductor like Li2SO4 was utilized to seal micron sized iron oxides and also work as an aggregation barrier. Thus, the in situ formed nanoparticles were separated from the electrolyte and could provide huge capacity through interfacial charge storage. Therefore, the specific capacity of this unique composite continues to rise upon activation cycling and finally reaches 1708 mA h g–1, which is more than twice its theoretical capacity based on the conversion mechanism. The gradually increasing interfacial charge storage capacity was also directly confirmed by X-ray photoelectron spectroscopy tests. This novel strategy provides new opportunities for the design and commercialization of advanced energy storage systems.