Novel Charging-Optimized Cathode for a Fast and High-Capacity Zinc-Ion Battery.

A rechargeable aqueous zinc-ion battery (ZIB) is one of the attractive candidates for large-scale energy storage. Its further application relies on the exploitation of a high-capacity cathode and the understanding of an intrinsic energy storage mechanism. Herein, we report a novel layered K ₂ V ₃ O ₈ cathode material for the ZIB, adopting a strategy of charging first to extract part of K-ions from vanadate in initial few cycles, which creates more electrochemically active sites and lowers charge-transfer resistance of the ZIB system. As a result, a considerable specific capacity of 302.8 mA h g ^-1 at 0.1 A g ^-1 , as well as a remarkable cycling stability (92.3% capacity retention at 4 A g ^-1 for 2000 cycles) and good rate capability, are achieved. Besides, the energy storage mechanism was studied by in situ X-ray diffraction, in situ Raman spectroscopy, X-ray photoelectron spectroscopy, and inductively coupled plasma mass spectroscopy. An irreversible K-ion deintercalation in the first charge process is proved. It is believed that this novel cathode material for the rechargeable aqueous ZIB and the optimizing strategy will shed light on developing next-generation large-scale energy storage devices.