Bimetallic ions pre-intercalated hydrated vanadium oxides for high-performance aqueous zinc-ion batteries

A new generation of rechargeable batteries known as Aqueous Zinc-Ion Batteries (AZIB) offers benefits including affordability, eco-friendliness, dependability, and safety. Hydrated vanadium oxides (V2O5 center dot nH2O) show potential as cathodes for AZIB due to their layered structure and multivalent properties. However, the zinc storage performance is limited by the structural instability and slow zinc ion mobility. In this work, TiK-VOH (the bimetallic ions system of Ti4+ and K+ co-pre-intercalated in V2O5 center dot nH2O) with lamellar fish scale-like structure is synthesized using a simple sol-gel method. The high positive charge density of the tetravalent Ti4+ is more beneficial to attract the electrons in the V-O layer and regulate the layer spacing (12.1 & Aring;), which not only improves the diffusion kinetics of zinc ions, but also acts as a pillar to stabilize the layer structure. K+ mainly plays the role of improving electrical conductivity, and then accelerates the charge transfer in the electrode reaction process. Auxiliary density functional theory simulation further confirms that the diffusion energy barrier and Fermi level are optimized by pre-intercalating bimetallic ions. Based on the synergistic effect of Ti4+ and K+, the TiK-VOH material shows excellent zinc storage performance, the highest specific capacity of TiK-VOH reaches 393.4 mAh g- 1 at a current density of 0.2 A g- 1, even at 10 A g- 1 (increased by 20 times), it still maintains a discharge specific capacity of 202 mAh g- 1 with a capacity retention rate of 94 % after 2000 cycles, the overall performance is much better than the Ti-VOH and K-VOH. This work offers an alternative perspective for the modification of vanadium-based cathode of AZIBs.