In-situ preparation of amorphous VO2@rGO cathode for ultra-high capacity and ultra-long cycle life aqueous zinc ion batteries

Aqueous zinc-ion batteries (AZIBs) are considered as a promising alternative to lithium-ion batteries for stationary energy storage due to their environmental benignity and cost-effectiveness. However, the development of AZIBs continues to be plagued by a lack of cathode materials with high specific capacity and superior lifetime. Herein, we in-situ synthesize amorphous VO2@rGO assisted by controlling the charging cut-off voltage. Experimental results and theoretical calculations confirm that the amorphous VO2(A)@rGO can effectively reduce the migration energy barrier of Zn2+, improve the conductivity of the electrode, and promote the insertion/extraction of Zn2+. Consequently, the Zn//VO2(A)@rGO battery exhibits an ultra-high specific capacity of 527.0 mAh·g−1 at 1 A·g−1 after 100 cycles, an ultra-long cycle stability of 183.4 mAh·g−1 at 20 A·g−1 after 30,000 cycles, and an energy of 316.1 Wh·Kg−1 at a power density of 6082.9 W·Kg−1 power density. Meanwhile, we reveal that the amorphous VO2@rGO electrode follows a hybrid mechanism of classical Zn2+ insertion/de-insertion and the reversible phase transition from amorphous VO2 to V2O3. This study highlights that in-situ preparation of amorphous VO2@rGO cathode materials by controlling the charging voltage interval, opening up further possibilities for the development of high-performance AZIB cathodes.