Hierarchical CoNi-LDH nanosheet array with hydrogen vacancy for high-performance aqueous battery cathode

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Aqueous rechargeable multiple metal-ion storage battery (ARSB) has a large potential in energy storage devices due to their safe usage, low cost and high rate capability. Nevertheless, the performance of practical ARSB is largely restricted by low capacity and limited cathode materials. Herein, we demonstrate an efficient cathode material based on CoNi-layered double hydroxide (LDH) nanosheets arrays with abundant hydrogen vacancy induced by electrochemical activation process for high performance of cations storage. Consequently, the electrochemical activated CoNi-LDH (ECA-CoNi-LDH) nanosheets arrays exhibit high metal ion (Li+, Na+, Zn2+, Mg2+ and Ca2+) storage capacities, which is 9 times and 3 times higher that of unactivated CoNi-LDH arrays and ECA-CoNi-LDH without hierarchical structure, respectively. Moreover, the ECA-CoFe-LDH also shows the possibility for practical applications in actual batteries. By coupling with a Fe2O3/C anode, the assembled aqueous battery delivered a large energy density of 184.4 Wh kg−1 at power density of 4 Wh kg−1 in high voltage range of 0–2 V. To our best knowledge, such high energy density and large working window of our assembled aqueous battery is exceeded other LDH-based aqueous battery or supercapacitor, and the energy density almost comparable than that of commercial Li-ion batteries. Moreover, almost no measurable capacitance losses can be detected even after 10000 cycles. In addition, this work also provides a strategy to develop a high energy density cathode for multiple metal-ion storage batteries.