We demonstrate a facile hydrothermal method for growth of ultrathin NiCo2S4 nanosheets on reduced graphene oxide (RGO), which exhibit remarkable electrochemical performance with higher capacitance and longer cycle life than the bare NiCo2S4 hollow spheres (HSs).

Aqueous Al-ion batteries (AAIBs) are the subject of great interest due to the inherent safety and high theoretical capacity of aluminum. The high abundancy and easy accessibility of aluminum raw materials further make AAIBs appealing for grid-scale energy storage. However, the passivating oxide film formation and hydrogen side reactions at the aluminum anode as well as limited availability of the cathode lead to low discharge voltage and poor cycling stability. Here, we proposed a new AAIB system consisting of an Al x MnO 2 cathode, a zinc substrate-supported Zn−Al alloy anode, and an Al(OTF) 3 aqueous electrolyte. Through the in situ electrochemical activation of MnO, the cathode was synthesized to incorporate a two-electron reaction, thus enabling its high theoretical capacity. The anode was realized by a simple deposition process of Al 3+ onto Zn foil substrate. The featured alloy interface layer can effectively alleviate the passivation and suppress the dendrite growth, ensuring ultralong-term stable aluminum stripping/ plating. The architected cell delivers a record-high discharge voltage plateau near 1.6 V and specific capacity of 460 mAh g −1 for over 80 cycles. This work provides new opportunities for the development of highperformance and low-cost AAIBs for practical applications.

Sodium-ion batteries (SIBs) are considered to be the most promising electrochemical energy storage devices for large-scale grid and electric vehicle applications due to the advantages of resource abundance and cost-effectiveness.