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Rechargeable aqueous metal-ion batteries made from non-flammable and low-cost materials offer promising opportunities in large-scale utility grid applications, yet low voltage and energy output, as well as limited cycle life remain critical drawbacks in their electrochemical operation. Here we develop a series of high-voltage aqueous metal-ion batteries based on ‘M + /N + -dual shuttles' to overcome these drawbacks. They utilize open-framework indium hexacyanoferrates as cathode materials, and TiP 2 O 7  and NaTi 2 (PO 4 ) 3  as anode materials, respectively. All of them possess strong rate capability as ultra-capacitors. Through multiple characterization techniques combined with  ab initio  calculations, water-mediated cation intercalation of indium hexacyanoferrate is unveiled. Water is supposed to be co-inserted with Li +  or Na + , which evidently raises the intercalation voltage and reduces diffusion kinetics. As for K + , water is not involved in the intercalation because of the channel space limitation.

Water-mediated cation intercalation of open-framework indium hexacyanoferrate with high voltage and fast kinetics