Optimal water concentration for aqueous Li+ intercalation in vanadyl phosphate

Development of high-performance aqueous batteries is an important goal for energy sustainability owing to their environmental benignity and low fabrication costs. Although a layered vanadyl phosphate is one of the most-studied host materials for intercalation electrodes with organic electrolytes, little attention has been paid to its use in aqueous Li⁺ systems because of its excessive dissolution in water. Herein, by controlling the water concentration, we demonstrate the stable operation of a layered vanadyl phosphate electrode in an aqueous Li⁺ electrolyte. The combination of experimental analyses and density functional theory calculations reveals that reversible (de)lithiation occurs between dehydrated phases, which can only exist in an optimal water concentration.

We demonstrate aqueous Li⁺ intercalation chemistry of vanadyl phosphate in the form of monohydrates, which are only stable in an optimal water-concentration environment.