In operando resonance Raman spectroscopy suggests quantitative correlation between phonon band properties and the amount of charge storage of high-energy density NiO2H x battery/pseudocapacitive material. Comparing the spectroscopic evolution using different electrolytes reveals the contributions of breaking/formation of O-H bonds and insertion/extraction of cations to electrochemical charge storage of NiO2H x .
Keywords: battery; nickel hydroxide/oxo‐hydroxide; reaction mechanisms; resonance Raman spectroscopy; supercapacitor.