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Secondary batteries are important energy storage devices for a mobileequipment, an electric car, and a large-scale energy storage. Nevertheless,variation of the local electronic state of the battery materials in the charge(or oxidization) process are still unclear. Here, we investigated the localelectronic state of cobalt-hexacyanoferrate (Na$_x$Co[Fe(CN)$_6$]$_{0.9}$), bymeans of resonant inelastic X-ray scattering (RIXS) with high energy resolution(~100 meV). The L-edge RIXS is one of the most powerful spectroscopic techniquewith element- and valence-selectivity. We found that the local electronic statearound Co$^{2+}$ in the partially-chargedNa$_{1.1}$Co$^{2+}$$_{0.5}$Co$^{3+}$$_{0.5}$[Fe$^{2+}$(CN)$_6$]$_{0.9}$ film (x= 1.1) is the same as that of the dischargedNa$_{1.6}$Co$^{2+}$[Fe$^{2+}$(CN)$_6$]$_{0.9}$ film (x = 1.6) within the energyresolution, indicating that the local electronic state around Co$^{2+}$ isinvariant against the partial oxidization. In addition, the local electronicstate around the oxidized Co$^{3+}$ is essentially the same as that of thefully-charged filmCo$^{3+}$[Fe$^{2+}$(CN)$_6$]$_{0.3}$[Fe$^{3+}$(CN)$_6$]$_{0.6}$ (x = 0.0) film.Such a strong localization of the oxidized Co$^{3+}$ state is advantageous forthe reversibility of the redox process, since the localization reduces extrareaction within the materials and resultant deterioration.

Strong localization of oxidized Co3+ state in cobalt-hexacyanoferrate