Publication date: 10th April 2024
Conventional cathode materials of sodium-ion batteries (SIBs) are pre-sodiated and store Na-ions electrochemically. Interestingly, pre-potassiated materials can be appealing cathodes for SIBs. Potassium Prussian blue analogues (K-PBAs) is an excellent example. K-PBAs are cost effective and sustainable materials that are based on earth-abundant elements, and they have the structural remits to allow fast migration of large-sized ions. I will show in this talk that in a hybrid SIB cell, where Na+ is in the electrolyte and K+ is in the K-PBA cathode, not only is the electrochemical mechanism of cation intercalation in K-PBA dominated by K-ion rather than Na-ion, but the mechanism can be affected by the [Fe(CN)6]4- anion vacancies present in K-PBA. K-PBA with 25% anion vacancies exhibits two cation intercalation steps in a hybrid SIB cell, both being dominated by K-ion and displaying a ~0.2 V voltage increase compared with Na-PBA. In contrast, K-PBA with 7% anion vacancies exhibits both K-ion intercalation (>2.8 V vs. Na+/Na) and Na-ion intercalation (<2.8 V). This is because a higher vacancy level enhances K-ion diffusion in the PBA framework, which facilitates K-ion intercalation and suppresses Na-ion intercalation. A lower vacancy level deteriorates K-ion diffusion and thus enhances Na-ion intercalation. In a full-cell that is consisted of the K-PBA cathode and the hard carbon anode, the electrochemical process proceeds in a similar manner as the half-cells. K-ion dominates the intercalation in the K-PBA cathode while Na-ion dominates the intercalation in the hard carbon anode; therefore, a hybrid SIB is formed.
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