Publication date: 10th April 2024
Na-ion battery (NIB) research is blooming at a rapid scale with the main purpose of reducing our extensive dependence on Li-ion batteries to fulfill the ever-increasing energy demands. While the Na-ion battery is effectively used for stationary applications, only the development of new high power and energy density cathode materials will increase the horizon of their utility. Layered transition-metal oxides (TMOs) are the state-of-the-art Na-ion battery cathode frameworks. However, the structural instability of TMOs at their fully desodiated state and detrimental phase transitions have directed the research towards polyanionic cathode frameworks, which exhibit better structural stability with Na-exchange and high voltages. Some of the most explored polyanionic frameworks, such as the sodium superionic conductors (NaSICONs), alluaudites, olivines, and pyro/fluoro-phosphates display a wide variety of electrochemical performances, with low capacity being a common drawback. In this context, oxyfluorides are a largely unexplored class of polyanionic cathode materials, that can exhibit a high capacity and voltage, theoretically, with the voltage enhancement arising from the inductive effect of the fluoride ions. Here, I will present a systematic computational exploration of the transition-metal-based oxyfluoride chemical space, including finding the groundstate polymorph, evaluating the average Na-intercalation voltage, estimating the 0 K thermodynamic stability and quantifying the mobility of Na-ion mobility within the framework. Our work identifies a few promising compositions for subsequent experimental validation and paves the way for constructing NIBs with enhanced energy densities.
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