Publication date: 10th April 2024
The high demand for lithium-ion batteries and for potentially improved alternatives is fuelling significant research in both academia and industry. Sodium-based solid-state batteries (SSBs) are promising candidates, offering reduced cost (when selecting, other than Na, abundant raw materials), and improved safety.
The key component of sodium SSBs is the sodium ion conductor. Metal halides have emerged as materials combining excellent mechanical processibility and compatibility with the electrodes. [1,2]
However, the low ionic conductivity problem remains unsolved (10-6~10-5 S/cm). [2]Work on the subject has proliferated over the recent years. The targeted introduction of vacancies, for example via aliovalent substitution, is widely employed to directly influence the ionic conductivity of the ion conductor. [3–6]
In this work, we synthesized and studied the influence of Zn2+ substitution in NaAlCl4 (Na1+xZnxAl1-xCl4 formula unit). [1] So far, no investigation on the doping of NaAlCl4 has been reported. Since the second end member Na2ZnCl4 belongs to a different structural type as compared to NaAlCl4, a solid solution is not guaranteed. In fact, we find phase separation does occur to some extent. Hence, we are also at the same time investigating the introduction of Al (and Na vacancies) in Na2ZnCl4. A whole series of samples has been synthesized by mechanochemical methods. The stability of a 2-phase system with enhanced ionic conductivity will be discussed based on DFT calculations and on the experimental results (XRD, ND).
Furthermore, the system is investigated by EIS and variable temperature NMR to clarify the Na conductivity and the origin of its improvement.
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