Publication date: 10th April 2024
Over the last decade, solid-state batteries (SSBs) showed great promise as future power storages, which provide high energy densities, while overcoming the safety issues of conventional Li-ion batteries with liquid electrolytes. [1] Alternative systems using other charge carrying ions like Na+ and K+ are also being investigated, owing to their higher elemental abundance and lower production cost than lithium-based materials. Key advantages of K+ over Na+ is the possibility to use graphite as anode material as well as a higher achievable cell voltage. [2] However, K+-conducting solid electrolytes (SEs) for SSBs are still in early development. [3,4] One promising K-based ionic conductor is W-substituted K3SbS4, which was already used as solid electrolyte within K-ion hybrid cells. [3] The W-substituted Na analogue is also amongst the fastest ion conductors reported for Na-ion SEs, making this material a promising prospect to study. [5]
Herein we investigate the impact of W-substitution on the crystal structure and ion transport of K3SbS4. Raman spectroscopy confirms the successful substitution of Sb with W. The orthorhombic phase of K3SbS4 [3,6] transitions into a monoclinic phase upon introduction of W. Utilizing synchrotron X-ray diffraction, we observe the coexistence of both phases in all W-doped samples up to 6% W content at room temperature. The introduction of W also creates K+ vacancies in the structure. Both cause a strongly enhanced ionic conductivity, while significantly decreasing the activation energy of K+-transport within the bulk material.
Due to its remarkable ionic conductivity W-substituted K3SbS4 is promising for the integration into K-ion SSBs, thereby expanding the yet insufficiently investigated field of K-ion SSBs and evaluating its feasibility as an alternative system to Li-based systems.
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