Publication date: 10th April 2024
Solid-state batteries (SSBs) are a potentially safe, next-generation energy-storage technology [1-2]. For SSBs to be commercially viable, the development of solid electrolytes (SEs) with high ionic conductivity, high (electro)chemical stability, and good processability is imperative [2]. A novel approach to modifying materials, potentially leading to improved properties, is the high-entropy concept, characterized by a ΔSconf > 1.5R (where ΔSconf and R represent configurational entropy and ideal gas constant, respectively) [3]. However, the effect of configurational entropy on lithium transport remains largely elusive.
Recently, our group has extended the choice of high-entropy SEs to include lithium argyrodites by multianionic and/or -cationic substitution [4-6]. For multicationic substituted litihum argyrodites with the composition Li6.5[Ge0.25Si0.25Sb0.25P0.25]S5I, high ionic conductivity (> 10 mS/cm at 25 °C) and a low activation energy for conduction (0.20 eV) were observed, as shown by 7Li pulsed field gradient (PFG) nuclear magnetic resonance (NMR) spectroscopy and electrochemical impedance spectroscopy (EIS) [5-6]. These results were rationalized from a structural perspective via neutron powder diffraction combined with magic angle spinning (MAS) NMR spectroscopy. In this case, high S2‒/I‒ site disorder (up to ~11%) and lithium re-distribution led to shortened Li-Li jump distances, facilitating long-range ion diffusion [5-6]. Subsequently, we have explored a series of multicationic substituted lithium argyrodites by tuning the cationic stoichiometry. Through complementary EIS and 7Li PFG NMR measurements, we found that compositionally complex substitution helps to significantly improve Li-ion mobility. Notably, our study provides clear evidence for the correlation between configurational entropy and ion mobility and indicates the potential for enhancing conductivity in ceramic ion conductors by tailoring the compositional complexity, opening up new avenues for research and development in this field.
J.L. acknowledges the Fonds der Chemischen Industrie (FCI) for financial support. F.S. is grateful to the Federal Ministry of Education and Research (BMBF) for funding within the project MELLi (03XP0447). This work was partially supported by BASF SE. The authors thank Institut Laue-Langevin (ILL) for beamtime allocation under proposal number 5-21-1164.
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