High-entropy solid electrolytes (HESEs) have emerged as a groundbreaking class of materials, leveraging the configurational entropy of multi-principal element systems to achieve unprecedented ionic conductivities. Recent studies have demonstrated HESEs with ionic conductivities exceeding 10^-2 S/cm at room temperature, rivaling liquid electrolytes. For instance, a Li7P2S8I-based HESE exhibited a conductivity of 12.3 mS/cm, attributed to the synergistic effects of multiple cations (e.g., Li, Na, K) and anions (e.g., S, O, Cl).
The structural diversity of HESEs enables the stabilization of metastable phases with low activation energies for ion migration. Computational studies reveal that the presence of five or more principal elements reduces energy barriers to ~0.2 eV, facilitating rapid Li+ diffusion. Experimental validation using neutron diffraction has confirmed these findings, showing disordered cation sublattices that enhance ionic mobility.
HESEs also exhibit exceptional electrochemical stability, withstanding voltages up to 5 V vs. Li/Li+. This stability is attributed to the formation of robust interphase layers that suppress dendrite growth and side reactions. For example, a (Li,Na,K)(S,O,Cl) HESE demonstrated a Coulombic efficiency of 99.8% over 500 cycles in a Li-metal battery configuration.
The scalability of HESEs is being explored through advanced manufacturing techniques such as spark plasma sintering (SPS) and aerosol deposition. SPS-processed HESEs have achieved densities >95% with minimal grain boundary resistance, while aerosol deposition enables the fabrication of thin films (<10 µm) suitable for solid-state batteries.
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