Yttrium Contenting Compositionally Complex Medium-Entropy Li-Garnet Electrolyte with Improved Ionic Conductivity

Li, Chang; Giri, Nava Raj; Chen, Yan; Soto, Fernando A; Fu, Zhezhen

doi:10.1021/acsami.5c10130

Yttrium Contenting Compositionally Complex Medium-Entropy Li-Garnet Electrolyte with Improved Ionic Conductivity

Journal Article · Mon Aug 18 04:00:00 EDT 2025 · ACS Applied Materials & Interfaces

DOI:https://doi.org/10.1021/acsami.5c10130· OSTI ID:2586835

Li, Chang ^[1]; Giri, Nava Raj ^[1]; ^[2]; Soto, Fernando A ^[1]; ^[1]

Pennsylvania State Univ., University Park, PA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

The compositionally complex medium/high-entropy design concept can greatly expand the categories and affect the properties of the materials. With such a designing concept, a medium-entropy Li-garnet electrolyte with appropriate yttrium content (formula Li_6.6La₃ZrNb_0.3Ta_0.3Hf_0.3Y_0.1O₁₂) shows a record-high ionic conductivity of ∼5.7 × 10^–4 S/cm, the highest reported for any single-site substituted high/medium-entropy Li-garnet. The assembled Li metal symmetric cells also show stable long-term cycling (0.1 mA/cm² for over 200 h). Neutron powder diffraction and Rietveld refinement results indicate that a competing conduction mechanism between (1) occupancy on high mobility of 96h sites and (2) the associated site vacancies and the bond length requires an appropriate content of Y for enhanced ionic conductivity. Li-ion hopping through the bottleneck can also contribute to the conductivity. Finally, density functional theory and Born–Oppenheimer molecular dynamics simulations also indicate the high mobility and number of hopping transitions of Li ions, contributing to the high ionic conductivity.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Science Foundation (NSF)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2586835

Journal Information:: ACS Applied Materials & Interfaces, Journal Name: ACS Applied Materials & Interfaces Journal Issue: 34 Vol. 17; ISSN 1944-8244; ISSN 1944-8252

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Yttrium Contenting Compositionally Complex Medium-Entropy Li-Garnet Electrolyte with Improved Ionic Conductivity

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