AUTHOR=Ye Ruijie , Ting Yin-Ying , Dashjav Enkhtsetseg , Ma Qianli , Taminato Sou , Mori Daisuke , Imanishi Nobuyuki , Kowalski Piotr M. , Eikerling Michael H. , Kaghazchi Payam , Finsterbusch Martin , Guillon Olivier 

TITLE=Preparation and electrochemical properties of Li6La3Zr0.7Ti0.3Ta0.5Sb0.5O12 high-entropy Li-garnet solid electrolyte

JOURNAL=Frontiers in Energy Research

VOLUME=12

YEAR=2024

URL=https://www.frontiersin.org/journals/energy-research/articles/10.3389/fenrg.2024.1379576

DOI=10.3389/fenrg.2024.1379576

ISSN=2296-598X

ABSTRACT=<p>Garnet-type solid electrolytes stand out as promising Li-ion conductors for the next-generation batteries. It has been demonstrated that the inherent properties of garnets can be tailored by introducing various dopants into their crystal structures. Recently, there has been a growing interest in the concept of high entropy stabilization for materials design. In this study, we synthesized high-entropy garnets denoted as Li<sub>6</sub>La<sub>3</sub>Zr<sub>0.7</sub>Ti<sub>0.3</sub>Ta<sub>0.5</sub>Sb<sub>0.5</sub>O<sub>12</sub> (LLZTTSO), wherein Ti, Sb, and Ta occupy the Zr site. The formation of the cubic garnet phase in LLZTTSO was confirmed through X-ray diffraction (XRD), and the resulting lattice parameter agreed with predictions made using computational methods. Despite the substantial porosity (relative density 80.6%) attributed to the low sintering temperature, LLZTTSO exhibits a bulk ionic conductivity of 0.099 mS cm<sup>−1</sup> at 25°C, and a total ionic conductivity of 0.088 mS cm<sup>−1</sup>, accompanied by an activation energy of 0.497 eV. Furthermore, LLZTTSO demonstrates a critical current density of 0.275 mA cm<sup>−2</sup> at 25°C, showcasing its potential even without any interfacial modification.</p>