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Research Article | Open Access

Fast ion-conducting high-entropy garnet solid-state electrolytes with excellent air stability

Shaoxiong Hana,b, Ziqi Wanga,b, Yue Maa,b, Yang Miaoa, Xiaomin Wanga, Yong Wanga,b( ), Yongzhen Wanga,b( )
College of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, China
Shanxi Joint Laboratory of Coal based Solid Waste Resource Utilization and Green Ecological Development, Taiyuan 030024, China
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Abstract

The garnet-type electrolyte is one of the most promising solid-state electrolytes (SSEs) due to its high ionic conductivity (σ) and wide electrochemical window. However, such electrolyte generates lithium carbonate (Li2CO3) in air, leading to an increase in impedance, which greatly limits their practical applications. In turn, high-entropy ceramics (HECs) can improve phase stability due to high-entropy effect. Herein, high-entropy garnet (HEG) Li6.2La3(Zr0.2Hf0.2Ti0.2Nb0.2Ta0.2)2O12 (LL(ZrHfTiNbTa)O) SSEs were synthesized by the solid-state reaction method. X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), electrochemical impedance spectroscopy (EIS), and scanning electron microscopy (SEM) characterizations indicated that the LL(ZrHfTiNbTa)O electrolyte has excellent air stability. Room-temperature conductivity of LL(ZrHfTiNbTa)O can be maintained at ~1.42×10−4 S/cm after exposure to air for 2 months. Single-element-doped garnets were synthesized to explain the role of different elements and the mechanism of air stabilization. In addition, a lithium (Li)/LL(ZrHfTiNbTa)O/Li symmetric cell cycle is stable over 600 h, and the critical current density (CCD) is 1.24 mA/cm2, indicating remarkable stability of the Li/LL(ZrHfTiNbTa)O interface. Moreover, the LiFePO4/LL(ZrHfTiNbTa)O/Li cell shows excellent rate performance at 30 ℃. These results suggest that HECs can be one of the strategies for improving the performance of SSEs in the future due to their unique effects.

Keywords

solid-state batterieshigh-entropy ceramics (HECs)garnet electrolytesair stability

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Journal of Advanced Ceramics
Volume 12 Issue 6,
June 2023
Pages 1201-1213
DOI: 10.26599/JAC.2023.9220749
Cite this article:
Han S, Wang Z, Ma Y, et al. Fast ion-conducting high-entropy garnet solid-state electrolytes with excellent air stability. Journal of Advanced Ceramics, 2023, 12(6): 1201-1213. https://doi.org/10.26599/JAC.2023.9220749

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Received: 20 December 2022
Revised: 15 March 2023
Accepted: 01 April 2023
Published: 19 May 2023
© The Author(s) 2023.

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