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

Shaoxiong Han; Ziqi Wang; Yue Ma; Yang Miao; Xiaomin Wang; Yong Wang; Yongzhen Wang

doi:10.26599/JAC.2023.9220749

Journal of Advanced Ceramics 2023, 12(6): 1201-1213 https://doi.org/10.26599/JAC.2023.9220749

Research Article |

Open Access | Issue | Published: 19 May 2023

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

Show Author's Information Hide Author's Information Shaoxiong Han^{^a^,^b}, Ziqi Wang^{^a^,^b}, Yue Ma^{^a^,^b}, Yang Miao^{^a}, Xiaomin Wang^{^a}, Yong Wang^{^a^,^b}(

), Yongzhen Wang^{^a^,^b}(

)

aCollege of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, China

bShanxi Joint Laboratory of Coal based Solid Waste Resource Utilization and Green Ecological Development, Taiyuan 030024, China

Keywords:

high-entropy ceramics (HECs), air stability, solid-state batteries, garnet electrolytes

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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Abstract Full text Electronic supplementary material About this article

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) Li_6.2La₃(Zr_0.2Hf_0.2Ti_0.2Nb_0.2Ta_0.2)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.

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About this article

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

Show Author's information Hide Author's Information Shaoxiong Han^{^a^,^b}, Ziqi Wang^{^a^,^b}, Yue Ma^{^a^,^b}, Yang Miao^{^a}, Xiaomin Wang^{^a}, Yong Wang^{^a^,^b}(

), Yongzhen Wang^{^a^,^b}(

)

aCollege of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, China

bShanxi Joint Laboratory of Coal based Solid Waste Resource Utilization and Green Ecological Development, Taiyuan 030024, China

Abstract

Keywords: high-entropy ceramics (HECs), air stability, solid-state batteries, garnet electrolytes

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Publication history

Received: 20 December 2022

Revised: 15 March 2023

Accepted: 01 April 2023

Published: 19 May 2023

Issue date: June 2023

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Acknowledgements

This work was funded by the Central Government Guides Local Science and Technology Development Special Fund Projects (Grant No. YDZJSX2022B003), the Shanxi Province Science and Technology Major Projects (Grant No. 202101120401008), the Key Research and Development Project of Shanxi Province (Grant No. 202102030201006), and Science and Technology Activities of Overseas Students Merit-based Funding Projects of Shanxi Province (Grant No. 2021037).

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