Journal Article

PUBDB-2025-02267

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Enhanced Ionic Conductivity and Electrochemical Properties of Li$_2$B$_{12}$H$_{12}$/ZrO$_2$ Nanocomposites for All-Solid-State Lithium Metal Batteries

Hehn, J.Extern* ; Rodenburg, H. P. ; Lazemi, M.Extern*XFEL.EU* ; Verschoor, J.Extern* ; Perich, M. P. ; Sundermann, M.Extern* ; Gretarsson, H.DESY* ; van der Hoeven, J. E. S. ; de Groot, F.Extern* ; de Jongh, P.Extern* ; Ngene, P. (Corresponding author)Extern*

2025
Soc. Washington, DC

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Please use a persistent id in citations: doi:10.1021/acsami.5c01939  doi:10.3204/PUBDB-2025-02267

Abstract: Solid-state electrolytes play a key role in the development of safe and high-capacity all-solid-state batteries. Complex hydrides such as Li$_2$B$_{12}$H$_{12}$ are attractive as solid electrolytes due to their low weight and good electrochemical stability, but suffer from low conductivities at room temperature. Herein, we report a three-order-magnitude increase in the ionic conductivity of Li$_2$B$_{12}$H$_{12}$ upon nanocomposite formation with ZrO$_2$ via mechanochemical treatment, reaching 2.9 × 10$^{–4}$ S cm$^{–1}$ at 30 °C. Results from infrared spectroscopy, X-ray Raman scattering and electron microscopy coupled with electron energy loss spectroscopy suggest that the increased ionic conductivity is due to strong interfacial interaction/reaction between Li$_2$B$_{12}$H$_{12}$ and ZrO$_2$. This leads to a highly defective interphase region where the Li, B, Zr, and O chemical environments are distinctively different from the bulk Li$_2$B$_{12}$H$_{12}$ and ZrO$_2$. The improved ionic conductivity of the nanocomposite compared to the pristine material enabled the realization of all-solid-state batteries with a Li metal anode and both TiS$_2$ and LiFePO$_4$ cathodes. We demonstrate the suitability of the nanocomposite at various charging rates up to C/2 (0.34 mA cm$^{–2}$) for over 170 cycles at 40–60 °C (Li|Li$_2$B$_{12}$H$_{12}$/ZrO2|TiS$_2$).

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Contributing Institute(s):

1. DOOR-User (DOOR ; HAS-User)
2. PETRA-S (FS-PETRA-S)

Research Program(s):

1. 632 - Materials – Quantum, Complex and Functional Materials (POF4-632) (POF4-632)
2. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)
3. SMART-X - Study of carrier transport in MAterials by time-Resolved specTroscopy with ultrashort soft X-ray light (860553) (860553)

Experiment(s):

1. PETRA Beamline P01 (PETRA III)

Appears in the scientific report 2025

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Database coverage:
; ; ; Clarivate Analytics Master Journal List ; Current Contents - Engineering, Computing and Technology ; Current Contents - Physical, Chemical and Earth Sciences ; Essential Science Indicators ; IF >= 5 ; JCR ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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