TY  - JOUR
AU  - Hehn, Jonas
AU  - Rodenburg, Hendrik P.
AU  - Lazemi, Masoud
AU  - Verschoor, Juliette
AU  - Perich, Marta Perxés
AU  - Sundermann, Martin
AU  - Gretarsson, Hlynur
AU  - van der Hoeven, Jessi E. S.
AU  - de Groot, Frank
AU  - de Jongh, Petra
AU  - Ngene, Peter
TI  - Enhanced Ionic Conductivity and Electrochemical Properties of Li<sub>2</sub>B<sub>12</sub>H<sub>12</sub>/ZrO<sub>2</sub> Nanocomposites for All-Solid-State Lithium Metal Batteries
JO  - ACS applied materials & interfaces
VL  - 17
IS  - 23
SN  - 1944-8244
CY  - Washington, DC
PB  - Soc.
M1  - PUBDB-2025-02267
SP  - 33824 – 33833
PY  - 2025
AB  - Solid-state electrolytes play a key role in the development of safe and high-capacity all-solid-state batteries. Complex hydrides such as Li<sub>2</sub>B<sub>12</sub>H<sub>12</sub> 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<sub>2</sub>B<sub>12</sub>H<sub>12</sub> upon nanocomposite formation with ZrO<sub>2</sub> via mechanochemical treatment, reaching 2.9 × 10<sup>–4</sup> S cm<sup>–1</sup> 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<sub>2</sub>B<sub>12</sub>H<sub>12</sub> and ZrO<sub>2</sub>. This leads to a highly defective interphase region where the Li, B, Zr, and O chemical environments are distinctively different from the bulk Li<sub>2</sub>B<sub>12</sub>H<sub>12</sub> and ZrO<sub>2</sub>. 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<sub>2</sub> and LiFePO<sub>4</sub> cathodes. We demonstrate the suitability of the nanocomposite at various charging rates up to C/2 (0.34 mA cm<sup>–2</sup>) for over 170 cycles at 40–60 °C (Li - Li<sub>2</sub>B<sub>12</sub>H<sub>12</sub>/ZrO2 - TiS<sub>2</sub>).
LB  - PUB:(DE-HGF)16
DO  - DOI:10.1021/acsami.5c01939
UR  - https://bib-pubdb1.desy.de/record/632939
ER  -