journal article·2025-07Open access

Influence of In‐Doping on the Structure and Electrochemical Performance of Compositionally Complex Garnet‐Type Solid Electrolytes

Alaa Alsawaf, Guruprakash Karkera, Thomas Diemant, Monaha Veerraju Kante, Yannik Schneider, Leonardo Velasco, Subramshu S. Bhattacharya, Florian Stainer, Martin Wilkening, Oliver Clemens, Jürgen Janek, Horst Hahn, Miriam Botros

Small Structures· Volume 6· Issue 7

Abstract

The electrochemical instability of electrode active materials as well as the flammability of the organic liquid electrolytes in Li‐ion batteries pose challenges for their safety and long cycle life. Solid electrolytes (SEs) that exhibit high ionic conductivity and a wide electrochemical stability window alleviate these challenges. Garnet‐type Li7La3Zr2O12 is a promising SE for next‐generation all‐solid‐state batteries. Herein, samples are prepared via a modified solid‐state reaction of compositionally complex Li6.3+zLa3Zr1.1−z Nb0.8Gd0.1InzO12 under different sintering atmospheres. X–ray diffraction patterns and Raman spectra prove the formation of a cubic garnet structure. Significant morphological changes are detected upon In‐doping and correlated to the ionic conductivity. The total Li‐ion conductivity of the dense pellets reaches 1 mS cm−1, among the highest reported to date, with an activation energy of 0.38 eV for the macroscopic ion transport obtained by impedance spectroscopy and as low as 0.24 eV for local Li‐ion hopping processes determined by 7Li nuclear magnetic resonance spin‐lattice relaxation measurements. The electronic contribution to the conductivity is negligible (10−10 S cm−1) making this compositionally complex SE a suitable candidate for all‐solid‐state battery applications.
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Research context

OpenAlex topics: Solid-state spectroscopy and crystallography · Perovskite Materials and Applications · Advanced Battery Materials and Technologies

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Institute of Nanotechnology Karlsruhe Institute of Technology (KIT) Hermann‐von‐Helmholtz Platz 1 76344 Eggenstein‐ Leopoldshafen Germany

Helmholtz Institute UIm (HIU) Electrochemical Energy Storage Helmholtz Straße 11 89081 UIm Germany

Institute for Physical Chemistry & Center for Materials Research Justus Liebig University Giessen Heinrich Buff Ring 17 35392 Giessen Germany

Universidad Nacional de Colombia sede de La Paz Km 9 via Valledupar‐La Paz La Paz, Cesar 202010 Colombia

Department of Metallurgical and Materials Engineering Indian Institute of Technology Madras Chennai 600036 India

Institute for Chemistry and Technology of Materials Graz University of Technology Stremayrgasse 9 8010 Graz Austria

Institute for Materials Science, Materials Synthesis Group University of Stuttgart Heisenbergstraße 3 70569 Stuttgart Germany

School of Sustainable Chemical, Biological and Materials Engineering The University of Oklahoma Norman OK 73019 USA

Funding

Deutsche Forschungsgemeinschaft · Universidad Nacional de Colombia

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