Publication date: 10th April 2024
Ceramic proton conductors are attracting more and more attention as they can be used in various applications like fuel cells or electrolysers. However, in most materials the proton conduction process requires high temperature (> 400 °C). Li6La3ZrTaO12 (LLZTO) is known for its rapid Li+ diffusivity as has been directly revealed by 7Li NMR measurements [1]. By exchanging parts of the highly mobile Li+ ions by protons through treatment of a single crystal in water or glacial acetic acid we obtained a mixed proton-lithium mixed ionic conductor [2]. Here, H+ proton diffusivity and Li+ diffusivity have separately been studied with element specific 1H and 7Li NMR spectroscopy. While long-range 7Li diffusion is noticeably slowed in Li-H exchanged LLZTO, we directly observe rather high H+ diffusivity, which is, however, significantly slower than Li+ dynamics. With the help of spin-lattice relaxation measurements we were able to measure local (and long-range) energy barriers (0.20(1) eV vs 0.45(3) eV) as well as the self-diffusion coefficient DH of H+ dynamics (1.2 × 10−15 m2 s−1 at 125 °C). We compare these results with those obtained for a nanocrystalline LLZTO sample studied recently. The encouraging results are assumed to open new directories in designing ceramics offering fast transport pathways for protons at low temperature.
We thank the DFG for financial support (WI3600).
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