Journal
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 16, Issue 20, Pages 9580-9590Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c4cp00422a
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Funding
- Deutsche Forschungsgemeinschaft (DFG) [SPP 1415, 1277, WI3600/2-1, WI3600/4-1]
- Austrian Federal Ministry of Economy, Family and Youth
- Austrian National Foundation for Research, Technology and Development
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Chemical reactions induced by mechanical treatment may give access to new compounds whose properties are governed by chemical metastability, defects introduced and the size effects present. Their interplay may lead to nanocrystalline ceramics with enhanced transport properties being useful to act as solid electrolytes. Here, the introduction of large amounts of La into the cubic structure of BaF2 served as such an example. The ion transport properties in terms of dc-conductivity values of the F-anion conductor Ba1-xLaxF2+x (here with x = 0.4) considerably exceed those of pure, nanocrystalline BaF2. So far, there is only little knowledge about activation energies and jump rates of the elementary hopping processes. Here, we took advantage of both impedance spectroscopy and F-19 NMR relaxometry to get to the bottom of ion jump diffusion proceeding on short-range and long-range length scales in Ba0.6La0.4F2.4. While macroscopic transport is governed by an activation energy of 0.55 to 0.59 eV, the elementary steps of hopping seen by NMR are characterised by much smaller activation energies. Fortunately, we were able to deduce an F-self-diffusion coefficient by the application of spin-locking NMR relaxometry.
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