5 years ago

Influence of Yttrium Concentration on Local Structure in BaZr1–xYxO3−δ Based Proton Conductors

Influence of Yttrium Concentration on Local Structure in BaZr1–xYxO3−δ Based Proton Conductors
Michael J. Gatari, Caroline W. Mburu, Maths Karlsson, Samuel M. Gaita, Christopher S. Knee
The evolution of local structure, coordination of protons, and proton conductivity in yttrium-doped barium zirconate, BaZr1–xYxO3−δ (x = 0–0.5), has been investigated using thermal-gravimetric analysis, impedance spectroscopy, and infrared spectroscopy. Low-frequency (50–1000 cm–1) infrared absorbance spectra provide evidence of increasing local structural distortions as a function of yttrium concentration as well as subtle differences, mainly linked to the oxygen sublattice, between the dry and hydrated samples. High-frequency (1700–4500 cm–1) spectra of the hydrated samples, distinguished by a broad O–H stretch continuum, manifest a varying degree of hydrogen bond interactions between the protons and nearest neighbor oxygens due to the disordered crystal structure with a general weakening in particular of the strongest hydrogen bonding interactions with increasing dopant levels. It is argued that compositions within the range 0.15 ⩽ x ⩽ 0.3 possess a favorable level of local structural distortions to facilitate high proton conductivity, and this, coupled with a significant proton concentration, may be a factor in explaining the high proton conductivity these phases display.

Publisher URL: http://dx.doi.org/10.1021/acs.jpcc.7b05023

DOI: 10.1021/acs.jpcc.7b05023

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