American Chemical Society
ja5b13409_si_005.txt (41.46 kB)

Interstitial Oxide Ion Distribution and Transport Mechanism in Aluminum-Doped Neodymium Silicate Apatite Electrolytes

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posted on 2016-03-25, 13:30 authored by Tao An, Tom Baikie, Alodia Orera, Ross O. Piltz, Martin Meven, Peter R. Slater, Jun Wei, María L. Sanjuán, T. J. White
Rare earth silicate apatites are one-dimensional channel structures that show potential as electrolytes for solid oxide fuel cells (SOFC) due to their high ionic conductivity at intermediate temperatures (500–700 °C). This advantageous property can be attributed to the presence of both interstitial oxygen and cation vacancies, that create diffusion paths which computational studies suggest are less tortuous and have lower activation energies for migration than in stoichiometric compounds. In this work, neutron diffraction of Nd(28+x)/3AlxSi6–xO26 (0 ≤ x ≤ 1.5) single crystals identified the locations of oxygen interstitials, and allowed the deduction of a dual-path conduction mechanism that is a natural extension of the single-path sinusoidal channel trajectory arrived at through computation. This discovery provides the most thorough understanding of the O2– transport mechanism along the channels to date, clarifies the mode of interchannel motion, and presents a complete picture of O2– percolation through apatite. Previously reported crystallographic and conductivity measurements are re-examined in the light of these new findings.