期刊
CHEMISTRY OF MATERIALS
卷 19, 期 23, 页码 5742-5747出版社
AMER CHEMICAL SOC
DOI: 10.1021/cm0715388
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The local structure and dynamics of oxide ions in yttria-doped ceria (YDC, 5 to 30% Y2O3) were studied using high-resolution Y-89 and O-17 MAS NMR spectroscopy at ambient temperature and high temperatures to 500 degrees C. Eight-, seven-, and six-coordinated yttriurn cations are clearly resolved in 89Y MAS NMR spectra, and their relative populations were measured. The derived average coordination number of yttrium is smaller than that for a random distribution of oxygen vacancies, suggesting that there is strong association between yttrium cations and vacancies and there is the possibility of pairing of two yttrium cations with one vacancy. In the 170 MAS NMR spectra, resonances for oxygens with different coordination environments are resolved and are assigned to oxygens with different numbers of yttrium cations in the first coordination sphere. The relative intensities of the 110 resonances also deviate from those expected from a random distribution, again indicating possible pairing of yttrium cations. High-temperature 110 MAS NNIR shows coalescence among various peaks. The exchange between oxygen sites with yttrium neighbors appears to occur at a lower temperature (about 100 degrees C than the exchange that involves the sites without yttrium neighbors; rapid exchange of all oxide anions throughout the structure occurs above 400 T.
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