期刊
JOURNAL OF PHYSICAL CHEMISTRY B
卷 104, 期 15, 页码 3481-3487出版社
AMER CHEMICAL SOC
DOI: 10.1021/jp000499j
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To understand the impact of particle size on phase stability and phase transformation during growth of nanocrystalline aggregates we conducted experiments using titania (TiO2) samples consisting of nanocrystalline anatase (46.7 wt %, 5.1 nm) and brookite (53.3 wt %, 8.1 nm). Reactions were studied isochronally at reaction times of 2 h in the temperature range 598-1023 K and isothermally at 723, 853, and 973 K by X-ray diffraction (XRD). A numerical deconvolution method was developed to separate overlapping XRD peaks, and an analytical method for determining phase contents of anatase, brookite, and rutile from XRD data was established. Results show that, in contrast to previous studies, anatase in our samples transforms to brookite and/or rutile before brookite transforms to rutile. Thermodynamic and kinetic analyses further support this conclusion. For general titania samples, the transformation sequence among anatase and brookite depends on the initial particle sizes of anatase and brookite, since particle sizes determine the thermodynamic phase stability at ultrafine sizes. These results highlight extremely important size-dependent behavior that may be expected in other nanocrystalline systems where multiple polymorphs are possible.
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