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Abrupt Structural Transformation in Hydrotalcite-like Compounds Mg1-xAlx(OH)2(NO3)x·nH2O as a Continuous Function of Nitrate Anions
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Section:Abstract
We report here a systematic XRD/FTIR/CHN/ICP investigation for structural transformation of hydrotalcite-like compounds Mg1-xAlx(OH)2(NO3)x·nH2O as a continuous function of nitrate anions (x = 0.18−0.34). With seven finely divided steps in x value, a clear relationship between basal spacing and nitrate anion content (and thus trivalent cation content) has been found. In particular, we have been able to “arrest” an intermediate hydrotalcite-like phase that situates at the midpoint of an abrupt structural transformation. Unlike that of normal hydrotalcites, the relationship revealed in our nitrated Mg1-xAlx(OH)2(NO3)x·nH2O samples is much more complicated. While the lattice parameter a decreases with increase of nitrate content, the parameter c decreases slightly over x = 0.18−0.22, rises abruptly with a further increase of nitrate anions at x = 0.26, and then reaches maximums at x = 0.31−0.34. The compound at x = 0.26 also shows a sharp decrease in mean crystallite dimension. The abrupt structural change is attributed to a drastic change in nitrate anion arrangement. On the basis of our FTIR observations and Coulombic energy estimation, a “stick-lying” model for nitrate arrangement has been proposed, which is apparently superior to a “tilt-lying” model reported previously. The saturated charge density of the brucite-like layers for the “stick-lying” nitrate anions is about 4 e/nm2. The sharp decrease in crystallite dimension can be ascribed to the change of nitrate configuration from “flat-lying” to “stick-lying” due to increasing lateral repulsion among the anions and thus discontinuation in the planar growth.
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History
- Published In Issue March 08, 2001
- Received August 10, 2000
Revised December 8, 2000
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