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X-Ray Absorption Spectroscopy of Strontium(II) Coordination: II. Sorption and Precipitation at Kaolinite, Amorphous Silica, and Goethite Surfaces

✍ Scribed by Nita Sahai; Susan A. Carroll; Sarah Roberts; Peggy A. O'Day


Book ID
102581281
Publisher
Elsevier Science
Year
2000
Tongue
English
Weight
243 KB
Volume
222
Category
Article
ISSN
0021-9797

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✦ Synopsis


Sorption of dissolved strontium on kaolinite, amorphous silica, and goethite was studied as a function of pH, aqueous strontium concentration, the presence or absence of atmospheric CO 2 or dissolved phosphate, and aging over a 57-day period. Selected sorption samples ([Sr(aq)] i β‰ˆ 0.5-1 Γ— 10 -3 m) were examined with synchrotron X-ray absorption spectroscopy (XAS) at low (13-23 K) and room temperatures to determine the local molecular coordination around strontium. Quantitative analyses of the extended X-ray absorption fine structure (EXAFS) of kaolinite, amorphous silica, and most goethite sorption samples showed a single first shell of 9-10 (Β±1) oxygen atoms around strontium at an average Sr-O bonddistance of 2.61 (Β±0.02) Γ…, indicating hydrated surface complexes. The EXAFS spectra were unchanged after reaction for up to 57 days. Likewise, in kaolinite sorption samples prepared in 100% nitrogen atmosphere, the presence of dissolved phosphate (0.5 Γ— 10 -3 m) in addition to strontium did not change the local coordination around strontium. In two goethite sorption samples reacted in air at pH ∼8.5, the EXAFS spectra (collected at low and room temperature) clearly showed that the local structure around strontium is that of strontianite (SrCO 3 (s)). We also noted an increase in strontium uptake on goethite in the presence of atmospheric CO 2 in batch experiments, relative to CO 2 -free experiments. These observations suggest that sorption of carbonate may nucleate the precipitation of SrCO 3 in the pH range in which carbonate sorption on goethite is near a maximum. At higher pH, carbonate surface sorption decreases as dissolved CO 2 decreases. For goethite sorption samples above pH 8.6, hydrated surface complexes, rather than a precipitate, were observed in the EXAFS spectra.


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