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1 Department of Geology, St. Francis Xavier University, Antigonish, Nova Scotia, B2G 2W5, Canada
2 Department of Physics and Astronomy, Southwest Missouri State University, Springfield, Missouri 65804, U.S.A.
3 Department of Geological Sciences, Cornell University, Ithaca, New York 14853, U.S.A.
4 MS 954, U.S. Geological Survey, Reston, Virginia 20192, U.S.A.
Correspondence: * E-mail: aanderso{at}stfx.ca
The first direct measurements are reported for the structure of the hydrated La3+ ion in an aqueous solution (containing 0.007 m La) over a range of temperatures from 25 to 300 °C and pressures up to 1600 bars. The radial distribution of atoms around the La3+ ion was measured using the X-ray absorption fine structure (XAFS) technique. La L3-edge spectra were collected in the fluorescence mode from nitrate solutions in a modified hydrothermal diamond anvil cell using the PNC-CAT X-ray microprobe at the Advanced Photon Source, Argonne National Laboratory. Analysis of the XAFS spectra collected at all temperatures indicates that each La3+ ion has a hydration number of nine and that the solvating waters surround the ion in a tricapped trigonal prismatic arrangement. As temperature is increased from 25 to 300 °C, the bond distance between the equatorial-plane O atoms and the La3+ ion increases from 2.59 ± 0.02 to 2.79 ± 0.04 Å, whereas the bond distance between La3+ and the O atoms at the ends of the prism decrease to 2.48 ± 0.03 Å. This study also demonstrates the unique capability of the modified hydrothermal diamond anvil cell for in situ low energy X-ray spectroscopic analysis of elements in dilute aqueous solutions at elevated temperatures and pressures.
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