The aqueous geochemistry of REE. Part 8: Solubility of ytterbium oxalate and the stability of Yb(III)-oxalate complexes in water at 25 degrees C to 80 degrees C
Ch. Gammons et Sa. Wood, The aqueous geochemistry of REE. Part 8: Solubility of ytterbium oxalate and the stability of Yb(III)-oxalate complexes in water at 25 degrees C to 80 degrees C, CHEM GEOL, 166(1-2), 2000, pp. 103-124
The solubility of ytterbium oxalate (Yb(2)Ox(3) . xH(2)O) in aqueous soluti
on was measured as a function of temperature (40 degrees C, 60 degrees C an
d 80 degrees C), ionic strength (0.05, 0.1 and 0.2 m NaCl), and free oxalat
e concentration (10(-7) to 10(-2) molal). At high oxalate and/or NaCl conce
ntration, the simple Yb-oxalate salt transforms into a double salt with the
stoichiometry NaYb(Ox)(2) . yH(2)O. Our solubility data were used to obtai
n smoothed equilibrium constants (I = 0, P = SVP) for the solubility produc
ts of both solid phases, and for the stepwise and cumulative association co
mplexes of the aqueous Yb(III)-oxalate complexes, between 25 degrees C and
100 degrees C. Whereas the solubility of the simple Yb-oxalate salt changes
little in this temperature range, the Na-Yb oxalate salt becomes less stab
le and significantly more soluble with an increase in temperature. The ytte
rbium oxalate complexes are strong, and may predominate over inorganic Yb(I
II) complexes (e.g., carbonate, chloride, sulfate, and phosphate) at geolog
ically realistic Ligand concentrations. Our results are relevant to researc
hers interested in the transport of ytterbium and other rare earth elements
(REE) in near-surface waters and sedimentary basin fluids, and may also ha
ve engineering applications with regards to the precipitation of oxalate sa
lts as a means of removing actinides and radioactive REE from aqueous nucle
ar wastes. (C) 2000 Elsevier Science B.V. All rights reserved.