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Title:Solubility and speciation of plutonium(VI) with orthophosphate
Author(s):Weger, Hans Thomas
Doctoral Committee Chair(s):Landsberger, Sheldon
Department / Program:Nuclear, Plasma, and Radiological Engineering
Discipline:Nuclear, Plasma, and Radiological Engineering
Degree Granting Institution:University of Illinois at Urbana-Champaign
Subject(s):Engineering, Nuclear
Abstract:Pu(VI) speciation and solubility with phosphate was examined at pH from 0.3 to 12.2, Pu(VI) concentrations from 5 $\times\ {\rm 10}\sp{-5}$ M to 1.3 $\times\ {\rm 10}\sp{-3}$ M and phosphate concentrations up to 0.6 M. Absorption spectroscopy, solubility experiments, scanning electron microscopy and photon correlation spectroscopy were utilized.
The species PuO$\sb2{\rm H}\sb2{\rm PO}\sb4\sp{+}$ and PuO$\sb2{\rm (H}\sb2{\rm PO}\sb4{\rm )}\sb2$ formed at pH $$ 2.4. The aqueous plutonium concentration was 10$\sp{-5}$ M at pH from 3.5 to 6 and 10$\sp{-6}$ M at pH from 6 to 8. Plutonium(VI) favored complexation with phosphate only at Pu(VI) concentrations greater than 1.5 $\times\ {\rm 10}\sp{-4}$ M. Evidence exists that mixed phosphate-carbonate species were formed.
The species (PuO$\sb2{\rm HPO}\sb4$)$\sb{\rm n}$ and (PuO$\sb2{\rm NaPO}\sb4$)$\sb{\rm n},$ characterized by absorption bands at 842.3 $\pm$ 0.05 nm and 846 $\pm$ 0.05 nm, are formed at pH between 2.4 and 9. The species (PuO$\sb2{\rm HPO}\sb4$)$\sb{\rm n}$ has $\varepsilon$ = 340 $\pm$ 20, log $\beta$ = $-$4.32 + 10.73n $\pm$ ($-$0.20 + 0.41n) and log $\beta\sp{T}$ = log $\beta$ + 1.2n $\pm$ ($-$0.10 + 0.41n). The species (PuO$\sb2{\rm NaPO}\sb4{\rm )}\sb{\rm n}$ has $\varepsilon$ = 380 $\pm$ 20 and log $\beta\sp{T}\sb{846}$ = log $\beta\sp{T}\sb{842}$ - (4.4 $\pm$ 0.3)n. At pH $>$ 9, Pu(VI)-phosphate species formed with absorption bands at 857 $\pm$ 1 nm ($\varepsilon$ = 200 $\pm$ 30) and 866 nm ($\varepsilon$ = 123 $\pm$ 15).
Issue Date:1994
Rights Information:Copyright 1994 Weger, Hans Thomas
Date Available in IDEALS:2011-05-07
Identifier in Online Catalog:AAI9512590
OCLC Identifier:(UMI)AAI9512590

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