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Landsberger, Sheldon Weger, Hans Thomas 2011-05-07T14:00:38Z 2011-05-07T14:00:38Z 10000-01-01 1994 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). Made available in DSpace on 2011-05-07T14:00:38Z (GMT). No. of bitstreams: 2 license.txt: 4922 bytes, checksum: 910b249b4beec47e7ab768910c8f966f (MD5) 9512590.pdf: 10319080 bytes, checksum: 257fe27ecbf3e0986de45c76c03f8056 (MD5) Previous issue date: 1994 Item marked as restricted to the 'UIUC Users [automated]' Group (id=2) by Howard Ding (hding2@illinois.edu) on 2011-05-07T15:01:53Z Item is restricted indefinitely. Restriction data tranferred 2014-07-01T11:29:23-05:00 Original Data Group with Access UIUC Users [automated] Release Date: none Reason: ETDs are only available to UIUC Users without author permission ETDs are only available to UIUC Users without author permission U of I Only AAI9512590 (UMI)AAI9512590 http://hdl.handle.net/2142/23058 eng Copyright 1994 Weger, Hans Thomas Engineering, Nuclear Geochemistry Solubility and speciation of plutonium(VI) with orthophosphate text Nuclear, Plasma, and Radiological Engineering Nuclear, Plasma, and Radiological Engineering University of Illinois at Urbana-Champaign Dissertation Ph.D.