Chemical solubility of alkali metal uranate(VI) species in molten carbonates under basic and acidic conditions / Volkovich V.A., Griffiths T.R., Fray D.J., Thied R.C. // Physical Chemistry Chemical Physics. - 2000. - V. 2, l. 13. - P. 3029-3035.

ISSN:
14639076
Type:
Article
Abstract:
A detailed investigation of the dissolution of alkali metal uranates in carbonate melts under the influence of CO2 and O2 partial pressures has been performed between 450 and 800°C. At low temperatures or high CO2 pressure an acidic melt is formed. Acidic dissolution of uranates releases oxide ions and the possible dissolution routes of mono- and diuranates are discussed. At high temperatures carbonates begin to decompose, lose CO2, and become basic melts. Under these conditions, basic dissolution of uranates occurs and again the possible routes and products are discussed. Oxygen partial pressure influences uranate dissolution due to the formation of peroxycarbonate complexes. Under acidic conditions and using pure O2 under pressure a maximum solubility of K2UO4 of ca. 37 mol ppm in (Li-Na-K)2CO3 eutectic was evaluated. This system, when under CO2 and below 600°C, did not produce the expected yellow coloured (quenched) melts from the dissolution of uranates, but gave grey melts that became yellow only on heating above 600°C. The reproducible grey colour is due to a minor contribution from intervalence bands resulting from the formation of very low concentrations of oxygen-deficient polyuranates under these conditions.
Author keywords:
Index keywords:
alkali metal; carbon dioxide; carbonic acid derivative; oxygen; article; carbon dioxide tension; chemical reaction; oxygen tension; pressure; solubility; temperature
DOI:
10.1039/b001936o
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Affiliations School of Chemistry, University of Leeds, Leeds LS2 9JT, United Kingdom; Dept. of Mat. Science/Metallurgy, University of Cambridge, Pembroke Street, Cambridge CB2 3QZ, United Kingdom; British Nuclear Fuels plc., Sellafield R and D, Sellafield, Seascale, Cumbria CA20 1PG, United Kingdom; Department of Rare Metals, Physical-Engineering Faculty, Ural State Technical University-UPI, 19 Mira Ul, Ekaterinburg, 620002, Russian Federation
Chemicals/CAS carbon dioxide, 124-38-9, 58561-67-4; oxygen, 7782-44-7
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Correspondence Address Volkovich, V.A.; School of Chemistry, University of Leeds, Leeds LS2 9JT, United Kingdom
CODEN PPCPF
Language of Original Document English
Abbreviated Source Title Phys. Chem. Chem. Phys.
Source Scopus