NDLI: Experimental study of uraninite solubility in aqueous HCl solutions at 500°C and 1 kbar

Content Provider	Springer Nature Link
Author	Kovalenko, N. I. Ryzhenko, B. N. Prisyagina, N. I. Bychkova, Ya. V.
Copyright Year	2011
Abstract	Uraninite solubility in 0.001–2.0 m HCl solutions was experimentally studied at 500°C, 1000 bar, and hydrogen fugacity corresponding to the Ni/NiO buffer. It was shown that the following U(IV) species dominate in the aqueous solution: U(OH)40, U(OH)$_{2}$Cl20, and UOH Cl30 Using the results of uraninite solubility measurement, the Gibbs free energies of U(IV) species at 500°C and 1000 bar were calculated (kJ/mol): −9865.55 for UO$_{2}$(aq), −1374.57 for U(OH)$_{2}$ Cl20, and −1265.49 for UOH Cl30, and the equilibrium constants of uraninite dissolution in water and aqueous HCl solutions were estimated: UO$_{2}$(cr) = UO$_{2}$(aq), pK $_{0}$ = 6.64; UO$_{2}$(cr) + 2HCl$^{0}$ = U(OH)$_{2}$ Cl20, pK $_{2}$ = 3.56; and UO$_{2}$(cr) + 3HCl$^{0}$ = UOHcl30 + H$_{2}$O, pK $_{3}$ = 3.05. The value pK $_{1}$ ≈ 5.0 was obtained as a first approximation for the equilibrium UO$_{2}$(cr) + H$_{2}$O + HCl$^{0}$ = U(OH)$_{3}$Cl$^{0}$. The constant of the reaction UO$_{2}$(cr) + 4HCl$^{0}$ = UCl40 + 2H$_{2}$O (pK $_{4}$ = 7.02) was calculated taking into account the ionization constants of U Cl40 and U(OH)40, obtained by extrapolation from 25 to 500°C at 1000 bar using the BR model. Intense dissolution and redeposition of gold (material of experimental capsules) was observed in our experiments. The analysis and modeling of this phenomenon suggested that the UO$_{2 + x }$/UO$_{2}$ redox pair oxidized Au(cr) to Au$^{+}$(aq), which was then reduced under the influence of stronger reducers.
Starting Page	262
Ending Page	273
Page Count	12
File Format	PDF
ISSN	00167029
Journal	Geochemistry International
Volume Number	49
Issue Number	3
e-ISSN	15561968
Language	English
Publisher	SP MAIK Nauka/Interperiodica
Publisher Date	2011-03-23
Publisher Place	Dordrecht
Access Restriction	One Nation One Subscription (ONOS)
Subject Keyword	uranium uraninite hydrothermal solutions uranium geochemistry experimental study of solubility gold Geochemistry
Content Type	Text
Resource Type	Article
Subject	Geophysics Geochemistry and Petrology

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