Article ID | Journal | Published Year | Pages | File Type |
---|---|---|---|---|
6476888 | The Journal of Chemical Thermodynamics | 2017 | 26 Pages |
Abstract
Samples of synthetic analogs of uranyl phosphate minerals have been prepared at room temperature by slow mixing of reactants by a diffusion method. Reaction products were analyzed using powder X-ray diffraction (PXRD), thermogravimetric analysis (TGA), inductively coupled plasma optical emission spectrophotometry (ICP-OES), and inductively coupled plasma mass spectrometry (ICP-MS). Calorimetric measurements have been performed in a Calvet-type twin calorimeter using sodium molybdate (3Na2O-4MoO3) solvent at 976 K as a flux. The enthalpy of formation from the binary oxides, ÎHf-ox, at 298 K was calculated for each compound from the respective drop solution enthalpies, ÎHds. Calculated standard enthalpies of formation from the elements, ÎH0f, at 298 K are â3425 ± 9 kJ/mol for meta-ankoleite (KUP), â6233 ± 17 kJ/mol for meta-autunite (CaUP), â6921 ± 13 kJ/mol for meta-torbernite (CuUP), â7254 ± 17 kJ/mol for meta-saléeite (MgUP), â3264 ± 12 kJ/mol for Rb-meta-autunite (RbUP), â3580 ± 7 kJ/mol for meta-natro-autunite (NaUP), â3692 ± 11 kJ/mol for Li-meta-autunite (LiUP), â6402 ± 5 kJ/mol for meta-uranocircite (BaUP), â3277 ± 6 kJ/mol for Cs-meta-autunite (CsUP), and â7109 ± 19 kJ/mol for Co-meta-autunite (CoUP). The results exhibit trends of the thermodynamic stability of these compounds. The normalized charge deficiency per anion (NCDA) approach relates the thermodynamic stability of these compounds to their crystal structures. The thermodynamic stability of uranyl phosphate minerals is important for understanding their formation in Nature, as well as their fate in a geological repository for nuclear waste, and their existence in the subsurface of anthropogenically contaminated environments.
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Authors
Ewa A. Dzik, Haylie L. Lobeck, Lei Zhang, Peter C. Burns,