The Heat of Formation of the Uranyl Dication: Theoretical Evaluation Based on Relativistic Density Functional Calculations Full article
Journal |
Chemistry - A European Journal
ISSN: 0947-6539 , E-ISSN: 1521-3765 |
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Output data | Year: 2006, Volume: 12, Number: 2, Pages: 629-634 Pages count : 6 DOI: 10.1002/chem.200500628 | ||
Tags | Actinides, Density functional calculations, Heats of formation, Relativistic effects, Uranyl | ||
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Abstract:
By using a set of model reactions, we estimated the heat of formation of gaseous UO22+ from quantum-chemical reaction enthalpies and experimental heats of formation of reference species. For this purpose, we performed relativistic density functional calculations for the molecules UO22+, UO2, UF6, and UF5. We used two gradient-corrected exchange-correlation functionals (revised Perdew–Burke–Ernzerhof (PBEN) and Becke–Perdew (BP)) and we accounted for spin-orbit interaction in a self-consistent fashion. Indeed, spin-orbit interaction notably affects the energies of the model reactions, especially if compounds of UIV are involved. Our resulting theoretical estimates for Δfequation image(UO22+), 365±10 kcal mol−1 (PBEN) and 370±12 kcal mol−1 (BP), are in quantitative agreement with a recent experimental result, 364±15 kcal mol−1. Agreement between the results of the two different exchange-correlation functionals PBEN and BP supports the reliability of our approach. The procedure applied offers a general means to derive unknown enthalpies of formation of actinide species based on the available well-established data for other compounds of the element in question.
Cite:
Moskaleva L.V.
, Matveev A.V.
, Krüger S.
, Rösch N.
The Heat of Formation of the Uranyl Dication: Theoretical Evaluation Based on Relativistic Density Functional Calculations
Chemistry - A European Journal. 2006. V.12. N2. P.629-634. DOI: 10.1002/chem.200500628 WOS Scopus РИНЦ
The Heat of Formation of the Uranyl Dication: Theoretical Evaluation Based on Relativistic Density Functional Calculations
Chemistry - A European Journal. 2006. V.12. N2. P.629-634. DOI: 10.1002/chem.200500628 WOS Scopus РИНЦ
Dates:
Submitted: | Jun 2, 2005 |
Published online: | Dec 6, 2005 |
Published print: | Jan 1, 2006 |
Identifiers:
Web of science | WOS:000234453300032 |
Scopus | 2-s2.0-29544444687 |
Elibrary | 15345105 |
Chemical Abstracts | 2006:57792 |
Chemical Abstracts (print) | 144:199820 |
OpenAlex | W2148033633 |