Prediction of Redox Potentials for Different Oxidation States of U, Np, Pu, and Am in Alkaline Aqueous Solution

Dutra, Felipe R.; Dixon, David A.

doi:10.1021/acs.jpca.4c08794

Prediction of Redox Potentials for Different Oxidation States of U, Np, Pu, and Am in Alkaline Aqueous Solution

Journal Article · Thu Feb 27 00:00:00 EST 2025 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI:https://doi.org/10.1021/acs.jpca.4c08794· OSTI ID:3022004

Dutra, Felipe R. ^[1]; ^[2]

Universidade Estadual de Campinas, São Paulo (Brazil); The University of Alabama, Tuscaloosa, AL (United States)
The University of Alabama, Tuscaloosa, AL (United States)

The redox potentials for U, Np, Pu, and Am for oxidation states +III up to +VIII in alkaline aqueous solutions were predicted using density functional theory (DFT) and small-core pseudopotentials and their basis sets, with a hybrid explicit/implicit solvent model using SHE = 4.28 V. For each oxidation state, various oxo/hydroxo complexes were evaluated resulting in a variety of one-electron redox pathways. For An(VIII/VII) couples, the predicted redox potentials for the [An(VIII)O₅(OH)]^-3/[An(VII)O₄(OH)₂]^-3, or [An(VIII)O₄(OH)₂]^-2/[An(VII)O₄(OH)₂]^-3 couples are in good agreement with existing estimates. For An(VII/VI) redox couples, all couples, particularly [An(VII)O₄(OH)₂]^-3/[An(VI)O₂(OH)₄]^-2, were in agreement with experimental values for U, Np, and Pu, but the results for Am showed larger differences from the estimated potentials. The An(VI/V) couples were consistent with experiment for dioxo/tetrahydroxo couples, and the An(V/IV) couples showed acceptable agreement based on actinide-specific couples, with neutral hydroxides often favored in the +IV state. The An(IV/III) couples were consistent with literature values when modeled as soluble neutral hydroxides. The use of our approach yielded calculated redox potentials that were within ±0.2 V from experimental or estimated values consistent with our prior calculations on redox potentials of actinides from Ac to Am in acidic aqueous solutions. Finally, as a result, this supports the robustness of our DFT-based methodology for predicting actinide redox potentials, offering valuable insights for actinide chemistry in aqueous solutions.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Alabama, Tuscaloosa, AL (United States); University of Alabama, Tuscaloosa, AL (United States)

Sponsoring Organization:: São Paulo Research Foundation (FAPESP); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0018921

Other Award/Contract Number:: 2023/02596-0

OSTI ID:: 3022004

Alternate ID(s):: OSTI ID: 3004795

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Journal Name: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory Journal Issue: 10 Vol. 129; ISSN 1089-5639; ISSN 1520-5215

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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