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• W2809016279 abstract "Abstract Neptunium (Np) is a key element of concern for the safety aspects regarding the reprocessing and handling of spent nuclear fuel owing to its long half life (t1/2 = 2.14 × 106 years). Np can exist in several oxidation states in aquatic environments depending on the surrounding conditions in which it exists. The +5 oxidation state of Np as NpO2+ is the most stable and least binding moiety that can migrate in aquatic arena to far away positions from its source of origin. Humic acids, which are omnipresent in aquifers, are the major source of binding for the actinides including Np to facilitate their migration and transportation phenomenon. Probing the systematic knowledge of neptunium (Np), such as, speciation and coordination as function of its oxidation states in presence of chelating agents is essential aspect of its solution chemistry. The present study aimed at investigating the redox and complexation of Np with phenylphosphonic acid (PhPO3H2) (PPA) as mimic for binding of aromatic phosphorus functionalities in humic substances by using electrochemical and UV–Visible absorption spectroscopy and density functional calculations. The cyclic voltammetric measurement indicates the complexation of both oxidation states (V & VI) of Np with [PhPO3]2−. The presence and stability region (via Eh-pH plot) of new species of Np-PhPO3 in two different oxidation states (V & VI) in aqueous solution at varying physicochemical conditions are identified. The kinetics for reduction of Np complexes in different oxidation states are explored by evaluation of heterogeneous electron-transfer kinetic (D0, ko and α) parameters by cyclic voltammetric results. The spectral parameters, namely λmax and its molal extinction coefficient (e) are obtained from UV–Visible spectrophotometric measurements and are found to be 988.2 nm and 302 ± 8 mol−1 L cm−1 respectively. The electrochemical as well as UV–Visible spectrophotometric measurements showed the formation of 1:1 complex only and the stability constant (logβ) obtained for the same from both the methods found to be in agreement with each other. Density Functional Theory (DFT) calculations are carried out to optimize the geometries of Np-PhPO3 complex for the Np in +5 and +6 oxidation states with [PhPO3]2− in mono and bidentate mode to identify the most probable coordination mode for complex formation." @default.
• W2809016279 created "2018-06-29" @default.
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• W2809016279 date "2018-10-01" @default.
• W2809016279 modified "2023-10-01" @default.
• W2809016279 title "Electrochemical, spectroscopic and theoretical studies on redox speciation of neptunium with phenylphosphonic acid" @default.
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• W2809016279 doi "https://doi.org/10.1016/j.ica.2018.06.001" @default.
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