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- W1993301464 abstract "A detailed reevaluation of the complexation equilibria of plutonium(IV) with the polyaminocarboxylic sequestering agent EDTA4− has been performed in 1 M (H,K)NO3 media at 298 K by means of visible absorption spectrophotometry and glass-electrode potentiometry at millimolar concentration levels. The high binding affinity even under strongly acidic conditions supports the exclusive formation of the neutral Pu(EDTA) complex over the range 0.01 ≤ [H+] ≤ 0.9 M with an apparent formation constant of log β110 = 25.8(1) at 0.9 M HNO3. Extrapolation to zero ionic strength using the SIT approach provides the first ever-reported NEA–TDB compliant estimate of β1100(logβ1100=32.2(3)). A global modeling procedure of the potentiometric data collected for three different metal over ligand ratios (1:1, 1:1.5, and 1:2) ascertained the formation of four additional species for pH values comprised between 2 and 6.5, namely [Pu(EDTA)(OH)]−, [Pu(EDTA)2H2]2−, [Pu(EDTA)2H]3−, and [Pu(EDTA)2]4−. The visible absorption spectra for the first three complexes have also been determined. Data recorded above pH 3.5 (for a 1:1 molar ratio) or 6.5 (for a 1:2 molar ratio) were finally excluded from the global fitting procedure as speciation calculations suggested the precipitation of amorphous Pu(OH)4(am) according to the latest critical value quoted in the literature for its solubility product. La nature et la stabilité des complexes formés à l'équilibre entre le plutonium(IV) et l'EDTA4− ont été réévaluées en milieu nitrique à force ionique (I = 1 M (H,K)NO3) et à température (T = 298 K) contrôlées par spectrophotométrie d'absorption et potentiométrie. L'affinité élevée de l'agent chélateur dans des conditions fortement acides (log β110 = 25,8(1) en milieu 0,9 M HNO3) s'explique par la formation exclusive du complexe neutre Pu(EDTA) dans la gamme 0,01 ≤ [H+] ≤ 0,9 M. L'extrapolation à force ionique nulle à l'aide de la théorie des interactions spécifiques dite SIT, permet de proposer la première valeur de β1100(logβ1100=32.2(3)) qui soit conforme aux recommandations de la base de données thermodynamiques de l'Agence pour l'énergie nucléaire. L'ajustement simultané des courbes de titrage potentiométrique enregistrées pour trois rapports métal/ligand différents (1:1, 1:1,5 et 1:2) est compatible avec la formation de quatre espèces additionnelles entre pH 2 et 6,5, à savoir [Pu(EDTA)(OH)]−, [Pu(EDTA)2H2]2−, [Pu(EDTA)2H]3− et [Pu(EDTA)2]4−. L'exploitation des données spectrophotométriques a également permis d'accéder aux spectres d'absorption électroniques dans le domaine visible pour les trois premiers complexes. Les données collectées au-delà de p[H] 3,5 pour un rapport molaire 1:1 ou 6,5 pour un rapport 1:2 ont été exclues lors de la procédure d'affinement des constantes d'équilibre, en raison de l'apparition de la phase solide amorphe Pu(OH)4(am) suggérée par les calculs de spéciation effectués en parallèle, qui s'appuient sur la valeur critique la plus récente du produit de solubilité du tétrahydroxyde de plutonium." @default.
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- W1993301464 date "2007-10-01" @default.
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- W1993301464 title "Thermodynamic studies of actinide complexes. 1. A reappraisal of the solution equilibria between plutonium(IV) and ethylenediaminetetraacetic acid (EDTAH4) in nitric media" @default.
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- W1993301464 doi "https://doi.org/10.1016/j.crci.2007.04.006" @default.
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