Thermodynamics of Cm(III) in Concentrated Salt Solutions: Carbonate Complexation in NaCl Solution at 25°C

Fanghänel, Th.; Könnecke, Th.; Weger, Hans; Paviet-Hartmann, Patricia; Neck, V.; Kim, J. I.

doi:10.1023/a:1022664013648

Cited by 35 publications

(27 citation statements)

References 13 publications

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“…In order to study the influence of carbonate on the complexation of Cm(III) with hTf/2N, the complex formation was studied as a function of pH at physiological carbonate concentration (c(carbonate) tot = 25 mM). The term physiological carbonate concentration describes a total concentration of the species CO 32 Comparison with blank solutions (without hTf/2N) in the same pH range proves that these emission bands result from Cm(III) carbonate interactions and do not represent additional transferrin species. The Cm(III) hTf/2N species with λ max = 619.7 nm is formed at pH ≥ 10.5 which indicates a distinct competition between carbonate and hTf/2N.…”

Section: Complexation Of Cm(iii) With Htf/2n At Physiological Carbonamentioning

confidence: 85%

Complexation of Cm(iii) with the recombinant N-lobe of human serum transferrin studied by time-resolved laser fluorescence spectroscopy (TRLFS)

et al. 2015

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The complexation of Cm(III) with the recombinant N-lobe of human serum transferrin (hTf/2N) is investigated in the pH range from 4.0 to 11.0 using TRLFS. At pH ≥ 7.4 a Cm(III) hTf/2N species is formed with Cm(III) bound at the Fe(III) binding site. The results are compared with Cm(III) transferrin interaction at the C-lobe and indicate the similarity of the coordination environment of the C- and N-terminal binding sites with four amino acid residues of the protein, two H2O molecules and three additional ligands (e.g. synergistic anions such as carbonate) in the first coordination sphere. Measurements at c(carbonate)tot = 0.23 mM (ambient carbonate concentration) and c(carbonate)tot = 25 mM (physiological carbonate concentration) show that an increase of the total carbonate concentration suppresses the formation of the Cm(III) hTf/2N species significantly. Additionally, the three Cm(III) carbonate species Cm(CO3)(+), Cm(CO3)2(-) and Cm(CO3)3(3-) are formed successively with increasing pH. In general, carbonate complexation is a competing reaction for both Cm(III) complexation with transferrin and hTf/2N but the effect is significantly higher for the half molecule. At c(carbonate)tot = 0.23 mM the complexation of Cm(III) with transferrin and hTf/2N starts at pH ≥ 7.4. At physiological carbonate concentration the Cm(III) transferrin species II forms at pH ≥ 7.0 whereas the Cm(III) hTf/2N species is not formed until pH > 10.0. Hence, our results reveal significant differences in the complexation behavior of the C-terminal site of transferrin and the recombinant N-lobe (hTf/2N) towards trivalent actinides.

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Section: Complexation Of Cm(iii) With Htf/2n At Physiological Carbonamentioning

confidence: 85%

Complexation of Cm(iii) with the recombinant N-lobe of human serum transferrin studied by time-resolved laser fluorescence spectroscopy (TRLFS)

et al. 2015

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“…The main objectives were then the determination of the nature of the species, such as hydrolyzed species, inorganic or organic complexes, and their formation energies. A typical Cm(III) as Cm 3+ 394 594 65 10 − 9 5 × 10 − 13 example is the study of the complexation of Cm(III) by carbonates; TRLIF was used to determine the stoichiometries of the carbonate complexes and the thermodynamic formation constants (Fangh ä nel et al , 1999;Vercouter et al , 2005b). Other complex formation reactions have been successfully investigated by TRLIF (Eliet et al , 1995;Colette et al , 2004;Geipel, 2006;Vercouter et al , 2008), as a complement to classical methods for the determination of chemical data (potentiometry, spectrophotometry, solvent extraction, solubility, electrochemistry, etc.).…”

Section: Time-resolved Laser-induced Fluorescence (Lif) For Analysis mentioning

confidence: 99%

Applications of laser spectroscopy in nuclear research and industry

Mauchien

Pailloux

Vercouter

2014

Laser Spectroscopy for Sensing

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“…Mixing of the Pitzer databases should be avoided. Parameters for the Pitzer model used in our calculations are available in the extended Harvie-Møller-Weare database (Na-K-Mg-Ca-H-Cl-SO 4 -OH-HCO 3 -CO 3 /CO 2 -H 2 O system), 9) but also for selected RN, [10][11][12][13][14] heavy metals, and other relevant elements. For systems including cement, aqueous silicate and aluminate species as well as additional solid phases had to be incorporated into the database.…”

Section: Thermodynamic Databasementioning

confidence: 99%

Geochemically Based Safety Assessment

Kienzler

Metz

Lützenkirchen

et al. 2007

J. Nucl. Sci. Technol.

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ÃÃPerformance assessment (PA) for nuclear waste disposal based on transport processes frequently neglects significant safety factors by overestimation of radionuclide mobilization and underestimation of radionuclide retention processes. To include well understood geochemical knowledge into PA, the quasi-closed system approach (QCS) was developed. The QCS approach is described and applied to a LLW disposal in a German salt mine with respect to the disposed waste forms, geo-engineered barriers, and backfill strategies. The geochemical tools and the thermodynamic database for modelling highly concentrated salt systems are discussed. Applications are demonstrated which cover the long-term geochemical environment in the disposal caverns, the optimization of buffer materials, radionuclide retention, and the overall robustness of the approach. Also the effect of a potential solution exchange between different emplacement caverns is investigated. It is shown that the QCS approach provides essential data concerning the long-term geochemistry and related radionuclide concentrations to be used in PA and safety analysis.

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Thermodynamics of Cm(III) in Concentrated Salt Solutions: Carbonate Complexation in NaCl Solution at 25°C

Cited by 35 publications

References 13 publications

Complexation of Cm(iii) with the recombinant N-lobe of human serum transferrin studied by time-resolved laser fluorescence spectroscopy (TRLFS)

Complexation of Cm(iii) with the recombinant N-lobe of human serum transferrin studied by time-resolved laser fluorescence spectroscopy (TRLFS)

Applications of laser spectroscopy in nuclear research and industry

Geochemically Based Safety Assessment

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