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Analyse critique des données de complexation des lanthanides et actinides par la matière organique naturelle : cas des substances humiques

Abstract : Critical analysis of the data on complexation of lanthanides and actinides by natural organic matter: particular case of humic substances.» Abstract-This document proposes a critical analysis of the models that describe the actinides and lanthanides complexation by natural organic matter in general and by humic substances in particular. In order to better delimit the particular properties of these substances the most influent physical and chemical properties on complexation are recalled as a preamble. Models as well as data that has been used are reviewed, compiled, and eventually compared to independent data in order to identify (i) their application domain, (ii) the possible simplifications which permit to obtain operational models, (iii) the conditions in which simplifications cannot be ascertained yet, and (iv) the data or fields of knowledge which are still too uncertain. A comparison between the different models is proposed in order to adapt parameters from one model to another minimising the experimental acquisitions, or at least to focus on missing data. Usually, data on the complexation of free ions M$^{z+}$ are reliable; as soon as hydrolysis, or competition with another ligand in general, in at stake data are much less reliable. Predictions from models are much more uncertain: formation of mixed complexes with hydroxide or carbonate anions is not univocal whatever the modelling strategy. Hints for transfer functions between models which are believed to be incompatible could be explored in order to justify necessary simplifications for using operational modelling. Influence on the solubility of oxides could be quantified, but it is difficult to clearly separate it from colloidal particles stabilisation. The account of the competition between cations by the models has also been tested. In view of the small number of available experimental data there still lie some uncertainties especially for the media that are close to neutrality and in the case of competition with magnesium, but overall in the case of the competition with aluminium and iron. The influence of redox activity of humic substances is also approached in the case of iron and actinides. Although the formal redox couple(s) cannot be yet identified, it seems that an operational E$_h$ = f(pH) relationship can be proposed
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Pascal E. Reiller. Analyse critique des données de complexation des lanthanides et actinides par la matière organique naturelle : cas des substances humiques. [Rapport de recherche] CEA-R-6240, CEA. 2010, pp.184. ⟨cea-02285988⟩

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