Thermodynamics of Np(IV) complexes with gluconic acid under alkaline conditions: sorption studies

被引:10
|
作者
Rojo, H. [1 ]
Tits, J. [2 ]
Gaona, X. [3 ]
Garcia-Gutierrez, M. [1 ]
Missana, T. [1 ]
Wieland, E. [2 ]
机构
[1] CIEMAT, Sorpt Migrat & Colloids Lab, E-28040 Madrid, Spain
[2] Paul Scherrer Inst, Lab Waste Management, Villigen, Switzerland
[3] Karlsruhe Inst Technol, Inst Nukl Entsorgung, D-76021 Karlsruhe, Germany
关键词
Neptunium(IV); Gluconate; Complexation; Sorption; Thermodynamic description; ALPHA-ISOSACCHARINIC ACID; EU(III); TH(IV);
D O I
10.1524/ract.2013.2022
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
The complexation of Np(IV) with gluconic acid (GLU) under alkaline conditions was investigated in the absence of Ca by carrying out a series of sorption experiments. The decrease of Np(IV) sorption on the sorbing material at increasing concentrations of GLU was interpreted as the formation of Np(IV)-GLU aqueous complexes. The modelling of experimental data according to the Schubert method [1] confirmed the formation of a complex with a Np : GLU ratio 1: 1. The stoichiometry of the complex Np(OH)(4)GLU(-) was proposed based on the experimental observation that no proton exchange occurred during the course of the complexation reaction and that Np(OH)(4)(aq) was the predominant hydrolysis product in the absence of GLU. A log*beta(0)(1,4,1) = 2.92 +/- 0.30 for the formation reaction Np4+ + 4H(2)O + GLU(-) double left right arrow Np(OH)(4)GLU(-) +4H(+) was calculated based on the conditional stability constants determined from sorption experiments and using the Np(IV) thermodynamic data selected in the NEA reviews [2]. Linear free energy relationships (LEER) confirmed that the stoichiometry and stability of the Np(IV)-GLU complex characterized in this work are consistent with data available for Th(IV)-, U(IV)- and Pu(IV)-GLU complexes.
引用
收藏
页码:133 / 138
页数:6
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