Sorption and redox speciation of plutonium at the illite surface under highly saline conditions

JOURNAL OF COLLOID AND INTERFACE SCIENCE

卷:485

Article

Marsac, Remi^1,2  Banika, Nidhu Lal^1,3  Luetzenkirchen, Johannes¹  Diascorn, Alexandre^1,4  Bender, Kerstin¹  Marquardt, Christian Michael¹  Geckeis, Horst¹ 

[1] Karlsruhe Inst Technol, Inst Nukl Entsorgung, POB 3640, D-76021 Karlsruhe, Germany

[2] Ecole Natl Super Chim Rennes, CNRS, UMR 6226, 11 Allee Beaulieu, F-35708 Rennes 7, France

[3] European Commiss, Inst Transuranium Elements, POB 2340, D-76125 Karlsruhe, Germany

[4] BCRM Cherbourg, EAMEA, GEA, CC19, F-50115 Octeville, France

关键词: Plutonium;    Illite;    Clay;    Saline;    Speciation;    Redox;    Sorption;    Surface complexation model;    Ion exchange;   

DOI  :  10.1016/j.jcis.2016.09.013

来源: Elsevier

【 摘 要 】

Natural groundwater may contain high salt concentrations, such as those occurring at several potential deep geological nuclear waste repository sites. Actinide sorption to clays (e.g. illite) under saline conditions has, however, been rarely studied. Furthermore, both illite surface and ionic strength may affect redox speciation of actinides like plutonium. In the present study, Pu sorption to illite is investigated under anaerobic conditions for 3 < pH(m) (=-log m(H+)) < 10 and m(Nacl) = 1.0 and 3.2 molal (m). Results are compared with previous data for m(Nacl) = 0.1 m. According to redox potential measurements and based on Eu(III)-illite sorption data (taken as analogue of Pu(III)), the strong effect of m(Nacl) on overall Pu uptake observed for pH(m) < 6 is mainly attributed to the presence of Pu(III) and its competition with Na+ for ion exchange sites. For pH(m) > 6, overall Pu uptake is largely insensitive to m(Nacl) due to the prevalence of strongly adsorbed Pu(IV). By applying appropriate corrections to the activity coefficients of dissolved ions and using the 2-site protolysis non-electrostatic surface complexation and cation exchange (2 SPNE SC/CE) model, experimental data on Pu sorption to illite as a function of pH, Eh and m(Nacl) can be very well reproduced. (C) 2016 Elsevier Inc. All rights reserved.

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