Effect of Natural Organic Matter on Plutonium Sorption to Goethite

Conroy, Nathan A.; Zavarin, Mavrik; Kersting, Annie B.; Powell, Brian A.

doi:10.1021/acs.est.6b03587

Effect of Natural Organic Matter on Plutonium Sorption to Goethite

Journal Article · Sun Nov 20 23:00:00 EST 2016 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.6b03587· OSTI ID:1409924

Conroy, Nathan A. ^[1]; Zavarin, Mavrik ^[2]; Kersting, Annie B. ^[2]; ^[3]

Clemson Univ., SC (United States). Department of Environmental Engineering and Earth Sciences
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Glenn T. Seaborg Institute, Physical and Life Sciences Directorate
Clemson Univ., SC (United States). Department of Environmental Engineering and Earth Sciences

For this research, the effect of citric acid (CA), desferrioxamine B (DFOB), fulvic acid (FA), and humic acid (HA) on plutonium (Pu) sorption to goethite was studied as a function of organic carbon concentration and pH using batch sorption experiments at 5 mg_C·L^–1 and 50 mg_C·L^–1 natural organic matter (NOM), 10^–9–10^–10 M ²³⁸Pu, and 0.1 g·L^–1 goethite concentrations, at pH 3, 5, 7, and 9. Low sorption of ligands coupled with strong Pu complexation decreased Pu sorption at pH 5 and 7, relative to a ligand-free system. Conversely, CA, FA, and HA increased Pu sorption to goethite at pH 3, suggesting ternary complex formation or, in the case of humic acid, incorporation into HA aggregates. Mechanisms for ternary complex formation were characterized by Fourier transform infrared spectroscopy in the absence of Pu. CA and FA demonstrated clear surface interactions at pH 3, HA appeared unchanged suggesting HA aggregates had formed, and no DFOB interactions were observed. Plutonium sorption decreased in the presence of DFOB (relative to a ligand free system) at all pH values examined. Thus, DFOB does not appear to facilitate formation of ternary Pu-DFOB-goethite complexes. At pH 9, Pu sorption in the presence of all NOM increased relative to pH 5 and 7; speciation models attributed this to Pu(IV) hydrolysis competing with ligand complexation, increasing sorption. In conclusion, the results indicate that in simple Pu-NOM-goethite ternary batch systems, NOM will decrease Pu sorption to goethite at all but particularly low pH conditions.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1409924

Report Number(s):: LLNL-JRNL--734915

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 1 Vol. 51; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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