期刊
ENVIRONMENTAL SCIENCE & TECHNOLOGY
卷 47, 期 12, 页码 6214-6222出版社
AMER CHEMICAL SOC
DOI: 10.1021/es304677c
关键词
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资金
- National Science Foundation
- Austrian Academy of Sciences
- U.S. DOE NABIR Program
- U.S. DOE Subsurface Biogeochemical Research program's Sustainable Systems Science Focus Area at Lawrence Berkeley National Laboratory [DE-AC02-05CH11231]
This study focuses on the effects of fulvic acid (FA) on uranium(VI) sorption kinetics to a silica sand. Using a tritium-labeled FA in batch experiments made it possible to investigate sorption rates over a wide range of environmentally relevant FA concentrations (0.37-23 mg L-1 TOC). Equilibrium speciation calculations were coupled with an evaluation of U(VI) and FA sorption rates based on characteristic times. This allowed us to suggest plausible sorption mechanisms as a function of solution conditions (e.g., pH, U(VI)/FA/surface site ratios). Our results indicate that U(VI) sorption onto silica sand can be either slower or faster in the presence of FA compared to a ligand-free system. This suggests a shift in the underlying mechanisms of FA effects on U(VI) sorption, from competitive sorption to influences of U(VI)-FA complexes, in the same system. Changes in metal sorption rates depend on the relative concentrations of metals, organic ligands, and mineral surface sites. Hence, these results elucidate the sometimes conflicting information in the literature about the influence of organic matter on metal sorption rates. Furthermore, they provide guidance for the selection of appropriate sorption equilibration times for experiments that are designed to determine metal distribution coefficients (K-d values) under equilibrium conditions.
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