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Effect of Natural Organic Matter on Plutonium Sorption to Goethite

机译:天然有机物对P吸附针铁矿的影响

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摘要

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 mgr-L~(-1) and 50 mgc.L~(-1) natural organic matter (NOM), 10~(-9)-10~(-10) M ~(238)Pu, and 0.1 g•L~(-1) goethite concentrations, at pH 3, 5, 7, and 9. Low sorption of ligands coupled with strong Pu compilation 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 fonnation 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 facitate fonnation 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. 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.
机译:通过分批吸附实验研究了柠檬酸(CA),去铁草胺B(DFOB),富里酸(FA)和腐殖酸(HA)对go(Pu)吸附针铁矿的影响与有机碳浓度和pH的关系在5 mgr-L〜(-1)和50 mgc.L〜(-1)天然有机物(NOM),10〜(-9)-10〜(-10)M〜(238)Pu和0.1 g •L〜(-1)针铁矿浓度,pH为3、5、7和9。相对于不含配体的系统,低配体吸附以及强Pu汇编降低了pH 5和7时Pu的吸附。相反,在pH 3时,CA,FA和HA会增加Pu对针铁矿的吸附,表明形成三元络合物,或者在腐殖酸的情况下,掺入HA聚集体中。在不存在Pu的情况下,通过傅里叶变换红外光谱法表征了三元络合物的形成机理。 CA和FA在pH 3下显示出清晰的表面相互作用,HA保持不变,表明已形成HA聚集体,未观察到DFOB相互作用。在所有检查的pH值下,在DFOB存在下(相对于无配体系统),的吸附均降低。因此,DFOB似乎不促进三元Pu-DFOB-针铁矿复合物的形成。在pH为9时,在所有NOM存在下,Pu的吸附量相对于pH 5和7有所增加。形态模型将其归因于Pu(IV)水解与配体络合竞争,从而增加了吸附。结果表明,在简单的Pu-NOM-针铁矿三元批料系统中,NOM在所有条件下(特别是在低pH条件下)都会降低Pu对针铁矿的吸附。

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  • 来源
    《Environmental Science & Technology》 |2017年第1期|699-708|共10页
  • 作者单位

    Department of Environmental Engineering and Earth Sciences, Clemson University, Clemson, South Carolina 29634, United States;

    Glenn T. Seaborg Institute, Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, California 94550, United States;

    Glenn T. Seaborg Institute, Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, California 94550, United States;

    Department of Environmental Engineering and Earth Sciences, Clemson University, Clemson, South Carolina 29634, United States;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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