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首页> 外文期刊>Environmental Science & Technology >Plutonium Partitioning Behavior to Humic Acids from Widely Varying Soils Is Related to Carboxyl-Containing Organic Compounds
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Plutonium Partitioning Behavior to Humic Acids from Widely Varying Soils Is Related to Carboxyl-Containing Organic Compounds

机译:Wide从多种多样的土壤中分配给腐殖酸的行为与含羧基的有机化合物有关

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摘要

In order to examine the influence of the HA molecular composition on the partitioning of Pu, ten different kinds of humic acids (HAs) of contrasting chemical composition, collected and extracted from different soil types around the world were equilibrated with groundwater at low Pu concentrations (10~(-14) M). Under mildly acidic conditions (pH ∼ 5.5), 29 ± 24% of the HAs were released as colloidal organic matter (>3 kDa to <0.45 μm), yet this HA fraction accounted for a vast majority of the bound Pu, 76 ± 13% on average. In comparison, the particulate HA fraction bound only 8 ± 4% on average of the added Pu. The truly dissolved Pu fraction was typically <1%. Pu binding was strongly and positively correlated with the concentrations of organic nitrogen in both particulate (>0.45 μm) and colloidal phases in terms of activity percentage and partitioning coefficient values (logK_d). Based on molecular characterization of the HAs by solid state ~(13)C nuclear magnetic resonance (NMR) and elemental analysis, Pu binding was correlated to the concentration of carboxylate functionalities and nitrogen groups in the particulate and colloidal phases. The much greater tendency of Pu to bind to colloidal HAs than to particulate HA has implications on whether NOM acts as a Pu source or sink during natural or man-induced episodic flooding.
机译:为了检查HA分子组成对Pu分配的影响,我们用低Pu浓度的地下水平衡了从世界各地不同土壤类型收集和提取的十种化学组成不同的腐殖酸(HAs)( 10〜(-14)M)。在弱酸性条件下(pH〜5.5),有29±24%的HA以胶态有机物形式释放(> 3 kDa至<0.45μm),但该HA占结合Pu的绝大部分,为76±13 % 一般。相比之下,颗粒HA分数平均仅占添加Pu的8±4%。真正溶解的Pu分数通常小于1%。在活性百分比和分配系数值(logK_d)方面,Pu的结合与颗粒态(> 0.45μm)和胶态相中有机氮的浓度呈强正相关。基于固态〜(13)C核磁共振(NMR)的分子表征和元素分析,Pu结合与颗粒和胶体相中羧酸盐官能团和氮基的浓度相关。 Pu结合胶体HA的趋势比颗粒HA的趋势大得多,这关系到NOM在自然或人为诱发的洪水泛滥期间是否充当Pu的来源或汇。

著录项

  • 来源
    《Environmental Science & Technology》 |2017年第20期|11742-11751|共10页
  • 作者单位

    Department of Marine Science, Texas A and M University at Galveston, Galveston, TX, United States;

    Department of Marine Science, Texas A and M University at Galveston, Galveston, TX, United States;

    Department of Marine Science, Texas A and M University at Galveston, Galveston, TX, United States;

    Division of Agroenvironmental Biology, Graduate School of Agriculture Science, Kobe University, Kyoto, Japan;

    Savannah River National Laboratory, Aiken, SC, United States;

    Los Alamos National Laboratory, Los Alamos, NM, United States;

    School of Human Science and Environment, University of Hyogo, 1-1-12 Shinzaike-Honcho, Himeji, Hyogo, Japan;

    Department of Marine Science, Texas A and M University at Galveston, Galveston, TX, United States;

    Department of Marine Science, Texas A and M University at Galveston, Galveston, TX, 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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  • 正文语种 eng
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