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土壤中砷(V)的吸附、螯合及生物可利用性

Adsorption, sequestration, and bioaccessibility of As(V) in soils.

作者信息

Yang Jae-Kyu, Barnett Mark O, Jardine Philip M, Basta Nicholas T, Casteel Stan W

机构信息

Department of Civil Engineering, Auburn University, Alabama 36849, USA.

出版信息

Environ Sci Technol. 2002 Nov 1;36(21):4562-9. doi: 10.1021/es011507s.

Abstract

The influence of various soil physical and chemical properties (Fe and Mn oxides, pH, cation exchange capacity, total inorganic and organic carbon, and particle size) on As(V) adsorption, sequestration, and relative bioaccessibility (as a surrogate for oral bioavailability) was investigated in a wide range of well-characterized soils over a 6-month period. Arsenic(V) bioaccessibility was measured using a streamlined version of a physiologically based extracton test (PBET), designed to replicate the solubility-limiting conditions in a child's digestive tract. The soil's dithionite-citrate-bicarbonate (DCB) extractable Fe oxide content was the most important land only statistically significant) soil property controlling the initial degree of adsorption. Sequestration, as measured by the reduction in bioaccessibility over time, occurred to a significant extent in 17 of 36 (47.2%) soils over the first 3 months. In contrast, only 4 of 36 (11.1%) soils exhibited a significant reduction in bioaccessibility from 3 to 6 months. Soil pH was the most important (and only statistically significant) soil property affecting the decrease in bioaccessibility upon aging for 6 months. Soils with pH < 6 generally sequestered As(V) more strongly over time, whereas those with pH > 6 generally did not. The Fe oxide content and pH were the most important soil properties governing the steady-state bioaccessibility of As(V) in soil. Two multivariable linear regression models of steady-state As(V) bioaccessibility were developed using soil properties as independent variables. Generally, soils having higher Fe oxide content and lower soil pH exhibited lower bioaccessibility. These models were able to account for approximately 75-80% of the variability in steady-state bioaccessibility and independently predict bioaccessibility in five soils within a root-mean-square error (RMSE) of 8.2-10.9%. One of these models was also able to predict within an RMSE of 9.5% the in vivo bioavailability of As in nine contaminated soils previously used in swine dosing trials. These results indicate the bioaccessibility, and thus, potentially the bioavailability of otherwise soluble As(V) added to soils (i.e., the worst-case bioavailability scenario) is significantly reduced in some soils over time, particularly those with lower pH and higher Fe oxide content. These results also provide a means of estimating As(V) bioaccessibility and bioavailability on the basis of soil properties.

摘要

在6个月的时间里,研究了各种土壤物理和化学性质(铁和锰氧化物、pH值、阳离子交换容量、总无机碳和有机碳以及粒径)对五价砷(As(V))吸附、固存和相对生物可利用性(作为口服生物利用度的替代指标)的影响,研究对象为一系列特征明确的土壤。使用基于生理学的提取试验(PBET)的简化版本测量了五价砷的生物可利用性,该试验旨在模拟儿童消化道中的溶解度限制条件。土壤连二亚硫酸盐 - 柠檬酸盐 - 碳酸氢盐(DCB)可提取的铁氧化物含量是控制初始吸附程度的最重要(且仅具有统计学意义)的土壤性质。在前3个月中,36种土壤中有17种(47.2%)的固存现象(通过生物可利用性随时间的降低来衡量)显著发生。相比之下,36种土壤中只有4种(11.1%)在3至6个月期间生物可利用性显著降低。土壤pH值是影响老化6个月后生物可利用性降低的最重要(且仅具有统计学意义)的土壤性质。pH值<6的土壤通常随着时间的推移对五价砷的固存作用更强,而pH值>6的土壤通常并非如此。铁氧化物含量和pH值是控制土壤中五价砷稳态生物可利用性的最重要土壤性质。利用土壤性质作为自变量,建立了两个五价砷稳态生物可利用性的多变量线性回归模型。一般来说,铁氧化物含量较高且土壤pH值较低的土壤生物可利用性较低。这些模型能够解释稳态生物可利用性中约75 - 80%的变异性,并能在均方根误差(RMSE)为8.2 - 10.9%的范围内独立预测五种土壤中的生物可利用性。其中一个模型还能够在RMSE为9.5%的范围内预测先前用于猪给药试验的九种受污染土壤中砷的体内生物利用度。这些结果表明,随着时间的推移,添加到土壤中的原本可溶的五价砷的生物可利用性,进而潜在的生物利用度(即最坏情况下的生物利用度情况)在某些土壤中会显著降低,特别是那些pH值较低且铁氧化物含量较高的土壤。这些结果还提供了一种基于土壤性质估算五价砷生物可利用性和生物利用度的方法。

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