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腐殖质与砷形态在模拟环境条件下的相互作用。

Interaction between humic substances and arsenic species simulating environmental conditions.

机构信息

Instituto de Química e Biotecnologia, Universidade Federal de Alagoas, Campus A. C. Simões, 57072-900 Maceió, AL, Brazil.

Instituto de Química e Biotecnologia, Universidade Federal de Alagoas, Campus A. C. Simões, 57072-900 Maceió, AL, Brazil.

出版信息

Sci Total Environ. 2022 Jan 1;802:149779. doi: 10.1016/j.scitotenv.2021.149779. Epub 2021 Aug 25.

Abstract

The importance of evaluating how natural organic matter influences the mobility of arsenic species in an ecosystem is an environmental concern. This work aimed to evaluate the interaction between humic substances (HS) and four arsenic species of high toxicity [As(III), As(V), MMA(V), and DMA(V)] (HS-As) under the influence of HS concentration and pH. Next, the complexing capacity (CC) of HS by As(III) was determined in function of pH, ionic strength and co-existing ions. The free arsenic (As) was determined after a tangential flow ultrafiltration procedure by hydride generation atomic fluorescence spectrometry. The better HS-As interactions for As(III) and As(V) at pH 10.5 reached 52% and 61%, respectively. The increase in pH and ionic strength, as well as co-existing ions increased the CC, which reached 1.57 mg of As(III) g HS. We proposed a HS-As interaction model based on the inner and outer binding sites of HS from these results. The inner sites were occupied through hydrogen bonds, Pearson acid-base, hydrophobic, and van der Waals interactions for trivalent arsenic species, while the interactions through the outer sites for pentavalent arsenic species were mostly by hydrogen bonds and electrostatic forces. According to ecotoxicological studies against Artemia salina, the presence of HS decreased the toxicity of As(III) and As(V) as the lethal concentration increased from 5.81 to 8.82 mg L and from 8.82 to 13.37 mg L, respectively. From the results through the proposed model, it was possible to successfully understand the interaction dynamic between soil HS and As(III), As(V), MMA(V) and DMA(V) under simulated environmental conditions.

摘要

评估自然有机质如何影响生态系统中砷形态迁移的重要性是一个环境关注点。本工作旨在评估腐殖质(HS)浓度和 pH 影响下,HS 与四种高毒性砷形态[三价砷(As(III))、五价砷(As(V))、一甲基砷酸(MMA(V))和二甲基砷酸(DMA(V))](HS-As)之间的相互作用。接下来,确定了 pH、离子强度和共存离子对 HS 与 As(III)络合能力(CC)的影响。通过氢化物发生原子荧光光谱法,在切向流超滤程序后测定游离砷(As)。在 pH 10.5 时,HS-As 对 As(III)和 As(V)的相互作用最好,分别达到 52%和 61%。pH 和离子强度的增加以及共存离子的增加增加了 CC,达到 1.57mg 的 As(III)g HS。根据这些结果,我们提出了一个基于 HS 内、外结合位点的 HS-As 相互作用模型。内结合位点通过氢键、Pearson 酸碱、疏水性和范德华相互作用被三价砷物种占据,而外结合位点的相互作用主要通过氢键和静电力对五价砷物种进行。根据对卤虫的生态毒理学研究,HS 的存在降低了 As(III)和 As(V)的毒性,致死浓度分别从 5.81mg/L 增加到 8.82mg/L 和从 8.82mg/L 增加到 13.37mg/L。根据所提出模型的结果,可以成功地理解在模拟环境条件下土壤 HS 与 As(III)、As(V)、MMA(V)和 DMA(V)之间的相互作用动态。

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