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在广泛的温带土壤中,pH、表面电荷和土壤特性对全氟烷基物质(PFASs)的固-液分配的影响。

Effect of pH, surface charge and soil properties on the solid-solution partitioning of perfluoroalkyl substances (PFASs) in a wide range of temperate soils.

机构信息

Department of Soil and Environment, Swedish University of Agricultural Sciences (SLU), Box 7014, SE-750 07, Uppsala, Sweden.

Department of Soil and Environment, Swedish University of Agricultural Sciences (SLU), Box 7014, SE-750 07, Uppsala, Sweden; Swedish Geotechnical Institute (SGI), SE-581 93, Linköping, Sweden.

出版信息

Chemosphere. 2023 Apr;321:138133. doi: 10.1016/j.chemosphere.2023.138133. Epub 2023 Feb 13.

Abstract

The pH-dependent soil-water partitioning of six perfluoroalkyl substances (PFASs) of environmental concern (PFOA, PFDA, PFUnDA, PFHxS, PFOS and FOSA), was investigated for 11 temperate mineral soils and related to soil properties such as organic carbon content (0.2-3%), concentrations of Fe and Al (hydr)oxides, and texture. PFAS sorption was positively related to the perfluorocarbon chain length of the molecule, and inversely related to solution pH for all substances. The negative slope between log K and pH became steeper with increasing perfluorocarbon chain length of the PFAS (r = 0.75, p ≤ 0.05). Organic carbon (OC) alone was a poor predictor of the partitioning for all PFASs, except for FOSA (r = 0.71), and the OC-normalized PFAS partitioning, as derived from organic soil materials, underestimated PFAS sorption to the soils. Multiple linear regression suggested sorption contributions (p ≤ 0.05) from OC for perfluorooctane sulfonate (PFOS) and FOSA, and Fe/Al (hydr)oxides for PFOS, FOSA, and perfluorodecanoate (PFDA). FOSA was the only substance under study for which there was a statistically significant correlation between its binding and soil texture (silt + clay). To predict PFAS sorption, the surface net charge of the soil organic matter fraction of all soils was calculated using the Stockholm Humic Model. When calibrated against charge-dependent PFAS sorption to a peat (Oe) material, the derived model significantly underestimated the measured K values for 10 out of 11 soils. To conclude, additional sorbents, possibly including silicate minerals, contribute to the binding of PFASs in soil. More research is needed to develop geochemical models that can accurately predict PFAS sorption in soils.

摘要

六种环境关注的全氟烷基物质(PFAS)(PFOA、PFDA、PFUnDA、PFHxS、PFOS 和 FOSA)在 pH 值依赖条件下于 11 种温带矿物土壤中的土壤水分分配情况,以及与土壤性质(如有机碳含量(0.2-3%)、铁和铝(氢)氧化物浓度和质地)的关系进行了研究。所有物质的 PFAS 吸附均与分子的全氟碳链长度呈正相关,与溶液 pH 值呈负相关。对于所有 PFAS,log K 与 pH 之间的负斜率随 PFAS 全氟碳链长度的增加而变得更加陡峭(r = 0.75,p ≤ 0.05)。除了 FOSA(r = 0.71)之外,有机碳(OC)单独作为所有 PFAS 分配的预测因子表现不佳,并且源自有机土壤材料的 OC 归一化 PFAS 分配低估了 PFAS 对土壤的吸附。多元线性回归表明,对于全氟辛烷磺酸(PFOS)和 FOSA,吸附的贡献(p ≤ 0.05)来自 OC,对于 PFOS、FOSA 和全氟癸酸(PFDA),吸附的贡献(p ≤ 0.05)来自铁/铝(氢)氧化物。FOSA 是唯一一种在所研究的物质中,其结合与土壤质地(粉土+粘土)之间存在统计学显著相关性的物质。为了预测 PFAS 的吸附,使用斯德哥尔摩腐殖质模型计算了所有土壤有机质部分的表面净电荷。当用腐殖质(Oe)物质的电荷依赖型 PFAS 吸附来校准时,所得到的模型显著低估了 11 种土壤中 10 种土壤的实测 K 值。总之,可能包括硅酸盐矿物在内的其他吸附剂可能有助于 PFAS 在土壤中的结合。需要开展更多的研究来开发能够准确预测土壤中 PFAS 吸附的地球化学模型。

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