Multicomponent and Surface Charge Effects on PFOS Sorption and Transport in Goethite-Coated Porous Media under Variable Hydrochemical Conditions,Environmental Science & Technology

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Multicomponent and Surface Charge Effects on PFOS Sorption and Transport in Goethite-Coated Porous Media under Variable Hydrochemical Conditions
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2024-07-22 , DOI: 10.1021/acs.est.4c02164
Jacopo Cogorno _{1,

2} , Massimo Rolle _{1,

3}

Affiliation

Perfluorooctanesulfonate (PFOS), a toxic anionic perfluorinated surfactant, exhibits variable electrostatic adsorption mechanisms on charge-regulated minerals depending on solution hydrochemistry. This work explores the interplay of multicomponent interactions and surface charge effects on PFOS adsorption to goethite surfaces under flow-through conditions. We conducted a series of column experiments in saturated goethite-coated porous media subjected to dynamic hydrochemical conditions triggered by step changes in the electrolyte concentration of the injected solutions. Measurements of pH and PFOS breakthrough curves at the outlet allowed tracking the propagation of multicomponent reactive fronts. We performed process-based reactive transport simulations incorporating a mechanistic network of surface complexation reactions to quantitatively interpret the geochemical processes. The experimental and modeling outcomes reveal that the coupled spatio-temporal evolution of pH and electrolyte fronts, driven by the electrostatic properties of the mineral, exerts a key control on PFOS mobility by determining its adsorption and speciation reactions on goethite surfaces. These results illuminate the important influence of multicomponent transport processes and surface charge effects on PFOS mobility, emphasizing the need for mechanistic adsorption models in reactive transport simulations of ionizable PFAS compounds to determine their environmental fate and to perform accurate risk assessment.

中文翻译：

多组分和表面电荷对可变水化学条件下针铁矿涂层多孔介质中全氟辛烷磺酸吸附和传输的影响

全氟辛烷磺酸 (PFOS) 是一种有毒的阴离子全氟化表面活性剂，根据溶液水化学，对电荷调节矿物质表现出不同的静电吸附机制。这项工作探讨了流过条件下多组分相互作用和表面电荷效应对全氟辛烷磺酸在针铁矿表面吸附的相互作用。我们在饱和针铁矿涂层多孔介质中进行了一系列柱实验，该介质受到由注入溶液的电解质浓度阶跃变化触发的动态水化学条件的影响。在出口处测量 pH 和 PFOS 突破曲线可以跟踪多组分反应前沿的传播。我们进行了基于过程的反应输运模拟，结合了表面络合反应的机械网络，以定量解释地球化学过程。实验和建模结果表明，在矿物静电特性的驱动下，pH 值和电解质前沿的耦合时空演化通过确定其在针铁矿表面的吸附和形态反应，对 PFOS 的迁移率发挥关键控制作用。这些结果阐明了多组分传输过程和表面电荷效应对 PFOS 迁移率的重要影响，强调了在可电离 PFAS 化合物的反应传输模拟中需要机械吸附模型来确定其环境归宿并进行准确的风险评估。

更新日期：2024-07-22

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