Key Laboratory of Integrated Regulation and Resource Development on Shallow Lakes, Ministry of Education, College of Environment, Hohai University, Nanjing 210098, PR China; Yangtze Institute for Conservation and Development, Hohai University, Nanjing 210098, PR China.
Key Laboratory of Integrated Regulation and Resource Development on Shallow Lakes, Ministry of Education, College of Environment, Hohai University, Nanjing 210098, PR China; Yangtze Institute for Conservation and Development, Hohai University, Nanjing 210098, PR China.
Sci Total Environ. 2024 Nov 20;952:175997. doi: 10.1016/j.scitotenv.2024.175997. Epub 2024 Sep 2.
Solving the challenges faced during the measurement of the cross-interface transfer of perfluoroalkyl acids (PFAAs) in lakes is crucial for clarifying environmental behaviours of these chemicals and their efficient governance. This study developed a multimedia fugacity model based on the quantitative water-air-sediment interaction (QWASI) covering abiotic/biotic matrices to investigate the cross-interface transfer and fate of PFAAs in Luoma Lake, a typical PFAA-contaminated shallow lake in eastern China. The accuracy and reliability of the established model were confirmed using Percent bias and Monte Carlo simulation, respectively. Using the QWASI model, the multimedia transfer of the PFAAs and their accumulation and persistence in different sub-compartments were described and measured, and the differences among individual PFAAs were explored. The simulation results showed that the sedimentation and resuspension of PFAAs were the most intense cross-interfacial transfers, and the sediments served as a chemical sink in the long term. A significant negative correlation of N (the number of CF bonds) with the relative outflow flux (T) but a positive correlation with the relative net transfer across the interface between water and aquatic plants (T) was detected, indicating that the PFAA migration capacity decreased but the bioaccumulation potential increased with the CF bond number. The persistence in water (P) of individual PFAAs ranged from 19.65d (PFOA) to 32.22d (PFOS), with an average of 26.15d; their persistence in sediment (P) ranged from 432d (PFBA) to 3216d (PFOS), with an average of 1524d, increasing linearly with an increase in N. The water advection flows into and out of the lake (Q and Q), the PFAA concentration of water inflow (C), and bioconcentration factor of aquatic plants (BCF) were the primary parameters sensitive to PFAAs in all sub-compartments, which are essential indexes for exploring promising remediation pathways for lacustrine PFAA contamination based on the fugacity model simulation.
解决湖泊中全氟烷基酸 (PFAAs) 界面迁移测量所面临的挑战对于阐明这些化学物质的环境行为及其有效治理至关重要。本研究开发了一种基于定量水-气-沉积物相互作用 (QWASI) 的多介质逸度模型，涵盖了非生物/生物矩阵，以调查中国东部典型 PFAAs 污染浅水湖——骆马湖中 PFAAs 的界面迁移和归宿。分别采用百分偏差和蒙特卡罗模拟验证了所建立模型的准确性和可靠性。利用 QWASI 模型，描述并测量了 PFAAs 的多介质迁移及其在不同亚区的积累和持久性，并探讨了各个 PFAAs 之间的差异。模拟结果表明，PFAAs 的沉降和再悬浮是最强烈的界面间迁移，沉积物在长期内充当了化学汇。发现 N（CF 键数）与相对流出通量（T）呈显著负相关，与水和水生植物界面间的净转移相对通量（T）呈显著正相关，表明 PFAA 的迁移能力随 CF 键数的增加而降低，但生物积累潜力增加。各 PFAAs 在水中的持久性（P）范围为 19.65d（PFOA）至 32.22d（PFOS），平均为 26.15d；在沉积物中的持久性（P）范围为 432d（PFBA）至 3216d（PFOS），平均为 1524d，随 N 的增加呈线性增加。湖水的水流入流（Q 和 Q）、入水的 PFAAs 浓度（C）和水生植物的生物浓缩系数（BCF）是所有亚区中对 PFAAs 敏感的主要参数，是基于逸度模型模拟探索有前景的湖泊 PFAAs 污染修复途径的重要指标。
