Nanoelectrochemistry Reveals Selective Interactions of Perfluoroalkyl Substances (PFASs) with Silver Nanoparticles
Nanoelectrochemistry Reveals Selective Interactions of Perfluoroalkyl Substances (PFASs) with Silver Nanoparticles
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DOI：
10.1002/anie.202209164
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发表时间：
2022-08-03
影响因子：
16.6
通讯作者：
Andreescu, Silvana
中科院分区：
文献类型：
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作者：
Khan, Reem;Andreescu, Daniel;Andreescu, Silvana
纳米电化学可以研究全氟烷基物质和多氟烷基物质 (PFAS) 与银纳米颗粒 (AgNP) 的相互作用，并以高灵敏度阐明 PFAS 与纳米级表面的结合行为。单粒子碰撞电化学 (SPCE)、光谱和密度泛函理论 (DFT) 计算支持的机理研究表明，多氟辛烷磺酸 (PFOS)（一种代表性的 PFAS）具有选择性结合和诱导 AgNP 聚集的能力。单颗粒测量可识别通过颗粒间 F-F 相互作用以及 PFOS 磺酸盐选择性替代柠檬酸盐稳定剂形成的“离散”AgNP 团聚体（例如 2-3 个 NP）。这种相互作用仅是长链 PFAS (-SO3-) 的特征，提供了一种选择性识别低至 ppt 水平的这些物质的方法。测量和了解 PFAS 在纳米级表面的相互作用对于设计超灵敏的检测方法以及建模和预测它们在环境中的相互作用至关重要。
Nanoelectrochemistry allows for the investigation of the interaction of per- and polyfluoroalkyl substances (PFASs) with silver nanoparticles (AgNPs) and the elucidation of the binding behaviour of PFASs to nanoscale surfaces with high sensitivity. Mechanistic studies supported by single particle collision electrochemistry (SPCE), spectroscopic and density functional theory (DFT) calculations indicate the capability of polyfluorooctane sulfonic acid (PFOS), a representative PFAS, to selectively bind and induce aggregation of AgNPs. Single-particle measurements provide identification of the "discrete" AgNPs agglomeration (e.g. 2-3 NPs) formed through the inter-particles F-F interactions and the selective replacement of the citrate stabilizer by the sulfonate of the PFOS. Such interactions are characteristic only for long chain PFAS (-SO3-) providing a means to selectively identify these substances down to ppt levels. Measuring and understanding the interactions of PFAS at nanoscale surfaces are crucial for designing ultrasensitive methods for detection and for modelling and predicting their interaction in the environment.