EAGER: Inexpensive and Rapid Detection of Per- and Polyfluoalkyl Substances in Drinking Water Supplies Using Macrocycle-Functionalized Gold Nanoparticles

全氟和多氟烷基物质(PFAS)由4,000多种合成化学品组成，用于制造各种产品，包括不粘锅、食品包装和灭火泡沫。全氟辛烷磺酸通常被称为“永久化学品”，因为它们一旦释放到环境中就极难分解和持久存在。全氟辛烷磺酸因其毒性、移动性以及在环境介质(如土壤和水)以及生物和植物中的高蓄积性，已成为人类和生态系统健康所关注的污染物。人类接触全氟辛烷磺酸的主要途径之一是饮用自来水。然而，目前用于测量水中全氟辛烷磺酸浓度的分析分析和工具(例如，样品预浓缩，然后进行液相色谱和质谱分析)昂贵、耗时，而且仅限于专业实验室。这个高风险、高回报的急切项目的目标是开发一种新的分析工具，基于新的表面增强拉曼光谱(SERS)平台，用于水样中全氟辛烷磺酸的廉价快速检测和定量。该项目的成功完成可能导致开发和验证一种快速、成本效益高和更有效的分析工具，以检测和量化饮用水水源中的全氟辛烷磺酸。将通过学生教育和培训进一步造福社会，包括指导一名博士生和两名本科生。由于摄入饮用水而长期接触全氟辛烷磺酸已成为一个全球健康问题。这个高风险、高回报、急切渴望的项目的首要目标是开发一种廉价和可靠的方法来量化饮用水中的全氟辛烷磺酸。为了推进这一目标，首席研究人员(PI)建议利用和整合等离子体和超分子化学的最新进展：1)从水样中提取PFAS分子并将其浓缩到固定在细菌纤维素(BC)基质中的大环(MC)功能化金(Au)纳米颗粒(NP)上，以及2)使用激光激发负载PFAS的MC功能化Au纳米颗粒以产生热点归一化表面增强拉曼光谱。收集的拉曼光谱随后由光学光谱仪进行分析，以识别提取的PFAS分子并估计其在测试水样中的浓度。为了验证他们的新分析方法，私人投资机构建议在与环境有关的条件下，包括在存在溶解有机物的情况下，研究全氟辛烷磺酸的检测和定量。该项目的成功完成可能导致开发一种紧凑和模块化的装置，用于饮用水供应中快速和现场的全氟辛烷磺酸定量。最终，PIs希望他们的新分析方法能够改变目前政府和行业用来监测PFAS对饮用水水源污染的基于液相色谱-串联质谱仪的范例。这一奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

Per- and polyfluoroalkyl substances (PFAS) consist of over 4,000 synthetic chemicals that are used in the manufacturing of a variety products including non-stick cookware, food wrappers, and fire-fighting foams. PFAS are commonly referred to as "forever chemicals" because they are extremely difficult to break down and become persistent once released into the environment. PFAS have emerged as contaminants of great concern for human and ecosystem health due to their toxicity, mobility, and high tendency to accumulate in environmental media (e.g., soils and water) and living organisms and plants. One of the major routes for human exposure to PFAS is via the ingestion of drinking tap water. However, current analytical assays and tools used to measure PFAS concentrations in water (e.g., sample preconcentration followed by liquid chromatography and mass spectrometry) are expensive, time-consuming, and restricted to specialized laboratories. The goal of this high-risk high-reward EAGER project is to develop a novel analytical tool for the inexpensive and rapid detection and quantification of PFAS in water samples based on a new Surface Enhanced Raman Spectroscopy (SERS) platform. The successful completion this project could lead to the development and validation of a rapid, cost effective and more efficient analytical tool to detect and quantify PFAS in drinking water sources. Further benefits to society will be achieved through student education and training including the mentoring of one doctoral student and two undergraduate students.Chronic exposure to PFAS through the ingestion of drinking water has become a global health concern. The overarching goal of this high-risk high-reward EAGER project is to develop an inexpensive and robust method to quantify PFAS in drinking water. To advance this goal, the Principal Investigators (PIs) propose to leverage and integrate recent advances in plasmonics and supramolecular chemistry to 1) extract and concentrate PFAS molecules from water samples onto macrocycles (MCs) functionalized gold (Au) nanoparticles (NPs) immobilized within a bacterial cellulose (BC) matrix, and 2) use laser illumination to excite the PFAS laden MC functionalized Au NPs to generate hot-spot normalized surface-enhanced Raman spectra. The collected Raman spectra are subsequently analyzed by an optical spectrometer to identify the extracted PFAS molecules and estimate their concentration in the tested water samples. To validate their new analytical method, the PIs propose to investigate PFAS detection and quantification under environmentally relevant conditions including in the presence of dissolved organic matter. The successful completion of this project could lead to the development of a compact and modular device for rapid and onsite PFAS quantification in drinking water supplies. Ultimately, the PIs hope that their new analytic approach could shift the liquid chromatography-tandem mass spectrometry-based paradigm currently used by government and industry to monitor the contamination of drinking water sources by PFAS.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.