School of Environmental & Municipal Engineering, Qingdao University of Technology, Qingdao 266033, China.
School of Environmental & Municipal Engineering, Qingdao University of Technology, Qingdao 266033, China.
J Hazard Mater. 2023 Jan 15;442:130125. doi: 10.1016/j.jhazmat.2022.130125. Epub 2022 Oct 4.
Novel per- and polyfluoroalkyl substances (PFASs) raise global concerns due to their toxic effects on environment and human health. However, researches on analytical methods of novel PFASs are lacking. Here, a kind of selective cationic covalent organic framework (iCOF) was designed and loaded on the surface of cotton as an adsorbent. Then, a simple solid-phase extraction (SPE) method based on the cotton@iCOF was developed for high throughput rapid extraction of six novel PFASs in water samples, coupled with ultrahigh-performance liquid chromatography-tandem mass spectrometry (UHPLC-MS/MS) determination. Several important SPE parameters, such as the amount of iCOF, sample pH, desorption conditions and salinity were systematically investigated. Under optimal conditions, the limits of detection and quantification of this SPE-UHPLC-MS/MS method were as low as 0.08-2.14 ng/L and 0.28-7.15 ng/L, respectively. The recoveries were 77.9-117.6 % for the tap water and surface water, and F-53 B in surface water were detected. Notably, this SPE process was rapid (1 h for 500 mL water sample) compared with commercial SPE (normal 2-3 h), owing to little resistance of cotton@iCOF and omission of nitrogen blowing process, and high throughput with 12 samples concurrently extracted. Additionally, various characterization means and density functional theory (DFT) calculations showed that ion-exchange effect, hydrophobic interaction, hydrogen bonding and ordered channel structure synergistically contributed to the PFASs adsorption on cotton@iCOF. The cotton@iCOF-based SPE method with simplicity, rapidity, selectivity and efficiency provided new research ideas for the analysis and control of ionic emerging pollutants in water.
新型全氟和多氟烷基物质（PFASs）因其对环境和人类健康的毒性影响而引起全球关注。然而，新型 PFASs 的分析方法研究还很缺乏。本研究设计了一种选择性的阳离子共价有机框架（iCOF），并将其负载在棉花表面作为吸附剂。然后，基于棉花@iCOF 建立了一种简单的固相萃取（SPE）方法，用于高通量快速提取水样中的六种新型 PFASs，并用超高效液相色谱-串联质谱（UHPLC-MS/MS）进行测定。系统研究了几个重要的 SPE 参数，如 iCOF 的用量、样品 pH 值、洗脱条件和盐度等。在最佳条件下，该 SPE-UHPLC-MS/MS 方法的检测限和定量限分别低至 0.08-2.14 ng/L 和 0.28-7.15 ng/L。自来水中和地表水中的回收率为 77.9-117.6%，并在地表水中检测到 F-53B。值得注意的是，与商业 SPE（通常为 2-3 小时）相比，这种 SPE 过程非常快速（500 mL 水样 1 小时），这是由于棉花@iCOF 的阻力小且省略了氮气吹脱过程，并且具有高通量的特点，可同时提取 12 个样本。此外，各种表征手段和密度泛函理论（DFT）计算表明，离子交换作用、疏水相互作用、氢键和有序通道结构协同作用促进了 PFASs 在棉花@iCOF 上的吸附。基于棉花@iCOF 的 SPE 方法具有简单、快速、选择性和高效的特点，为水中离子型新兴污染物的分析和控制提供了新的研究思路。
