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An amine-functionalized olefin-linked covalent organic framework used for the solid-phase microextraction of legacy and emerging per- and polyfluoroalkyl substances in fish
Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2021-09-16 , DOI: 10.1016/j.jhazmat.2021.127226
Xin Song 1 , Rongyu Wang 1 , Xiao Wang 2 , Haoyue Han 1 , Zhaoyu Qiao 1 , Xiaowei Sun 1 , Wenhua Ji 2
Affiliation  

Due to the environmental persistence and various health problems associated with per- and polyfluoroalkyl substances (PFASs), they have come under increased public scrutiny. However, the efficient extraction of PFASs from complex media remains challenging. Herein, an olefin-linked covalent organic framework (COF-CN) has been prepared via a Knoevenagel condensation reaction, followed by reduction using LiAlH4 to form an amine-functionalized COF (COF-NH2). The characterization results demonstrated that the crystal structure was maintained during the post-modification step. Isothermal and kinetic adsorption studies showed the higher affinity of COF-NH2 toward PFASs. Based on density functional theory, the adsorption mechanism of the stable six-member-ring structure formed between COF-NH2 and PFASs via hydrogen bonding was tentatively revealed. After optimizing the solid-phase microextraction parameters, legacy and emerging PFASs were efficiently extracted from fish using the COF-NH2 coating, followed by detection using ultra-performance liquid chromatography-tandem mass spectrometry. The method exhibited ideal linearity, low limits of quantification, excellent precision, and high relative recoveries. Finally, the bioconcentration kinetics for goldfish was studied, which can provide a feasible platform for investigating the accumulate ion and toxicity of PFASs.



中文翻译:

一种胺官能化烯烃连接的共价有机框架,用于固相微萃取鱼类中遗留和新兴的全氟和多氟烷基物质

由于与全氟和多氟烷基物质 (PFAS) 相关的环境持久性和各种健康问题,它们受到了越来越多的公众审查。然而,从复杂介质中有效提取 PFAS 仍然具有挑战性。在此,通过Knoevenagel缩合反应制备了烯烃连接的共价有机骨架(COF-CN),然后使用LiAlH 4还原形成胺官能化COF(COF-NH 2)。表征结果表明,晶体结构在后改性步骤期间保持不变。等温和动力学吸附研究表明 COF-NH 2的亲和力更高PFASs。基于密度泛函理论,初步揭示了COF-NH 2与PFASs之间通过氢键形成的稳定六元环结构的吸附机理。在优化固相微萃取参数后,使用 COF-NH 2涂层从鱼类中高效提取传统和新兴 PFAS,然后使用超高效液相色谱-串联质谱进行检测。该方法具有理想的线性、低定量限、出色的精密度和较高的相对回收率。最后,研究了金鱼的生物富集动力学,为研究PFASs的累积离子和毒性提供了一个可行的平台。

更新日期:2021-09-20
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