PDF(Pubmed)
Abstract：
A growing number of studies have reported that routinely monitored per- and polyfluoroalkyl substances (PFAS) are not sufficient to explain the extractable organic fluorine (EOF) measured in human blood. In this study, we address this gap by screening pooled human serum collected over 3 decades (1986-2015) in Tromsø (Norway) for >5000 PFAS and >300 fluorinated pharmaceuticals. We combined multiple analytical techniques (direct infusion Fourier transform ion cyclotron resonance mass spectrometry, liquid chromatography-Orbitrap-high-resolution mass spectrometry, and total oxidizable precursors assay) in a three-step suspect screening process which aimed at unequivocal suspect identification. This approach uncovered the presence of one PFAS and eight fluorinated pharmaceuticals (including some metabolites) in human serum. While the PFAS suspect only accounted for 2-4% of the EOF, fluorinated pharmaceuticals accounted for 0-63% of the EOF, and their contribution increased in recent years. Although fluorinated pharmaceuticals often contain only 1-3 fluorine atoms, our results indicate that they can contribute significantly to the EOF. Indeed, the contribution from fluorinated pharmaceuticals allowed us to close the organofluorine mass balance in pooled serum from 2015, indicating a good understanding of organofluorine compounds in humans. However, a portion of the EOF in human serum from 1986 and 2007 still remained unexplained.
摘要：
越来越多的研究报告说，常规监测的全氟烷基和多氟烷基物质（PFAS）不足以解释人体血液中测量的可萃取有机氟（EOF）。在这项研究中,我们通过筛查在Tromsø(挪威)收集的超过30年(1986-2015年)的人类血清中>5000PFAS和>300种氟化药物来解决这一差距.我们结合了多种分析技术（直接输注傅里叶变换离子回旋共振质谱，液相色谱-Orbitrap-高分辨质谱,和总可氧化前体测定）在三步可疑筛选过程中，旨在明确可疑鉴定。这种方法揭示了人血清中一种PFAS和八种氟化药物(包括一些代谢物)的存在。虽然PFAS嫌疑人仅占EOF的2-4%，氟化药物占EOF的0-63%，近年来，他们的贡献有所增加。虽然氟化药物通常只含有1-3个氟原子，我们的结果表明，它们可以对EOF做出显著贡献。的确,氟化药物的贡献使我们能够从2015年起关闭合并血清中的有机氟质量平衡,这表明我们对人类中的有机氟化合物有很好的了解.然而,1986年和2007年人类血清中的部分EOF仍然无法解释.
