Fosella Joseph, Ceja-Vega Jasmin, Rabadi Amani, Panella Micaela, Said Jessica, Perla Wilber, Poust Christopher, Herrera Mary, Lee Sunghee
Department of Chemistry and Biochemistry, Iona University, 715 North Avenue, New Rochelle, New York 10801, United States.
J Phys Chem B. 2025 Aug 7;129(31):7951-7963. doi: 10.1021/acs.jpcb.5c02472. Epub 2025 Jul 28.
There has been a rising concern about negative impacts of per- and polyfluoroalkyl substances (PFAS) on human and environmental health, given the environmental persistence and bioaccumulation potential of PFAS. In this study, two exemplary PFAS, a long-chain perfluorooctanoic acid (PFOA) and a short-chain alternative perfluorobutanesulfonic acid (PFBS), are investigated to assess their potential to modify bilayers of model membranes formed from 1,2-dioleoyl--glycero-3-phosphocholine (DOPC). A comprehensive suite of experimental techniques, including water permeability assays, thermal phase behavior analysis (DSC), vibrational spectroscopy (Raman and ATR-FTIR), and evaluations of interfacial properties, reveals concentration-dependent perturbations to DOPC membranes. Water permeability measurements reveal biphasic characteristics in PFAS-membrane interactions, corroborated by phase separation observed via DSC. PFOA and PFBS exhibit distinct impacts on membrane properties, reflecting a sensitivity to PFAS molecular structures. Higher membrane/water partition coefficients for PFOA underscore the role of hydrophobic effect in long- versus short-chain PFAS interactions. PFOA demonstrates a more pronounced effect than PFBS at lower concentrations, but they both exhibit similar impacts on DOPC membranes at higher levels. Notably, PFBS's significant membrane modifications at high concentrations challenge the assumption that shorter-chain PFAS alternatives are inherently safer. These findings highlight the complex nature of PFAS-membrane interactions and emphasize the importance of molecular structure in assessing environmental and health impacts.
鉴于全氟和多氟烷基物质（PFAS）在环境中的持久性和生物累积潜力，人们越来越关注其对人类和环境健康的负面影响。在本研究中，对两种典型的PFAS，即长链全氟辛酸（PFOA）和短链替代物全氟丁烷磺酸（PFBS）进行了研究，以评估它们改变由1,2-二油酰基-sn-甘油-3-磷酸胆碱（DOPC）形成的模型膜双层的潜力。一套综合的实验技术，包括水渗透性测定、热相行为分析（DSC）、振动光谱（拉曼和衰减全反射傅里叶变换红外光谱）以及界面性质评估，揭示了PFAS对DOPC膜的浓度依赖性扰动。水渗透性测量揭示了PFAS与膜相互作用中的双相特征，并通过DSC观察到的相分离得到证实。PFOA和PFBS对膜性质表现出不同的影响，反映了对PFAS分子结构的敏感性。PFOA较高的膜/水分配系数突出了疏水效应在长链与短链PFAS相互作用中的作用。在较低浓度下，PFOA比PFBS表现出更明显的影响，但在较高浓度下，它们对DOPC膜都表现出相似的影响。值得注意的是，PFBS在高浓度下对膜的显著修饰挑战了短链PFAS替代物本质上更安全的假设。这些发现突出了PFAS与膜相互作用的复杂性，并强调了分子结构在评估环境和健康影响中的重要性。
