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在空气-水界面处,多氟烷基物质介导的磷脂臭氧分解作用。

Ozonolysis of phospholipids at the air-water interface intervened by polyfluoroalkyl substances.

作者信息

Jiang Jie, Liu Yaqi, He Yuwei, Niu Yuqing, Wang Yanjie, Chen Yijing, Yang Yali, He Jing, Liu Zhuo, Jiang Yanxiao, Zhang Hong

机构信息

School of Marine Science and Technology, Harbin Institute of Technology at Weihai, Weihai, Shandong, 264209, PR China; State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin, Heilongjiang, 150090, PR China.

School of Marine Science and Technology, Harbin Institute of Technology at Weihai, Weihai, Shandong, 264209, PR China.

出版信息

Talanta. 2024 Aug 15;276:126278. doi: 10.1016/j.talanta.2024.126278. Epub 2024 May 17.

DOI:10.1016/j.talanta.2024.126278
PMID:38776776
Abstract

Perfluoroalkyl substances (PFASs) are ubiquitous in the environment and even accumulate in the human body associated with their excellent stability and persistence. However, the effect and reaction mechanism at the molecular level on the cell phospholipid peroxidation remained unclear. In this work, the interfacial reaction of model phospholipids (POPG) intervened by per- and polyfluoroalkyl substances (PFASs) at the air-water interface of a hanged droplet exposed to ozone (O) was investigated. Perfluorinated carboxylates and sulfonates were evaluated. Four-carbon PFASs promoted interfacial ozonolysis, but PFASs with longer carbon skeletons impeded this chemistry. A model concerning POPG packing was proposed and it was concluded that the interfacial chemistry was mediated by chain length rather than their functional groups. Four-carbon PFASs could couple into POPG ozonolysis by mainly reacting with aldehyde products along with minor Criegee intermediates, but this was not observed for longer PFASs. This is different from that condensed-phase Criegee intermediates preferred to reacting with per-fluoroalkyl carboxylic acids. These results provide insight into the adverse health of PFASs on cell peroxidation.

摘要

全氟烷基物质(PFASs)在环境中无处不在,由于其出色的稳定性和持久性,甚至会在人体中蓄积。然而,PFASs在分子水平上对细胞磷脂过氧化的影响及反应机制仍不清楚。在这项工作中,研究了全氟和多氟烷基物质(PFASs)干预下的模型磷脂(POPG)在暴露于臭氧(O)的悬滴气-水界面处的界面反应。对全氟羧酸盐和磺酸盐进行了评估。含四个碳的PFASs促进界面臭氧分解,但具有更长碳骨架的PFASs则阻碍了这种化学反应。提出了一个关于POPG堆积的模型,并得出结论:界面化学是由链长而非官能团介导的。含四个碳的PFASs主要通过与醛产物以及少量的Criegee中间体反应而参与到POPG的臭氧分解中,但对于更长链的PFASs则未观察到这种情况。这与凝聚相Criegee中间体更倾向于与全氟烷基羧酸反应不同。这些结果为PFASs对细胞过氧化的不良健康影响提供了见解。

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