Photochemical formation of water-soluble oxyPAHs, naphthenic acids, and other hydrocarbon oxidation products from Cook Inlet, Alaska crude oil and diesel in simulated seawater spills
Photochemical formation of water-soluble oxyPAHs, naphthenic acids, and other hydrocarbon oxidation products from Cook Inlet, Alaska crude oil and diesel in simulated seawater spills
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模拟海水泄漏中库克湾、阿拉斯加原油和柴油中水溶性多环芳烃、环烷酸和其他碳氢化合物氧化产物的光化学形成
DOI：
10.1039/d2va00325b
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发表时间：
2023
期刊：
影响因子：
--
通讯作者：
Tomco, Patrick L.
中科院分区：
文献类型：
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作者：
Harsha, Maxwell L.;Redman, Zachary C.;Wesolowski, Josh;Podgorski, David C.;Tomco, Patrick L.
由原油和柴油形成的碳氢化合物氧化产物 (HOP) 是在模拟阿拉斯加库克湾的环境条件下，在四个不同时期（1、4、7 和 10 天）的实验室模拟泄漏中形成的。进行了两组分析来识别和表征 HOP。进行的第一组分析是非靶向的，包括高分辨率质谱分析和荧光激发-发射矩阵光谱分析。液相色谱与 Orbitrap 质谱仪结合发现，库克湾 (CI) 原油和柴油中形成的 HOP 是相对还原的饱和和不饱和化合物。来自原油的 HOP 的分子组成更具芳香族性，而由柴油形成的 HOP 则更具脂肪族性。此外，还报道了 HOP 中环烷酸（一类有毒物质）的分子特征。通过荧光激发-发射矩阵光谱揭示了 HOP 的六种独特的化学特征，包括两种独特的石油特征。荧光激发-发射矩阵光谱的并行因子模型准确跟踪 HOP 的时间组成变化。第二组分析是有针对性的，包括使用串联质谱法对 HOP 中的多环芳烃 (PAH) 和氧化多环芳烃 (oxyPAH) 进行定量。对 CI 原油形成的 HOP 中的两种 oxyPAH、菲醌和 1,4-蒽醌进行了定量，并与 11 种 PAH 相关。这项研究的结果揭示了一种监测泄漏事件中碳氢化合物氧化产物成分变化的综合方法。
Hydrocarbon oxidation products (HOPs) formed from crude oil and diesel were formed from laboratory simulated spills at four different periods (1, 4, 7, and 10 days) under environmental conditions that mimicked those in Cook Inlet, Alaska. Two sets of analyses were performed to identify and characterize the HOPs. The first set of analyses performed was non-targeted and included high-resolution mass spectrometry and fluorescence excitation-emission matrix spectroscopy. Liquid chromatography coupled with an Orbitrap mass spectrometer uncovered that HOPs formed from Cook Inlet (CI) crude oil and diesel are relatively reduced, saturated, and unsaturated compounds. The molecular compositions of HOPs from crude oil are more aromatic, whereas those formed from diesel are more aliphatic. Moreover, molecular signatures of naphthenic acids, a class of toxicants, in HOPs are reported. Six unique chemical features of HOPs were revealed by fluorescence excitation-emission matrix spectroscopy, including two unique petroleum signatures. The parallel factor model for fluorescence excitation-emission matrix spectroscopy accurately tracks temporal compositional changes of HOPs. The second set of analyses was targeted and included the quantification of polycyclic aromatic hydrocarbons (PAHs) and oxygenated polycyclic aromatic hydrocarbons (oxyPAHs) in HOPs using tandem mass spectrometry. Two oxyPAHs, phenanthrenequinone, and 1,4-anthraquinone were quantified in HOPs formed from CI crude oil and related to eleven PAHs. The results from this study uncover a comprehensive approach to monitoring compositional changes of hydrocarbon oxidation products in a spill event.