Abstract In response to the Deepwater Horizon oil spill, critical research has tracked the changes in petroleum hydrocarbons with environmental weathering. There are limitations, however, whereby single analytical techniques cannot always identify the wide breadth of petroleum and petroleum-derived compounds. We explore the analytical capabilities of ramped pyrolysis-gas chromatography–mass spectrometry (Py-GC–MS) to evaluate environmental samples of petroleum hydrocarbons from the Deepwater Horizon oil spill. We show that bulk flow Py-GC–MS can quantify the overall degree of petroleum hydrocarbon weathering. Furthermore, thermal slicing Py-GC–MS can quantify specific compounds in the “thermal desorption zone” (50–370 °C), as well as characterize pyrolyzed fragments from non-GC-amenable petroleum hydrocarbons (including oxygenated hydrocarbons) in the “cracking zone” (370–650 °C). Our data also suggest an increase in thermochemical stability, concentration of oxygenated products and complexity of high molecular weight and/or polar components with advanced weathering. This analysis not only elucidates weathering trends in Deepwater Horizon oil over several years, but also illustrates the analytical capacity of this method for future petroleum hydrocarbon investigations, filling a void in research connecting Py-GC–MS and environmentally weathered oil samples.

中文翻译：

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使用梯度热解-气相色谱-质谱法分析环境石油污染

摘要 针对深水地平线漏油事件，批判性研究追踪了石油碳氢化合物随环境风化的变化。然而，存在局限性，单一分析技术无法始终识别广泛的石油和石油衍生化合物。我们探索了梯度热解-气相色谱-质谱 (Py-GC-MS) 的分析能力，以评估来自深水地平线石油泄漏的石油烃的环境样品。我们表明，大流量 Py-GC-MS 可以量化石油烃风化的整体程度。此外，热切片 Py-GC-MS 可以量化“热解吸区”（50-370 °C）中的特定化合物，以及在“裂化区”（370–650 °C）中表征来自非 GC 适合的石油烃（包括含氧烃）的热解碎片。我们的数据还表明热化学稳定性、氧化产物的浓度和高分子量和/或极性组分的复杂性增加，具有先进的风化。该分析不仅阐明了深水地平线石油多年来的风化趋势，而且说明了该方法对未来石油烃研究的分析能力，填补了将 Py-GC-MS 与环境风化油样品联系起来的研究空白。含氧产品的浓度和高分子量和/或具有高级风化的极性组分的复杂性。该分析不仅阐明了深水地平线石油多年来的风化趋势，而且说明了该方法对未来石油烃研究的分析能力，填补了将 Py-GC-MS 与环境风化油样品联系起来的研究空白。含氧产品的浓度和高分子量和/或具有高级风化的极性组分的复杂性。该分析不仅阐明了深水地平线石油多年来的风化趋势，而且说明了该方法对未来石油烃研究的分析能力，填补了将 Py-GC-MS 与环境风化油样品联系起来的研究空白。