Oil Photooxidation by Sunlight: Role of Reactive Species in the Transformation of Saturated and Aromatic Hydrocarbons

在NSF化学部环境化学科学计划的支持下，毕格罗海洋科学实验室的Christoph Aeppli将研究阳光介导的石油碳氢化合物转化机制。这是相关的，因为光氧化影响海洋溢油后石油的命运，从而从根本上改变石油残留物的性质，成分和环境命运。该项目将通过进行一系列的实验室辐照实验来提高对石油光化学机理的理解。该项目预期的知识和数据将改善溢油风险和损害评估。本项目还将培养一名博士后研究员和一名本科生。此外，该项目的结果和方法将在本科课程中实施，并且该项目的成果将通过外展计划传达给更广泛的社区。要阐明饱和化合物降解的相关途径在具有多个共存竞争途径的复杂混合物中具有挑战性。这个项目将使用一个逐步的方法与系统，有三个层次的复杂性。首先，基本的机械问题将首先解决使用模型油组成的一个明确的混合烃。其次，各种光化学途径将系统地测试这些模型化合物使用天然存在于石油中的敏化剂和猝灭剂。最后，所获得的知识将被应用到复杂的石油混合物中发生的复杂过程，目的是构建一个一般的概念机制，相关的石油光降解过程中的各种饱和烃和芳烃的石油。该项目将采用一种基于二维气相色谱的创新方法，用于石油降解的全面量化，并将开发定量方法来测量石油光产物的形成。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

With support from the Environmental Chemical Sciences Program in the Division of Chemistry at NSF, Christoph Aeppli at the Bigelow Laboratory for Ocean Sciences will investigate the mechanism of sunlight-mediated transformation of oil hydrocarbons. This is relevant since photooxidation affects the fate of oil after marine spills, thereby fundamentally altering the properties, composition, and environmental fate of oil residues. This project will improve the mechanistic understanding of oil photochemistry by conducting a series of laboratory irradiation experiments. The knowledge and data expected from this project will improve oil spill risk and damage assessment. This project will also train a postdoctoral researcher and undergraduate students. Furthermore, results and methods from this project will be implemented in undergraduate coursework, and outcomes of this project will be communicated to the broader community through outreach programs.To elucidate the relevant pathway for the degradation of saturated compounds is challenging in the complex mixture of oil with multiple co-occurring competing pathways. This project will use a step-wise approach with systems that have three levels of complexity. First, basic mechanist questions will first be addressed using a model oil consisting of a well-defined mixture of hydrocarbons. Second, various photochemical pathways will be systematically tested on these model compounds using sensitizers and quenchers naturally occurring in petroleum. Lastly, the gained knowledge will then be applied to the complex processes occurring in the complex mixture of petroleum, with the aim to construct a general conceptual mechanism of relevant oil photodegradation processes of the various saturated and aromatic hydrocarbons in oil. This project will employ an innovative method based on two-dimensional gas chromatography for the comprehensive quantification of oil degradation and will develop quantitative methods to measure the formation of oil photoproducts.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.