Investigation of the effects of transport infrastructure upon the environment using ultrahigh resolution mass spectrometry

沥青道路在经济和社会发展中发挥着关键作用，而经济和社会发展是地球仪不断增长的城市化的基石。英国有一个约40万公里的铺设道路网络，其中含有来自原油和/或煤炭蒸馏的沥青，这些沥青可能含有对环境有害的有机化合物。虽然在土壤和沉积物调查中测量了常见的有机污染物，如多环芳烃（PAH），但缺乏有关道路及其对周围城市土壤和沉积物影响的知识。这部分是因为其主要有机成分，即饱和烃和芳烃、沥青质和树脂的确切化学组成因原油来源和所用的精炼/蒸馏工艺而异。这些特征和变化也阻碍了我们真正理解这些化合物类的存在所导致的潜在毒性效应的能力。迫切需要改进环境监测方法，特别是在了解高度复杂样品的化学性质方面。超高分辨率质谱法，如傅里叶变换离子回旋共振质谱法（FTICR MS），是一种最先进的分析方法，在复杂混合物的现代表征中发挥着主导作用。该技术产生复杂的数据集，随后作为有机成分的分子“概况”或“指纹”。样品的详细分子表征，通常包括数万种有机成分，可以使用各种方法进行处理，可视化和比较。与统计部的合作还大大改进了复杂数据集的处理和与商业数据分析软件一起使用的内部软件的制作。最近与英国地质调查局合作的一个例子是对斯塔滕岛（美国）土壤芯的研究，对不同深度土壤的分析提供了该地区石油污染的化学历史。该博士旨在使用最先进的方法来模拟环境中的过程，并表征真实的世界样本，以更深入地了解英国道路对环境的影响。

Bitumen roadways play a critical role in the economic and social development that is the corner stone of ever-increasing urbanisation across the globe. The UK has a network of about 400,000 km paved roads containing bitumen sourced from the distillation of crude oil and or coals which can contain environmentally harmful organic compounds. Whilst common organic pollutants such as polyaromatic hydrocarbons (PAH) are measured in soil and sediment surveys there is a lack of knowledge concerning roadways and their impact on surrounding urban soils and sediments. This partly stems from the fact that the precise chemical composition of its principal organic constituents, namely, saturated and aromatic hydrocarbons, asphaltenes and resins varies depending on the source crude oil and refining/distillation process used. These characteristics and variations also hinder our ability to truly comprehend the potential for toxic effects resulting from the presence of these compound classes.There is a strong need for improved methodologies for environmental monitoring, particularly with respect to understanding the chemistry of highly complex samples. Ultrahigh resolution mass spectrometry, such as Fourier transform ion cyclotron resonance mass spectrometry (FTICR MS), is a state-of-the-art analytical method which has been playing a leading role in the modern characterization of complex mixtures. The technique produces complex data sets which subsequently serve as molecular "profiles" or "fingerprints" of the organic components. The detailed molecular characterization of samples, typically including tens of thousands of organic compositions, can be processed, visualized, and compared using a variety of methods. Collaboration with the Department of Statistics has also resulted in significantly improved processing of complex data sets and the production of in-house software, used in conjunction with commercial data analysis software. A recent example of collaboration with the British Geological Survey has included a study of soil cores from Staten Island (USA), where analysis of soil from varying depths provides a chemical history of oil contamination in the region. This PhD seeks to use state-of-the-art methods to model processes in the environment and to characterize real world samples to gain greater insights into the impact of UK roadways upon the environment.