Thermal analysis and ion mobility coupled to high-resolution mass spectrometry for organic aerosol characterization

人为空气污染使环境暴露于大量有机污染物，对健康和气候造成严重影响。罗斯托克大学（德国）和鲁昂-诺曼底大学（法国）计划开展为期三年的合作，主要目的是开发一套与最先进的质谱（MS）相结合的演化气体分析（EGA）技术一级和二级有机气溶胶的详细化学描述平台。在这方面，高分辨率MS的共享专业知识将使傅里叶变换离子回旋共振（FT-ICR）和高分辨率飞行时间MS成为中心分析平台，并允许分子水平的见解。三种主要的EGA方法将用于联用：大气固体分析探针（ASAP/DIP），热光碳分析仪（TOCA）和气相色谱（GC）。重要的离子迁移谱（IMS）将作为一种额外的分离技术，用于分离演化成分的大小和形状。来自不同方法的信息旨在实现三个主要成就：1）对有机气溶胶异构复杂性的认识，2）在分子水平上描述化学部分，3）初级排放物和化学反应形成的排放物的化学比较（二次老化气溶胶）。通过GC保留时间、选择性电离技术（例如，靶向芳族物质的光电离）、裂解模式（通过ASAP和串联质谱法）和离子迁移率响应。为此目的，将制定适当的数据处理策略，其中包括碰撞截面的理论计算，最后，这将使我们能够建立一个不同类型气溶胶源的分子库，特别侧重于航运排放。预计该分子库将适合于将人类健康方面联系起来，或有助于了解颗粒物对气候的各自影响。

Anthropogenic air pollution exposes the environment to a large number of organic contaminants with severe health and climate impacts. The major impact on humankind and the tremendous molecular complexity of organic aerosols motivates the development of novel analytical instrumentation approaches.The envisioned three-year corporate effort between the University of Rostock (Germany) and the University of Rouen-Normandy (France) primary aims to develop a set of evolved gas analysis (EGA) techniques coupled to state-of-the-art mass spectrometry (MS) platforms for the detailed chemical description of primary and secondary organic aerosols. In this respect, the shared expertise in high-resolution MS will make Fourier-transform ion cyclotron resonance (FT-ICR) and high-resolution time-of-flight MS the central analytical platforms and allow for molecular-level insights. Three main EGA approaches will be utilized for hyphenation: Atmospheric solids analysis probe (ASAP/DIP), thermal-optical carbon analyzer (TOCA), and gas chromatography (GC). Vital, ion mobility spectrometry (IMS) will serve as an additional separation technique for size and shape of the evolved constituents.The information from the different approaches aims to reach three main achievements: 1) insights into the isomeric complexity of organic aerosols, 2) description of the chemical moieties at the molecular level, and 3) chemical comparison of primary emissions and those formed by chemical reactions (secondary, aged aerosols). Structural information is gained by the combination of GC retention time, selective ionization techniques (e.g., photoionization targeting aromatic species), fragmentation pattern (both by ASAP and tandem mass spectrometry), and ion mobility response. For this purpose, adapted data processing strategies will be developed, among others, including the theoretical computation of collision cross-sections (CCS).Finally, this will allow us to set up a molecular repository for different types of aerosol sources, with a particular focus on shipping emissions. This molecular library is foreseen to be suitable to link human health aspects or to contribute to the understanding of the respective climate influence of particulate matter.