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中，对健康和气候造成严重影响。对人类的重大影响和有机气溶胶的巨大分子复杂性激发了新型分析仪器方法的发展。罗斯托克大学（德国）和鲁昂-诺曼底大学（法国）之间的合作计划为期三年，主要目的是开发一套与最先进的质谱分析（MS）平台相结合的进化气体分析（EGA）技术，用于对初级和次级有机气溶胶进行详细的化学描述。在这方面，高分辨率质谱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质谱成为中心分析平台，并允许分子水平的见解。三种主要的EGA方法将用于分离：大气固体分析探针（ASAP/DIP），热光学碳分析仪（TOCA）和气相色谱法（GC）。至关重要的是，离子迁移谱法（IMS）将作为一种额外的分离技术，用于进化成分的大小和形状。来自不同方法的信息旨在达到三个主要成就：1)洞察有机气溶胶的异构体复杂性，2)描述分子水平上的化学部分，以及3)初级排放物和化学反应形成的排放物（次级，老化的气溶胶）的化学比较。结构信息是通过GC保留时间、选择性电离技术（例如，针对芳香物质的光电离）、碎片模式（ASAP和串联质谱）和离子迁移率响应的组合获得的。为此，将开发适应的数据处理策略，其中包括碰撞横截面（CCS）的理论计算。最后，这将使我们能够为不同类型的气溶胶源建立一个分子储存库，特别关注航运排放。预计这一分子文库适合于将人类健康方面联系起来，或有助于了解颗粒物质各自对气候的影响。

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.