Characterisation of ship diesel primary particulate matter at the molecular level by means of ultra-high-resolution mass spectrometry coupled to laser desorption ionisation—comparison of feed fuel, filter extracts and direct particle measurements
Characterisation of ship diesel primary particulate matter at the molecular level by means of ultra-high-resolution mass spectrometry coupled to laser desorption ionisation—comparison of feed fuel, filter extracts and direct particle measurements
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DOI：
10.1007/s00216-014-8408-1
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发表时间：
2015-01
影响因子：
4.3
通讯作者：
C. Rüger;M. Sklorz;Theo Schwemer;R. Zimmermann
中科院分区：
文献类型：
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作者：
C. Rüger;M. Sklorz;Theo Schwemer;R. Zimmermann
本研究应用正模激光解吸-电离超高分辨率质谱仪(LDI-FT-ICR-MS)研究了某船用柴油机的燃烧气溶胶样品以及用于发动机运行的原料油。此外，使用冲击器从排气管中采样颗粒物，并直接从冲击箔中进行分析，而无需对样品进行处理。从共享总和公式的高百分比以及气溶胶和重油的化学扩散的相似性来看，结果表明，初级气溶胶主要由原料燃料中存活的、未燃烧的物质组成。可以观察到热解合成的影响，与其他化合物类相比，CH-类的效果略显着，但总的来说不占优势。使用双键当量的烷基化模式和芳香度分布表明，气溶胶向低烷基化态转变。最优势系列的烷基化模式显示不同气溶胶样品之间的相关性高于气溶胶和饲料样品之间的相关性。通过聚类分析证实了这一点。总体而言，这项研究表明，LDI-FT-ICR-MS可以成功地应用于分子水平上的燃烧气溶胶分析，并且总式信息可以用来识别气溶胶和燃料之间以及不同粒度颗粒物之间的化学差异。
In this study, positive-mode laser desorption-ionisation ultra-high-resolution mass spectrometry (LDI-FT-ICR-MS) was applied to study combustion aerosol samples obtained from a ship diesel engine as well as the feed fuel, used to operate the engine. Furthermore, particulate matter was sampled from the exhaust tube using an impactor and analysed directly from the impaction foil without sample treatment. From the high percentage of shared sum formula as well as similarities in the chemical spread of aerosol and heavy fuel oil, results indicate that the primary aerosol mainly consists of survived, unburned species from the feed fuel. The effect of pyrosynthesis could be observed and was slightly more pronounced for the CH-class compared to other compound classes, but in summary not dominant. Alkylation pattern as well as the aromaticity distribution, using the double bond equivalent, revealed a shift towards lower alkylation state for the aerosol. The alkylation pattern of the most dominant series revealed a higher correlation between different aerosol samples than between aerosol and feed samples. This was confirmed by cluster analysis. Overall, this study shows that LDI-FT-ICR-MS can be successfully applied for the analysis of combustion aerosol at the molecular level and that sum formula information can be used to identify chemical differences between aerosol and fuel as well as between different size fractions of the particulate matter.