期刊
ENVIRONMENTAL POLLUTION
卷 305, 期 -, 页码 -出版社
ELSEVIER SCI LTD
DOI: 10.1016/j.envpol.2022.119284
关键词
GC x GC-ToF-MS; I/SVOCs speciation; HDDVs; Oxygenated-I/SVOCs; SOA estimation
资金
- National Natural Science Foundation of China [51978404, 42105100, 41977180]
- Basic Research of Shenzhen Science and Technology Innovation Commission [JCYJ20190808145218827]
- Guangdong Basic and Applied Basic Research Fund Committee [2020B1515130003]
- Samsung Advanced Institute of Technology
- Tencent Foundation through the XPLORER PRIZE
This study develops a novel method for the comprehensive characterization of intermediate-volatility and semi-volatile organic compounds (I/SVOCs) using two-dimensional gas chromatography time-of-flight mass spectrometry. The study provides the first quantification of I/SVOC emissions from heavy-duty diesel vehicles and reveals that oxygenated compounds contribute to more than 20% of the total I/SVOC mass. The results have implications for the estimation of secondary organic aerosol.
Intermediate-volatility and semi-volatile organic compounds (I/SVOCs) are key precursors of secondary organic aerosol (SOA). However, the comprehensive characterization of I/SVOCs has long been an analytical challenge. Here, we develop a novel method of speciating and quantifying I/SVOCs using two-dimensional gas chromatography time-of-flight mass spectrometry (GC x GC-ToF-MS) by constructing class-screening programs based on their characteristic fragments and mass spectrum patterns. Using this new approach, we then present a comprehensive analysis of gaseous I/SVOC emissions from heavy-duty diesel vehicles (HDDVs). Over three thousand compounds are identified and classified into twenty-one categories. The dominant compound groups of I/SVCOs emitted by HDDVs are alkanes (including normal and branched alkanes, 37-66%), benzylic alcohols (7-20%), alkenes (3-11%), cycloalkanes (3-9%), and benzylic ketones (1-4%). Oxygenated I/SVOCs (O-I/ SVOCs, e.g., benzylic alcohols and ketones) are first quantified and account for > 20% of the total I/SVOC mass. Advanced aftertreatment devices largely reduce the total I/SVOC emissions but increase the proportion of O-I/ SVOCs. With the speciation data, we successfully map the I/SVOCs into the two-dimensional volatility basis set space, which facilitates a better estimation of SOA. As aging time goes by, approximate 45% difference between the two scenarios after seven-day aging is observed, which confirms the significant impact of speciated I/SVOC emission data on SOA prediction.
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