Molecular characterization of organic aerosol in the Himalayas: insight from ultra-high-resolution mass spectrometry

• Published in: Atmospheric Chemistry and Physics
• Main Authors: Y. An, J. Xu, L. Feng, X. Zhang, Y. Liu, S. Kang, B. Jiang, Y. Liao
• Format: Article
• Language: English
• Published: Copernicus Publications 2019-01-01
• Online Access: https://www.atmos-chem-phys.net/19/1115/2019/acp-19-1115-2019.pdf
• ISSN: 1680-7316; 1680-7324

<p>An increased trend in aerosol concentration has been observed in the Himalayas in recent years, but the understanding of the chemical composition and sources of aerosol remains poorly understood. In this study, molecular chemical composition of water-soluble organic matter (WSOM) from two filter samples collected during two high aerosol loading periods (denoted as P1 and P2) at a high-altitude station (Qomolangma Station, QOMS; 4276&thinsp;<span class="inline-formula">m</span>&thinsp;a.s.l.) in the northern Himalayas was identified using electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (ESI-FTICR MS). More than 4000 molecular formulas were identified in each filter sample which were classified into two compound groups (CHO and CHON) based on their elemental composition, with both accounting for nearly equal contributions in number (45&thinsp;%–55&thinsp;%). The relative abundance weighted mole ratio of <span class="inline-formula">O∕C_w</span> for P1 and P2 was 0.43 and 0.39, respectively, and the weighted double bond equivalents (DBE<span class="inline-formula">_w</span>), an index for the saturation of organic molecules, were 7.12 and 7.87, respectively. Although the <span class="inline-formula">O∕C_w</span> mole ratio was comparable for CHO and CHON compounds, the DBE<span class="inline-formula">_w</span> was significantly higher in CHON compounds than CHO compounds. More than 50&thinsp;% molecular formulas in the Van Krevelen (VK) diagram (<span class="inline-formula">H∕C</span> vs. <span class="inline-formula">O∕C</span>) were located in 1–1.5 (<span class="inline-formula">H∕C</span>) and 0.2–0.6 (<span class="inline-formula">O∕C</span>) regions, suggesting potential lignin-like compounds. The distributions of CHO and CHON compounds in the VK diagram, DBE vs. number of C atoms, and other diagnostic diagrams showed high similarities among each other, suggesting their similar source and/or atmospheric processes. Many formulas formed from biogenic volatile organic compounds (e.g., ozonolysis of <span class="inline-formula"><i>α</i></span>-pinene products) and biomass-burning-emitted compounds (e.g., phenolic compounds) were found in the WSOM, suggesting the important contribution of these two sources in the Himalayas. The high DBE and high fraction of nitrogen-containing aerosol can potentially impact aerosol light absorption in this remote region. Further comprehensive study is needed due to the complexity of organic aerosol and limited molecular number identified in this study.</p>