秸秆燃烧气溶胶中含氮有机化合物的光化学转化特征

Photochemical Transformation Characteristics of Nitrogen-Containing Organic Compounds in Straw Burning Aerosols

摘要

为研究秸秆燃烧产生含氮有机化合物(NOCs)影响二次气溶胶的形成机制,用自主搭建的烟雾箱系统模拟秸秆燃烧气溶胶(SBA)在有光(紫外光)和无光(黑暗)条件下的反应过程,采用高分辨率电喷雾质谱(HRESI-MS)结合Van Krevelen(VK)图分析方法,对SBA中NOCs的分子组成及氧化特征进行表征.结果表明,秸秆燃烧产生的有机化合物中60%以上为含氮有机物,包括CHN类(含C,H,N元素的化合物,9.61%~58.63%)、CHON类(含C,H,O,N元素的化合物,22.38%~62.89%)和CHONS类(含C,H,O,N,S元素的化合物,6.48%~29.90%);紫外光照条件下有机物整体氧化程度高于黑暗条件;HRESI-MS结合VK图可实现对SBA中NOCs组分的精准定性及氧化态特征表征,有效追踪不同老化阶段分子组成与元素比参数的动态变化,为生物质燃烧气溶胶中NOCs老化过程的分子层面研究提供可靠的分析方法.

Abstract

In order to study the mechanism by which nitrogen-containing organic compounds (NOCs) produced during straw burning affected the formation of secondary aerosols, a self-built smog-chamber system was used to simulate the aging processes of straw burning aerosol (SBA) under light (UV) and no light (dark) conditions. High-resolution electrospray ionization mass spectrometry (HRESI-MS) combined with Van Krevelen (VK) diagram analysis was used to characterize the molecular composition and oxidation features of NOCs in SBA. The results show that more than 60% of the organic compounds produced by straw burning are NOCs, including CHN (compounds containing C, H, N elements, 9.61%—58.63%), CHON (compounds containing C, H, O, N elements, 22.38%—62.89%), and CHONS (compounds containing C, H, O, N, S elements, 6.48%—29.90%). The overall oxidation state of the organic compounds under UV light is higher than that under dark conditions. The combination of HRESI-MS and VK diagram can achieve accurate qualitative and oxidation state characterization of NOCs components in SBA, effectively tracking dynamic changes of molecular composition and elemental ratio parameters at different aging stages, and providing a reliable analytical approach for molecular-level research on NOC aging process in biomass burning aerosols.

关键词

秸秆燃烧气溶胶 / 高分辨率电喷雾质谱 / 含氮有机化合物 / 光化学老化

Key words

straw burning aerosol / high resolution electrospray ionization mass spectrometry / nitrogen-containing organic compound / photochemical aging

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基金资助

国家级大学生创新创业训练计划项目(201910183076)