Aerosol Chemistry Resolved by Mass Spectrometry: Insights into Particle Growth after Ambient New Particle Formation.
Aerosol Chemistry Resolved by Mass Spectrometry: Insights into Particle Growth after Ambient New Particle Formation.
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通过质谱法解析气溶胶化学：洞察环境新颗粒形成后的颗粒生长
DOI：
10.1021/acs.est.6b01673
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发表时间：
2016
影响因子：
11.4
通讯作者：
中科院分区：
文献类型：
--
作者：
挥发性有机化合物（VOC）的大气氧化产生大量不同的有机分子，其包括宽范围的挥发性。根据它们的挥发性，它们可以参与新粒子的形成和粒子的增长，从而影响大气中云凝结核的数量浓度。在这里，我们确定了氧化产品的挥发性有机化合物在颗粒相在农村山顶站在德国中部的实地研究。我们使用大气压化学电离质谱（（−）APCI-MS）和气溶胶质谱分别对0.02 - 2.5和0.05 - 0.6 μ m尺寸范围内的有机物和总有机气溶胶（OA）质量进行时间分辨测量。有机分子的元素组成通过使用液相色谱耦合电喷雾电离超高分辨率质谱法对共定位的PM 2.5过滤器样品进行离线分析来确定。我们发现极低的挥发性有机化合物，可能来自倍半萜氧化，是新颗粒形成期间（−）APCI-MS质谱中的主要信号。当新形成的颗粒生长到更大的直径时，低挥发性有机化合物开始占主导地位。此外，APCI-MS质谱图表明OA级分的平均分子量范围在270和340 amu之间，与OA质量呈负相关。我们的观察可以帮助进一步了解哪些生物前体和哪些化学过程在大气新粒子形成后驱动粒子生长。
Atmospheric oxidation of volatile organic compounds (VOCs) yields a large number of different organic molecules which comprise a wide range of volatility. Depending on their volatility, they can be involved in new particle formation and particle growth, thus affecting the number concentration of cloud condensation nuclei in the atmosphere. Here, we identified oxidation products of VOCs in the particle phase during a field study at a rural mountaintop station in central Germany. We used atmospheric pressure chemical ionization mass spectrometry ((−)APCI-MS) and aerosol mass spectrometry for time-resolved measurements of organic species and of the total organic aerosol (OA) mass in the size range of 0.02–2.5 and 0.05–0.6 μm, respectively. The elemental composition of organic molecules was determined by offline analysis of colocated PM 2.5 filter samples using liquid chromatography coupled to electrospray ionization ultrahigh-resolution mass spectrometry. We found extremely low volatile organic compounds, likely from sesquiterpene oxidation, being the predominant signals in the (−)APCI-MS mass spectrum during new particle formation. Low volatile organic compounds started to dominate the spectrum when the newly formed particles were growing to larger diameters. Furthermore, the APCI-MS mass spectra pattern indicated that the average molecular weight of the OA fraction ranged between 270 and 340 amu, being inversely related to OA mass. Our observations can help further the understanding of which biogenic precursors and which chemical processes drive particle growth after atmospheric new-particle formation.
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