1,3-丁二烯的大气氧化：酸度和相对湿度对 SOA 成分和空气有毒化合物的影响

IF 5.2 1区地球科学 Q1 ENVIRONMENTAL SCIENCES

Atmospheric Chemistry and Physics Pub Date : 2024-07-08 DOI:10.5194/egusphere-2024-2032

Mohammed Jaoui, Klara Nestorowicz, Krzysztof Rudzinski, Michael Lewandowski, Tadeusz Kleindienst, Julio Torres, Ewa Bulska, Witold Danikiewicz, Rafal Szmigielski

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引用次数: 0

摘要

摘要本研究探讨了相对湿度（RH）对 1,3-丁二烯（13BD）在酸性和非酸性条件下与氮氧化物发生光氧化反应所形成的气体和颗粒相的化学组成的影响。实验在一个以稳态模式运行的 14.5 立方米烟雾室中进行。通过高效液相色谱法、气相色谱质谱法和超高效液相色谱-高分辨质谱法对产物进行了鉴定。确定了超过 48 种含氧产品，包括 33 种含氧有机物、10 种有机硫酸盐 (OS)、PAN、APAN、乙二醛、甲醛和丙烯醛。研究发现，二次有机气溶胶（SOA）的质量和反应产物取决于相对湿度和气溶胶的酸度。SOA 质量和大多数 SOA 产物（i）在酸性条件下比非酸性条件下高，（ii）随着相对湿度的增加而减少。在所有相对湿度水平下的酸性或非酸性条件下测得的主要物质包括甘油酸、苏糖醇、苏酸、四种二聚物、三种未知物和四种有机硫酸盐。在酸性和非酸性条件下，次生有机碳总量和碳产量随着相对湿度的增加而减少。在我们的系统中，13BD 的光化学反应活性随着相对湿度的增加而降低，并且在非酸性条件下比酸性条件下更快。为了确定 13BD 产品对环境气溶胶的贡献，我们分析了在波兰的三个欧洲监测站收集的 PM2.5 样品。现场样本中出现了几种 13BD SOA 产物（如甘油酸、酒石酸、苏氨酸、酒石酸和 OSs），这表明 13BD 可能有助于环境气溶胶的形成。

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Atmospheric oxidation of 1,3-butadiene: influence of acidity and relative humidity on SOA composition and air toxic compounds

Abstract. This study investigated the effect of relative humidity (RH) on the chemical composition of gas and particle phases formed from the photooxidation of 1,3-butadiene (13BD) in the presence of NOx under acidic and non-acidic conditions. The experiments were conducted in a 14.5 m³ smog chamber operated in a steady-state mode. Products were identified by high performance liquid chromatography, gas chromatography mass spectrometry and ultrahigh performance liquid chromatography coupled with high resolution mass spectrometry. More than 48 oxygenated products were identified including 33 oxygenated organics, 10 organosulfates (OSs), PAN, APAN, glyoxal, formaldehyde, and acrolein. Secondary organic aerosol (SOA) mass and reaction products were found to be dependent on RH and acidity of the aerosol. SOA mass, and most SOA products (i) were higher under acidic than non-acidic conditions, and (ii) decreased with increasing RH. Glyceric acid, threitols, threonic acids, four dimers, three unknowns, and four organosulfates were among the main species measured either under acidic or non-acidic conditions across all RH levels. Total secondary organic carbon and carbon yield decreased with increasing RH under both acidic and non-acidic conditions. The photochemical reactivity of 13BD in our systems decreased with increasing RH and was faster under non-acidic than acidic conditions. To determine the contribution of 13BD products to ambient aerosol, we analyzed PM_2.5 samples collected at three European monitoring stations located in Poland. The occurrence of several 13BD SOA products (e.g., glyceric acid, tartronic acid, threonic acid, tartaric acid, and OSs) in the ﬁeld samples suggests that 13BD could contribute to ambient aerosol formation.

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来源期刊

Atmospheric Chemistry and Physics 地学-气象与大气科学

CiteScore

10.70

自引率

20.60%

发文量

702

审稿时长

6 months

期刊介绍： Atmospheric Chemistry and Physics (ACP) is a not-for-profit international scientific journal dedicated to the publication and public discussion of high-quality studies investigating the Earth''s atmosphere and the underlying chemical and physical processes. It covers the altitude range from the land and ocean surface up to the turbopause, including the troposphere, stratosphere, and mesosphere. The main subject areas comprise atmospheric modelling, field measurements, remote sensing, and laboratory studies of gases, aerosols, clouds and precipitation, isotopes, radiation, dynamics, biosphere interactions, and hydrosphere interactions. The journal scope is focused on studies with general implications for atmospheric science rather than investigations that are primarily of local or technical interest.