1,3-丁二烯的大气氧化:种子气溶胶酸度和相对湿度对SOA组成和空气有毒化合物产生的影响

IF 5.2 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES
Atmospheric Chemistry and Physics Pub Date : 2025-01-01 Epub Date: 2025-01-31 DOI:10.5194/acp-25-1401-2025
Mohammed Jaoui, Klara Nestorowicz, Krzysztof J Rudzinski, Michael Lewandowski, Tadeusz E Kleindienst, Julio Torres, Ewa Bulska, Witold Danikiewicz, Rafal Szmigielski
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引用次数: 0

摘要

本研究研究了在酸化和非酸化种子气溶胶下,相对湿度(RH)对1,3-丁二烯(13BD)在NO存在下光氧化形成的气相和颗粒相化学组成的影响。实验在14.5 m3的雾霾室中进行,以稳态模式运行。采用高效液相色谱法、气相色谱-质谱法和超高效液相色谱-高分辨率质谱法对产物进行鉴定。共鉴定出50多种含氧产物,包括33种含氧有机物、10种有机硫酸盐(OSs)、PAN、APAN、乙二醛、甲醛和丙烯醛。二次有机气溶胶(SOA)的质量和反应产物的形成取决于RH和种子气溶胶的酸度。基于扩展气溶胶无机物模型(E-AIM),发现酸化溶液和非酸化溶液中的种子气溶胶分别存在于水相和固相中。虽然“酸化”和“非酸化”这两个术语对于种子雾化的溶液是正确的,但在物种从水/固两相中分离或分离的相状态之间存在着更根本的差异,这在很大程度上影响了它们的分离和形成机制。SOA质量和大多数SOA产品(i)在酸化种子条件下(气溶胶颗粒潮解)比在未酸化种子条件下(气溶胶颗粒不含任何水相)更高;(ii)在酸化种子条件下,随着气溶胶水相酸度的增加而增加;(iii)随RH的增加而降低。甘油、苏糖醇、苏酸、四种二聚体、三种未知物质和四种有机硫酸盐是在所有RH水平下酸化或非酸化条件下测量的主要物质。在酸化和非酸化种子条件下,总二次有机碳和碳产量均随RH的增加而降低。在我们的体系中,13BD的光化学反应活性随着RH的增加而降低,并且在未酸化的种子条件下比酸化的种子条件下更快。为了确定13BD产品对环境气溶胶的贡献,我们分析了位于波兰的三个欧洲监测站收集的PM2.5样本。在现场样品中出现了几种13BD SOA产物(如甘油酸、酒石酸、苏酸、酒石酸和os),表明13BD可能有助于环境气溶胶的形成。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Atmospheric oxidation of 1,3-butadiene: influence of seed aerosol acidity and relative humidity on SOA composition and the production of air toxic compounds.

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 NO x under acidified and non-acidified seed aerosol. 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 50 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 formed depended on RH and on the acidity of the seed aerosol. Based on the Extended Aerosol Inorganics Model (E-AIM), the seed aerosol originated from the acidified and non-acidified solutions was found to exist under aqueous and solid phases, respectively. Although the terms "acidified" and "non-acidified" are true for the solutions from which the seeds were atomized, there are far more fundamental differences between the phase states in which species partition to or from (aqueous/solid), which considerably affects their partitioning and formation mechanisms. SOA mass and most SOA products (i) were higher under acidified seed conditions, where the aerosol particles were deliquescent, than under non-acidified seed conditions, where the aerosol particles did not contain any aqueous phase; (ii) increased with the acidity of the aerosol aqueous phase in the experiments under acidified seed conditions; and (iii) decreased with increasing RH. Glyceric acid, threitols, threonic acids, four dimers, three unknowns, and four organosulfates were among the main species measured under either acidified or non-acidified conditions across all RH levels. Total secondary organic carbon and carbon yield decreased with increasing RH under both acidified and non-acidified seed conditions. The photochemical reactivity of 13BD in our systems decreased with increasing RH and was faster under non-acidified than acidified seed conditions. To determine the contribution of 13BD products to ambient aerosol, we analyzed PM2.5 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
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.
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