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相对湿度和种子颗粒对α-蒎烯二次有机气溶胶分子组成的影响

Influence of Relative Humidity and Seed Particles on Molecular Composition of α‑Pinene Secondary Organic Aerosol.

作者信息

Top Jens, Garner Natasha M, Sari Doré Félix, Zhang Yanjun, Carstens Cecilie, Dubois Clément, Mahrt Fabian, Ammann Markus, Prévôt André S H, Riva Matthieu, El Haddad Imad, Bell David M

机构信息

PSI Center for Energy and Environmental Sciences, 5232 Villigen PSI, Switzerland.

Université Claude Bernard Lyon 1, CNRS, IRCELYON, UMR 5256, Villeurbanne F-69100, France.

出版信息

ACS EST Air. 2025 Jul 7;2(8):1565-1574. doi: 10.1021/acsestair.5c00064. eCollection 2025 Aug 8.

Abstract

Secondary organic aerosol (SOA), a major component of submicrometer particles, is critical to the climate and human health. SOA can form through nucleation of low-volatility organic compounds, following atmospheric oxidation, or by condensing these vapors onto existing particles. In either of these cases, the formation of SOA particles could be affected by atmospheric conditions (e.g., relative humidity (RH)) and particle liquid water content. This study examines the effects of RH on the formation and composition of SOA from dark α-pinene (CH) ozonolysis, as a canonical system, with or without ammonium sulfate (AS, (NH)SO) seed particles across varying RH levels. Using online extractive electrospray ionization mass spectrometry, we identified monomers (C) and dimers (C) in the SOA with high chemical and temporal resolution. In both cases, high RH (>90%) promotes dimer formation in the particle phase, while they appear at the beginning of the experiment when (NH)SO seeds are present. The prompt increase in dimers in high RH seed containing experiments (60-65% dimers), which are absent at low RH (10%), suggests that intraparticle reactions are responsible for the dimer formation.

摘要

二次有机气溶胶(SOA)是亚微米颗粒的主要成分,对气候和人类健康至关重要。SOA可通过低挥发性有机化合物在大气氧化后成核形成,或通过将这些蒸汽凝结到现有颗粒上形成。在这两种情况下,SOA颗粒的形成都可能受到大气条件(如相对湿度(RH))和颗粒液态水含量的影响。本研究以黑暗条件下α-蒎烯(CH)臭氧化作为典型体系,研究了在不同RH水平下,有无硫酸铵(AS,(NH)SO)种子颗粒时,RH对SOA形成和组成的影响。使用在线萃取电喷雾电离质谱,我们以高化学和时间分辨率鉴定了SOA中的单体(C)和二聚体(C)。在这两种情况下,高RH(>90%)都会促进颗粒相中形成二聚体,而当存在(NH)SO种子时,二聚体在实验开始时就会出现。在含种子的高RH实验中(60 - 65%为二聚体)二聚体迅速增加,而在低RH(10%)时不存在,这表明颗粒内反应是二聚体形成的原因。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/66eb/12340754/97afaf54ad6f/ea5c00064_0001.jpg

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