Xiang Wang, Wang Weigang, Hou Chunyan, Fan CiCi, Lei Ting, Li Junling, Ge Maofa
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Beijing National Laboratory for Molecular Sciences (BNLMS), Chemistry Academy of Sciences Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China; University of Chinese Academy of Sciences, Beijing 100049, China.
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Beijing National Laboratory for Molecular Sciences (BNLMS), Chemistry Academy of Sciences Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China; University of Chinese Academy of Sciences, Beijing 100049, China.
Sci Total Environ. 2024 Mar 25;918:170379. doi: 10.1016/j.scitotenv.2024.170379. Epub 2024 Jan 26.
Alkyl-PAHs (APAHs) have been identified worldwide, which could rapidly react with chlorine and OH radicals in the atmosphere. In this study, a comprehensive investigation is conducted for SOA generated by a representative alkyl-naphthalene (1-methyl naphthalene, 1-MN) initiated by Cl, including yield, chemical composition, and volatility of SOA. To better understand 1-MN atmospheric oxidation, reaction mechanisms of 1MN with Cl atoms and OH radicals are proposed and compared under different nitrogen oxides (NO) conditions. The SOA yields are comparable for Cl-initiated and OH-initiated reactions under high NO conditions but increased in Cl-initiated reactions under low NO conditions. The compounds with ten carbons are more abundant in Cl-initiated SOA, while compounds with nine carbons have higher intensity, suggesting that Cl caused ring-retained and alkyl-lost products and OH produces ring-broken and alkyl-retained compounds. The volatility of SOA is remarkably low, and SOA formed from Cl oxidation is slightly higher than that from OH oxidation. These results reveal that 1MN-derived SOA with OH and Cl radicals would have different physical-chemical properties and may play an important role in air quality and health effects.
烷基多环芳烃(APAHs)在全球范围内都有发现,它们能在大气中迅速与氯和羟基自由基发生反应。在本研究中,对由氯引发的代表性烷基萘(1-甲基萘,1-MN)生成的二次有机气溶胶(SOA)进行了全面研究,包括SOA的产率、化学成分和挥发性。为了更好地理解1-MN的大气氧化过程,提出并比较了在不同氮氧化物(NO)条件下1-MN与氯原子和羟基自由基的反应机制。在高NO条件下,氯引发和羟基引发反应的SOA产率相当,但在低NO条件下,氯引发反应的SOA产率增加。在氯引发的SOA中,含十个碳原子的化合物更为丰富,而含九个碳原子的化合物强度更高,这表明氯导致了环保留和烷基损失产物,而羟基产生了环断裂和烷基保留化合物。SOA的挥发性非常低,由氯氧化形成的SOA略高于由羟基氧化形成的SOA。这些结果表明,由羟基和氯自由基产生的源自1-MN的SOA具有不同的物理化学性质,可能在空气质量和健康影响方面发挥重要作用。