Molecular characterization of diverse quinone analogs for discrimination of aerosol-bound persistent pyrolytic and photolytic radicals

IF 18.8 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Laijin Zhong , Bao Zhu , Wenyuan Su , Wenqing Liang , Haotian Wang , Tingyu Li , Dong Cao , Ting Ruan , Jianmin Chen , Guibin Jiang
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引用次数: 0

Abstract

Aerosol-bound organic radicals, including environmentally persistent free radicals (EPFRs), are key components that affect climate, air quality, and human health. While putative structures have been proposed, the molecular characteristics of EPFRs remain unknown. Here, we report a surrogate method to characterize EPFRs in real ambient samples using mass spectrometry. The method identifies chemically relevant oxygenated polycyclic aromatic hydrocarbons (OxPAH) that interconvert with oxygen-centered EPFR (OC-EPFR). We found OxPAH compounds most relevant to OC-EPFRs are structurally rich and diverse quinones, whose diversity is strongly associated with OC-EPFR levels. Both atmospheric oxidation and combustion contributed to OC-EPFR formation. Redundancy analysis and photochemical aging model show pyrolytic sources generated more oxidized OC-EPFRs than photolytic sources. Our study reveals the detailed molecular characteristics of OC-EPFRs and shows that oxidation states can be used to identify the origins of OC-EPFRs, offering a way to track the development and evolution of aerosol particles in the environment.

不同醌类似物在气溶胶结合的持久热解和光解自由基鉴别中的分子表征
气溶胶结合的有机自由基,包括环境持久性自由基(EPFRs),是影响气候、空气质量和人类健康的关键成分。虽然已经提出了假设的结构,但epfr的分子特征仍然未知。在这里,我们报告了一种替代方法,用质谱法来表征真实环境样品中的epfr。该方法确定了与氧中心EPFR (OC-EPFR)相互转化的化学相关的含氧多环芳烃(OxPAH)。我们发现与OC-EPFR最相关的OxPAH化合物是结构丰富多样的醌类,其多样性与OC-EPFR水平密切相关。大气氧化和燃烧都有助于OC-EPFR的形成。冗余分析和光化学老化模型表明,热解源比光解源产生更多的氧化OC-EPFRs。我们的研究揭示了OC-EPFRs的详细分子特征,并表明氧化态可以用来识别OC-EPFRs的起源,为跟踪环境中气溶胶颗粒的发展和演变提供了一种方法。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Science Bulletin
Science Bulletin MULTIDISCIPLINARY SCIENCES-
CiteScore
24.60
自引率
2.10%
发文量
8092
期刊介绍: Science Bulletin (Sci. Bull., formerly known as Chinese Science Bulletin) is a multidisciplinary academic journal supervised by the Chinese Academy of Sciences (CAS) and co-sponsored by the CAS and the National Natural Science Foundation of China (NSFC). Sci. Bull. is a semi-monthly international journal publishing high-caliber peer-reviewed research on a broad range of natural sciences and high-tech fields on the basis of its originality, scientific significance and whether it is of general interest. In addition, we are committed to serving the scientific community with immediate, authoritative news and valuable insights into upcoming trends around the globe.
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