Deciphering the key drivers of oxidative potential during ammonium nitrate-mediated aqueous-phase photoreaction of methoxyphenols

IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Atmospheric Environment Pub Date : 2024-10-26 DOI:10.1016/j.atmosenv.2024.120895
Racliffe Weng Seng Lai , Tian Qiu , Xuyang Zhang , Yalin Wang , Tianwei Hao , Xinlei Ge , Lin Du , Mingjin Tang , Ka In Hoi , Kai Meng Mok , Yong Jie Li
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Abstract

Methoxyphenols are released in abundance from lignin pyrolysis during biomass burning. Apart from being atmospheric brown carbon components that absorb solar radiation and warm the climate, methoxyphenols also undergo photoreaction in the atmospheric aqueous phase and form secondary organic aerosols (aqSOA). While efforts have been devoted to understanding chemical evolutions and climate-related optical properties of aqSOA, their potential health impacts also require timely investigations. Herein, we used the dithiothreitol (DTT) assay to investigate oxidative potential of the aqSOA formed during the 8-h aqueous-phase photoreaction of two typical methoxyphenols, vanillin and vanillic acid, under pH 2 or 8, and with or without ammonia nitrate. The highest DTT consumption rates (RDTT) were observed for vanillin aqSOA formed in the presence of ammonia nitrate and at pH 8. At pH 2, although RDTT increased rapidly during early photoreaction, it reduced after prolonged illumination. High-resolution mass spectrometry and linear regression analyses were performed to correlate the photoreaction products with the observed RDTT. Results showed that three products that present quinone, lactone and dimer structures, respectively, should be the key drivers of elevated RDTT for aqSOA formed during photoreaction of vanillin and vanillic acid alone, whereas it shifted to the nitrogen-containing aromatic compounds during their photoreaction with ammonia nitrate. Our results have revealed the role of nitrogen-containing aromatic compounds in the oxidative potential and health effects of aqSOA from biomass burning, which was rarely recognized before and warrants immediate assessments.

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解读硝酸铵介导的甲氧基苯酚水相光反应过程中氧化潜能的关键驱动因素
在生物质燃烧过程中,木质素热解会释放出大量甲氧基苯酚。除了作为大气中的褐碳成分吸收太阳辐射并使气候变暖之外,甲氧基苯酚还会在大气水相中发生光反应并形成二次有机气溶胶(aqSOA)。虽然人们一直致力于了解二次有机气溶胶的化学演变和与气候相关的光学特性,但它们对健康的潜在影响也需要及时调查。在此,我们使用二硫苏糖醇(DTT)测定法研究了两种典型的甲氧基苯酚(香兰素和香草酸)在 pH 值为 2 或 8、有或没有硝酸氨的条件下进行 8 小时水相光反应过程中形成的 aqSOA 的氧化潜能。在有硝酸氨和 pH 值为 8 的条件下,观察到形成的香兰素 aqSOA 的 DTT 消耗率(RDTT)最高。 在 pH 值为 2 的条件下,虽然 RDTT 在光反应早期迅速增加,但在长时间光照后会降低。为了将光反应产物与观察到的 RDTT 联系起来,进行了高分辨率质谱分析和线性回归分析。结果表明,在香兰素和香草酸单独发生光反应时形成的 aqSOA 的 RDTT 升高的主要驱动因素应该是三种分别具有醌、内酯和二聚体结构的产物,而在它们与硝酸氨发生光反应时,RDTT 则转移到含氮芳香化合物上。我们的研究结果揭示了含氮芳香族化合物在生物质燃烧产生的 aqSOA 的氧化潜能和健康影响中的作用,这一点以前很少被认识到,需要立即进行评估。
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来源期刊
Atmospheric Environment
Atmospheric Environment 环境科学-环境科学
CiteScore
9.40
自引率
8.00%
发文量
458
审稿时长
53 days
期刊介绍: Atmospheric Environment has an open access mirror journal Atmospheric Environment: X, sharing the same aims and scope, editorial team, submission system and rigorous peer review. Atmospheric Environment is the international journal for scientists in different disciplines related to atmospheric composition and its impacts. The journal publishes scientific articles with atmospheric relevance of emissions and depositions of gaseous and particulate compounds, chemical processes and physical effects in the atmosphere, as well as impacts of the changing atmospheric composition on human health, air quality, climate change, and ecosystems.
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