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Aromatic Photo-oxidation, A New Source of Atmospheric Acidity

机译：芳香的光氧化，一种新的大气酸度来源

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摘要

Formic acid (HCOOH), one of the most important and ubiquitous organic acids in the Earth's atmosphere, contributes substantially to atmospheric acidity and affects pH-dependent reactions in the aqueous phase. However, based on the current mechanistic understanding, even the most advanced chemical models significantly underestimate the HCOOH concentrations when compared to ambient observations at both ground-level and high altitude, thus underrating its atmospheric impact. Here we reveal new chemical pathways to HCOOH formation from reactions of both O_3 and OH with ketene-enols, which are important and to date undiscovered intermediates produced in the photo-oxidation of aromatics and furans. We highlight that the estimated yields of HCOOH from ketene-enol oxidation are up to 60% in polluted urban areas and greater than 30% even in the continental background. Our theoretical calculations are further supported by a chamber experiment evaluation. Considering that aromatic compounds are highly reactive and contribute ca. 10% to global nonmethane hydrocarbon emissions and 20% in urban areas, the new oxidation pathways presented here should help to narrow the budget gap of HCOOH and other small organic acids and can be relevant in any environment with high aromatic emissions, including urban areas and biomass burning plumes.
机译：甲酸（HCOOH）是地球大气层中最重要和最普遍无处不在的有机酸之一，基本上促进大气酸度，并影响水相中的pH依赖性反应。然而，基于目前的机械理解，与地面和高海拔的环境观测相比，即使是最先进的化学模型也明显低估了HCOOH浓度，从而越来越低于其大气影响。在这里，我们揭示了从酮烯的反应的HCOOH形成的新化学途径，这是在芳烃和呋喃的光氧化中产生的重要性和迄今为止的中间体。我们强调，氯烯-EnOL氧化的HCOOH的估计产量在污染的城市地区的60％高达60％，即使在大陆背景下也大于30％。我们的理论计算得到了分钟实验评估的进一步支持。考虑到芳族化合物是高反应性和贡献CA.全球非甲烷的烃排放量和20％的城市地区，此处呈现的新氧化途径应有助于缩小HCOOH和其他小有机酸的预算间隙，并且可以在任何具有高芳香排放的环境中相关，包括城市地区生物质燃烧羽毛。

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  • 来源
    《Environmental Science & Technology》 |2020年第13期|7798-7806|共9页
  • 作者

    Sainan Wang; Mike J. Newland; Wei Deng; Andrew R. Rickard; Jacqueline F. Hamilton; Amalia Munoz; Milagros Rodenas; Monica M. Vazquez; Liming Wang; Xinming Wang;

  • 作者单位

    State Key Laboratory of Organic Geochemistry and Guangdong Key Laboratory of Environmental Protection and Resources Utilization Guangzhou Institute of Geochemistry Chinese Academy of Sciences Guangzhou China;

    Wolfson Atmospheric Chemistry Laboratories Department of Chemistry University of York York YO10 5DD U.K.;

    State Key Laboratory of Organic Geochemistry and Guangdong Key Laboratory of Environmental Protection and Resources Utilization Guangzhou Institute of Geochemistry Chinese Academy of Sciences Guangzhou China;

    Wolfson Atmospheric Chemistry Laboratories Department of Chemistry and National Centre for Atmospheric Science Wolfson Atmospheric Chemistry Laboratories University of York York YOW SDD U.K.;

    Wolfson Atmospheric Chemistry Laboratories Department of Chemistry University of York York YOW SDD U.K.;

    Fundacibn CEAM EUPHORE Laboratories Paterna Valencia Spain;

    Fundacibn CEAM EUPHORE Laboratories Paterna Valencia Spain;

    Fundacibn CEAM EUPHORE Laboratories Paterna Valencia Spain;

    School of Chemistry & Chemical Engineering South China University of Technology Guangzhou China;

    State Key Laboratory of Organic Geochemistry and Guangdong Key Laboratory of Environmental Protection and Resources Utilization Guangzhou Institute of Geochemistry Chinese Academy of Sciences Guangzhou China;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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