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In-cloud formation of secondary species in iron-containing particles

机译：含铁颗粒中的二次物种的云形成

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摘要

The increase in secondary species through cloud processing potentially increases aerosol iron (Fe) bioavailability. In this study, a ground-based counterflow virtual impactor coupled with a real-time single-particle aerosol mass spectrometer was used to characterize the formation of secondary species in Fe-containing cloud residues (dried cloud droplets) at a mountain site in southern China for nearly 1 month during the autumn of 2016. Fe-rich, Fe-dust, Fe-elemental carbon (Fe-EC), and Fe-vanadium (Fe-V) cloud residual types were obtained in this study. The Fe-rich particles, related to combustion sources, contributed 84% (by number) to the Fe-containing cloud residues, and the Fe-dust particles represented 12 %. The remaining 4% consisted of the Fe-EC and Fe-V particles. It was found that above 90% (by number) of Fe-containing particles had already contained sulfate before cloud events, leading to no distinct change in number fraction (NF) of sulfate during cloud events. Cloud processing contributed to the enhanced NFs of nitrate, chloride, and oxalate in the Fe-containing cloud residues. However, the in-cloud formation of nitrate and chloride in the Fe-rich type was less obvious relative to the Fe-dust type. The increased NF of oxalate in the Fe-rich cloud residues was produced via aqueous oxidation of oxalate precursors (e.g., glyoxylate). Moreover, Fe-driven Fenton reactions likely increase the formation rate of aqueous-phase OH, improving the conversion of the precursors to oxalate in the Fe-rich cloud residues. During daytime, the decreased NF of oxalate in the Fe-rich cloud residues was supposed to be due to the photolysis of Fe-oxalate complexes. This work emphasizes the role of combustion Fe sources in participating in cloud processing and has important implications for evaluating Fe bioavailability from combustion sources during cloud processing.
机译：通过云处理的二次物种的增加可能会增加气溶胶铁（Fe）生物利用度。在该研究中，使用与实时单粒子气溶胶质谱仪结合的基于基于逆流虚拟撞击仪，以表征在中国南部山区的含Fe云残留（干燥云液滴）中的二次物种的形成在2016年秋季近1个月。在本研究中获得了Fe-Rich，Fe-Dust，Fe-Colute碳（Fe-EC）和Fe-Vainium（Fe-V）云残留类型。与燃烧源相关的Fe富含Fe的颗粒将84％（按数量）贡献给Fe的云残留物，并且Fe-粉尘颗粒表示为12％。其余4％由Fe-EC和Fe-V颗粒组成。发现在云事件之前已经含有硫酸盐的含硫颗粒以上的90％（按数量），导致云事件期间硫酸盐的数级分数（NF）没有明显的变化。云处理有助于在含Fe云残留物中硝酸盐，氯化物和草酸的增强NFS。然而，相对于Fe粉尘型，Fe-富含型硝酸盐和氯化物的云形成较小。通过草酸盐前体的水性氧化产生Fe-富含云残基中的草酸盐的NF增加（例如，乙醛酸）。此外，Fe-Drive Fenton反应可能增加水相OH的形成速率，从而改善Fe富含Fe云残留物中前体对草酸盐的转化物。在白天期间，由于Fe-草酸酯配合物的光解。这项工作强调了燃烧FE源在参与云加工方面的作用，并对云处理期间从燃烧来源评估Fe生物利用度具有重要意义。

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  • 来源
    《Atmospheric chemistry and physics》 |2019年第2期|共12页
  • 作者

    Lin Qinhao; Bi Xinhui; Zhang Guohua; Yang Yuxiang; Peng Long; Lian Xiufeng; Fu Yuzhen; Li Mei; Chen Duohong; Miller Mark; Ou Ji; Tang Mingjin; Wang Xinming; Peng Pingan; Sheng Guoying; Zhou Zhen;

  • 作者单位

    Chinese Acad Sci State Key Lab Organ Geochem Guangzhou Inst Geochem Guangzhou 510640 Guangdong Peoples R China;

    Chinese Acad Sci State Key Lab Organ Geochem Guangzhou Inst Geochem Guangzhou 510640 Guangdong Peoples R China;

    Chinese Acad Sci State Key Lab Organ Geochem Guangzhou Inst Geochem Guangzhou 510640 Guangdong Peoples R China;

    Chinese Acad Sci State Key Lab Organ Geochem Guangzhou Inst Geochem Guangzhou 510640 Guangdong Peoples R China;

    Chinese Acad Sci State Key Lab Organ Geochem Guangzhou Inst Geochem Guangzhou 510640 Guangdong Peoples R China;

    Chinese Acad Sci State Key Lab Organ Geochem Guangzhou Inst Geochem Guangzhou 510640 Guangdong Peoples R China;

    Chinese Acad Sci State Key Lab Organ Geochem Guangzhou Inst Geochem Guangzhou 510640 Guangdong Peoples R China;

    Jinan Univ Inst Mass Spectrometer &

    Atmospher Environm Guangzhou 510632 Guangdong Peoples R China;

    Guangdong Environm Monitoring Ctr State Environm Protect Key Lab Reg Air Qual Monit Guangzhou 510308 Guangdong Peoples R China;

    Rutgers State Univ Dept Environm Sci New Brunswick NJ 08901 USA;

    Shaoguan Environm Monitoring Ctr Shaoguan 512026 Peoples R China;

    Chinese Acad Sci State Key Lab Organ Geochem Guangzhou Inst Geochem Guangzhou 510640 Guangdong Peoples R China;

    Chinese Acad Sci State Key Lab Organ Geochem Guangzhou Inst Geochem Guangzhou 510640 Guangdong Peoples R China;

    Chinese Acad Sci State Key Lab Organ Geochem Guangzhou Inst Geochem Guangzhou 510640 Guangdong Peoples R China;

    Chinese Acad Sci State Key Lab Organ Geochem Guangzhou Inst Geochem Guangzhou 510640 Guangdong Peoples R China;

    Jinan Univ Inst Mass Spectrometer &

    Atmospher Environm Guangzhou 510632 Guangdong Peoples R China;

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  • 正文语种 eng
  • 中图分类 大气科学（气象学）;
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