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首页> 外文期刊>Environmental Science & Technology >Photochemical Aging of Guaiacol by Fe(Ⅲ)-Oxalate Complexes in Atmospheric Aqueous Phase
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Photochemical Aging of Guaiacol by Fe(Ⅲ)-Oxalate Complexes in Atmospheric Aqueous Phase

机译：Fe（Ⅲ）-草酸盐配合物在大气水相中对愈创木酚的光化学老化

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摘要

Fe(III)-oxalate complexes are likely abundant in clouds, fogs and aerosol water. They are photoreactive and can act as an important source of reactive oxygen species ((OH)-O-center dot, H2O2 and HO2 center dot) in tropospheric aqueous phases. Although the mechanisms involved in ferrioxalate photolysis have been investigated extensively, few kinetic and mechanistic information is available on the aging of dissolved organic compounds by this photochemical system. In this work, the Fe(III)-oxalate mediated photooxidation of guaiacol (GUA), a model for phenolic compounds emitted from biomass burning, was investigated under typical pH conditions of the atmospheric water. The effect of Fe(III) concentration, oxalate concentration and pH on the photooxidation of GUA was studied in detail. Our results revealed that oxalate can inhibit the oxidation of GUA by Fe(III) under the dark condition. However, the iron-catalyzed photooxidation of GUA can be strongly promoted in the presence of oxalate due to the formation of photoactive Fe(III)-oxalate complexes. GUA was rapidly oxidized to form a number of polymeric, and open-ring products with low volatility. Detailed reaction pathways for the photooxidation of GUA by Fe(III)-oxalate complexes were proposed based on the results of high-resolution mass spectrometry. This work suggests that ferrioxalate photochemistry can play an important role in the transformation of dissolved organics in atmospheric aqueous phases.
机译：草酸铁（III）络合物可能在云，雾和气溶胶水中富集。它们具有光反应性，可以作为对流层水相中重要的活性氧物质（（OH）-O-中心点，H2O2和HO2中心点）的来源。尽管广泛研究了草酸亚铁的光解涉及的机理，但是关于该光化学体系对溶解的有机化合物老化的动力学和机理信息很少。在这项工作中，在大气水的典型pH条件下，研究了草酸Fe（III）介导的愈创木酚（GUA）的光氧化，GUA是生物质燃烧产生的酚类化合物的模型。详细研究了Fe（III）浓度，草酸盐浓度和pH值对GUA光氧化的影响。我们的结果表明，草酸盐可以在黑暗条件下抑制Fe（III）氧化GUA。但是，由于存在光活性的Fe（III）-草酸盐络合物，在草酸盐存在下可以强烈促进GUA的铁催化光氧化作用。 GUA被快速氧化形成许多低挥发性的聚合物和开环产品。基于高分辨率质谱的结果，提出了Fe（III）-草酸酯络合物对GUA进行光氧化的详细反应途径。这项工作表明，草酸亚铁光化学可以在大气水相中溶解的有机物的转化中发挥重要作用。

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  • 来源
    《Environmental Science & Technology》 |2019年第1期|127-136|共10页
  • 作者

    Pang Hongwei; Zhang Qi; Wang Hongli; Cai Dongmei; Ma Yingge; Li Li; Li Kangning; Lu Xiaohui; Chen Hong; Yang Xin; Chen Jianmin;

  • 作者单位

    Fudan Univ, Dept Environm Sci & Engn, Shanghai Key Lab Atmospher Particle Pollut & Prev, Shanghai 200433, Peoples R China;

    Univ Calif Davis, Dept Environm Toxicol, Davis, CA 95616 USA;

    Shanghai Acad Environm Sci, State Environm Protect Key Lab Format & Prevent U, Shanghai 200233, Peoples R China;

    Fudan Univ, Dept Environm Sci & Engn, Shanghai Key Lab Atmospher Particle Pollut & Prev, Shanghai 200433, Peoples R China;

    Shanghai Acad Environm Sci, State Environm Protect Key Lab Format & Prevent U, Shanghai 200233, Peoples R China;

    Shanghai Acad Environm Sci, State Environm Protect Key Lab Format & Prevent U, Shanghai 200233, Peoples R China;

    Fudan Univ, Dept Environm Sci & Engn, Shanghai Key Lab Atmospher Particle Pollut & Prev, Shanghai 200433, Peoples R China;

    Fudan Univ, Dept Environm Sci & Engn, Shanghai Key Lab Atmospher Particle Pollut & Prev, Shanghai 200433, Peoples R China;

    Fudan Univ, Dept Environm Sci & Engn, Shanghai Key Lab Atmospher Particle Pollut & Prev, Shanghai 200433, Peoples R China;

    Fudan Univ, Dept Environm Sci & Engn, Shanghai Key Lab Atmospher Particle Pollut & Prev, Shanghai 200433, Peoples R China|Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China;

    Fudan Univ, Dept Environm Sci & Engn, Shanghai Key Lab Atmospher Particle Pollut & Prev, Shanghai 200433, Peoples R 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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