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首页> 外文期刊>Environmental Science & Technology >Modeling the Impact of Iron-Carboxylate Photochemistry on Radical Budget and Carboxylate Degradation in Cloud Droplets and Particles
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Modeling the Impact of Iron-Carboxylate Photochemistry on Radical Budget and Carboxylate Degradation in Cloud Droplets and Particles

机译：模拟羧酸铁光化学对云滴和颗粒中自由基收支和羧酸盐降解的影响

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To quantify the effects of an advanced iron photochemistry scheme, the chemical aqueous-phase radical mechanism (CAPRAM 3.0i) has been updated with several new Fe(Ⅲ)-carboxylate complex photolysis reactions. Newly introduced ligands are malonate, succinate, tartrate, tartronate, pyruvate, and glyoxalate. Model simulations show that more than 50% of the total Fe(Ⅲ) is coordinated by oxalate and up to 20 % of total Fe(Ⅲ) is bound in the newly implemented 1∶1 complexes with tartronate, malonate, and pyruvate. Up to 20% of the total Fe(Ⅲ) is found in hydroxo and sulfato complexes. The fraction of [Fe(oxalate)_2]~- and [Fe(pyruvate)]~(2+) is significantly higher during nighttime than during daytime, which points toward a strong influence of photochemistry on these species. Fe(Ⅲ) complex photolysis is an important additional sink for tartronate, pyruvate, and oxalate, with a complex photolysis contribution to overall degradation of 46,40, and 99%, respectively, compared to all possible sink reactions with atmospheric aqueous-phase radicals, such as ~(*)OH, NO_3~(*), and SO_4~(*). Simulated aerosol particles have a much lower liquid water content than cloud droplets, thus leading to high concentrations of species and, consequently, an enhancement of the photolysis sink reactions in the aerosol particles. The simulations showed that Fe(Ⅲ) photochemistry should not be neglected when considering the fate of carboxylic acids, which constitute a major part of aqueous secondary organic aerosol (aqSOA) in tropospheric cloud droplets and aqueous particles. Failure to consider this loss pathway has the potential to result in a significant overestimate of aqSOA production.
机译：为了量化先进的铁光化学方案的影响，化学水相自由基机理（CAPRAM 3.0i）已通过几种新的Fe（Ⅲ）-羧酸盐络合物光解反应进行了更新。新引入的配体是丙二酸酯，琥珀酸酯，酒石酸酯，酒石酸酯，丙酮酸酯和乙二醛。模型仿真表明，草酸能协调50％以上的Fe（Ⅲ），而新近实现的具有tartronate，丙二酸和丙酮酸的1∶1配合物中最多可结合20％的Fe（Ⅲ）。羟基和硫酸根络合物中的总Fe（Ⅲ）含量高达20％。 [Fe（草酸盐）_2]〜-和[Fe（丙酮酸盐）]〜（2+）在夜间的比例明显高于白天，这表明光化学对这些物种的影响很大。 Fe（Ⅲ）复合光解是酒石酸，丙酮酸和草酸的重要附加吸收剂，与所有可能的与大气水相自由基的吸收反应相比，复杂的光解作用分别使总降解分别为46,40和99％ ，例如〜（*）OH，NO_3〜（*）和SO_4〜（*）。模拟的气溶胶颗粒的液体水含量比云滴低得多，因此导致了高浓度的物种，因此，增强了气溶胶颗粒中的光解吸收反应。模拟表明，考虑到羧酸的命运时，不应忽略Fe（Ⅲ）的光化学，而羧酸是构成对流层云滴和含水颗粒中含水次要有机气溶胶（aqSOA）的主要部分。如果不考虑这种损失途径，则有可能导致aqSOA产量的过高估计。

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  • 来源
    《Environmental Science & Technology》 |2014年第10期|5652-5659|共8页
  • 作者

    Christian Weller; Andreas Tilgner; Peter Braeuer; Hartmut Herrmann;

  • 作者单位

    Leibniz-Institut fuer Troposphaerenforschung, Permoserstrasse 15, 04318 Leipzig, Germany;

    Leibniz-Institut fuer Troposphaerenforschung, Permoserstrasse 15, 04318 Leipzig, Germany;

    Leibniz-Institut fuer Troposphaerenforschung, Permoserstrasse 15, 04318 Leipzig, Germany;

    Leibniz-Institut fuer Troposphaerenforschung, Permoserstrasse 15, 04318 Leipzig, Germany;

  • 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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