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Influence of dissolved organic carbon on photochemically mediated cycling of hydrogen peroxide in rainwater

机译：溶解有机碳对雨水中过氧化氢的光化学介导循环的影响

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摘要

The influence of sunlight and dissolved organic carbon (DOC) on the photochemically mediated cycling of hydrogen peroxide (H_2O_2) was investigated in rainwater samples collected in Wilmington, North Carolina USA. Upon exposure to simulated sunlight 14 of 19 authentic rainwater samples exhibited significant decreases in H_2O_2. The concentration of hydrogen peroxide did not change significantly in organic-free synthetic rainwater spiked with H_2O_2 in the light or in dark controls suggesting that the loss was not due to direct photolysis or dark mediated reactions. There was a significant correlation between pseudo-first order rate constants of H_2O_2 decay and initial H_2O_2 concentrations. There was also a significant correlation between the rate constant and the abundance of DOC suggesting that rainwater organic carbon plays an important role during photolytic decay either via direct reaction or indirectly through production of peroxide reactive species or scavenging of peroxide generating radicals. Several rain samples exhibited an initial increase in H_2O_2 during the first 2 h of irradiation. These increases were generally small and most likely do not represent a significant input of peroxide in precipitation. The photo-induced destruction of H_2O_2 is important because it may partly explain the late afternoon decrease of peroxide concentrations observed in earlier field studies and the substantial under saturation (<10%) of this oxidant in rainwater compared with gas phase concentrations.
机译：在美国北卡罗来纳州威明顿市收集的雨水样品中，研究了阳光和溶解的有机碳（DOC）对光化学介导的过氧化氢（H_2O_2）循环的影响。在19个真实的雨水样品中，有14个暴露在模拟的阳光下，H_2O_2明显降低。在光照或黑暗对照中加有H_2O_2的不含有机物的合成雨水中，过氧化氢的浓度没有显着变化，表明该损失不是由于直接光解或黑暗介导的反应引起的。 H_2O_2衰变的拟一级反应速率常数与初始H_2O_2浓度之间存在显着相关性。速率常数与DOC含量之间也存在显着相关性，这表明雨水有机碳在光解衰变过程中起着重要作用，这可以通过直接反应或通过产生过氧化物反应性物种或清除过氧化物生成自由基来间接进行。在辐照的最初2小时内，一些雨水样品显示出H_2O_2的初始增加。这些增加通常很小，最有可能不代表沉淀中过氧化物的大量输入。 H_2O_2的光诱导破坏很重要，因为它可以部分解释早期田间研究中观察到的午后过氧化物浓度降低以及与气相浓度相比该氧化剂在雨水中的饱和度低于饱和（<10％）的现象。

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  • 来源
    《Journal of Atmospheric Chemistry》 |2009年第3期|p.149-158|共10页
  • 作者

    Robert J. Kieber; Jeremy Smith; Katherine M. Mullaugh; Melissa W. Southwell; G. Brooks Avery Jr.; Joan D. Willey;

  • 作者单位

    Department of Chemistry and Biochemistry, University of North Carolina Wilmington,601 S. College Rd., Wilmington, NC 28403, USA;

    rnDepartment of Chemistry and Biochemistry, University of North Carolina Wilmington,601 S. College Rd., Wilmington, NC 28403, USA;

    rnDepartment of Chemistry and Biochemistry, University of North Carolina Wilmington,601 S. College Rd., Wilmington, NC 28403, USA;

    rnDepartment of Chemistry and Biochemistry, University of North Carolina Wilmington,601 S. College Rd., Wilmington, NC 28403, USA;

    rnDepartment of Chemistry and Biochemistry, University of North Carolina Wilmington,601 S. College Rd., Wilmington, NC 28403, USA;

    rnDepartment of Chemistry and Biochemistry, University of North Carolina Wilmington,601 S. College Rd., Wilmington, NC 28403, USA;

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  • 原文格式 PDF
  • 正文语种 eng
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  • 关键词

    hydrogen peroxide; rainwater; photochemistry;

    机译：过氧化氢雨水;光化学;

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