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Chemistry of organic nitrogen in atmospheric waters and fine particles.

机译:大气水和细颗粒中有机氮的化学作用。

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摘要

Although a few past studies have found significant quantities of organic nitrogen (ON) in precipitation and dry deposition, not much is known about the atmospheric concentrations, composition, and environmental fates of these compounds. To fill in this gap, this study has focused on quantifying, speciating and characterizing the photochemical transformations of ON compounds in atmospheric water drops and fine particles (PM2.5).; PM2.5 and wintertime fog waters collected from Davis, California were analyzed for inorganic nitrogen species (i.e., NH4 +, NO3, and NO2), ON and free and combined amino compounds. Significant amounts of organic and inorganic N were measured in both types of samples—ON typically accounted for ∼20% of the total N and ∼20% of the total PM2.5 mass. Amino compounds, predominantly in combined forms, generally represented ∼20% of the ON in PM2.5 and fog waters.; We also examined transformations of ON compounds and the simultaneous formation of inorganic N species such as NOx, HNO3/NO 3, and NH3/NH4+ in fog waters during sunlight illumination and O3 exposure. Generally ON was destroyed at initial rates of ∼20 μM per hour, while NH 4+, NO3 and NO x were formed at rates on the order of a few μM per hour. This phototransformation of ON is a previously unrecognized pathway for producing inorganic N in the atmosphere and might significantly affect atmospheric chemistry and the bioavailability of atmospheric deposition.; Another facet of this study was to explore the possible sources of atmospheric nitrogen and phosphorus to a once pristine aquatic ecosystem—Lake Tahoe, California/Nevada. By characterizing the concentrations and speciation of airborne N and P along a transect from the Central Valley of California to the Tahoe basin and at the edge of a forest fire plume, we found that the Central Valley might be a significant source of N to the Tahoe basin during summer and that forest fires could be a significant source of atmospheric N and P to the lake.; Our findings indicate that ON compounds likely play important roles in tropospheric chemistry and that the deposition of ON might significantly affect nutrient balances in ecosystems.
机译:尽管过去的一些研究发现在沉淀和干法沉积中有大量的有机氮(ON),但对这些化合物的大气浓度,组成和环境影响知之甚少。为了填补这一空白,本研究着重于定量,确定和表征大气中的水滴和细颗粒(PM 2.5 )中ON化合物的光化学转化。分析了从加利福尼亚州戴维斯市收集的PM 2.5 和冬季雾水中的无机氮种类(即NH 4 + ,NO 3 -和NO 2 -),ON以及游离和结合的氨基化合物。在这两种类型的样品中都测量到了大量的有机和无机氮,通常,ON占总N的约20%,PM 2.5 的约20%。氨基化合物主要以混合形式存在,在PM 2.5 和雾水中通常占ON的约20%。我们还研究了ON化合物的转化以及无机N物种的同时形成,例如NO x ,HNO 3 / NO 3 - ,以及在阳光照射和O 3 暴露期间雾水中的NH 3 / NH 4 + 。通常,以每小时20μM的初始速率破坏ON,而NH 4 + ,NO 3 -和NO x 的形成速度约为每小时几微米。 ON的这种光转化是在大气中产生无机氮的先前未被认识的途径,并且可能显着影响大气化学和大气沉积物的生物利用度。这项研究的另一个方面是探索曾经原始的水生生态系统(加利福尼亚/内华达州塔霍湖)的大气氮和磷的可能来源。通过描述从加利福尼亚中央谷地到塔霍盆地和森林火灾羽流边缘的一条样带上的空气中氮和磷的浓度和形态,我们发现中央谷地可能是塔霍中氮的重要来源夏季流域,森林大火可能是湖泊中大气氮和磷的重要来源。我们的发现表明,ON化合物可能在对流层化学中起重要作用,ON的沉积可能会显着影响生态系统中的养分平衡。

著录项

  • 作者

    Zhang, Qi.;

  • 作者单位

    University of California, Davis.;

  • 授予单位 University of California, Davis.;
  • 学科 Chemistry Organic.; Chemistry Analytical.; Physics Atmospheric Science.
  • 学位 Ph.D.
  • 年度 2002
  • 页码 p.4183
  • 总页数 230
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 有机化学;
  • 关键词

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