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首页> 外文学位 >Observations of nitrites, peroxy nitrates, alkyl nitrates, nitric acid , and total nitrogen oxides in Houston, Texas: Implications for ozone photochemistry.
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Observations of nitrites, peroxy nitrates, alkyl nitrates, nitric acid , and total nitrogen oxides in Houston, Texas: Implications for ozone photochemistry.

机译：在德克萨斯州休斯顿的亚硝酸盐，过氧硝酸盐，硝酸烷基酯，硝酸和总氮氧化物的观测：对臭氧光化学的影响。

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In the troposphere, the oxidation of NO to NO2 is controlled by catalytic cycles that are coupled to the photochemical oxidation of hydrocarbons. These chemical cycles control the rate of O3 production. In this thesis, I describe novel in situ measurements aimed at improving our understanding the chemistry effecting the removal of NO and NO2 from the reactive pool of chemicals.; Measurements of NO2, SigmaPNs, SigmaANs, and HNO 3 by TD-LIF are described along with a comprehensive evaluation of the measurement accuracy. Secondary chemical effects in the TD-LIF inlet are examined using laboratory and field experiments in Chapter 2. The results show that SigmaPN, SigmaAN, and HNO3 measurements can be obtained with an accuracy of +/-15--20% over a wide range of atmospheric conditions. Comparison of SigmaPNs and the total available reactive nitrogen to other measurements are described in Chapters 3 and 4. The measurements agree to within 6% on average during the daytime and are almost always within their combined uncertainties (+/-15% each, +/-21% total). These three chapters provide strong evidence that TD-LIF is accurate with the capability of making observations at any location on Earth.; In Chapter 5 I describe measurements and analysis of SigmaANs. These compounds are formed in the same chemical channel as O3. TD-LIF measurements are the first observations of SigmaANs. At La Porte, mixing ratios of SigmaANs are nearly ten times larger than previous measurements of SigmaRONO2,i in other locations, with a midday median value of 1.2 ppbv. The observed correlation between Ox and SigmaANs has a slope that increases from 29 (R2 = 0.73) DeltaO x/DeltaSigmaANs at 0900--1200 CDT to 41 (R2 = 0.74) DeltaOx/DeltaSigmaANs at 1400--1800 CDT. Calculations constrained by simultaneous hydrocarbon observations demonstrate that the magnitude of the SigmaANs mixing ratio and the correlation of SigmaANs with Ox are to be expected based on reported branching ratios for alkyl nitrate formation in the RO2 + NO reaction. Chapter 6 demonstrates the implication of climate change for O3 production rates with specific emphasis on the roles of VOC and alkyl nitrate production.
机译：在对流层中，NO氧化为NO2的过程是由催化循环控制的，催化循环与烃类的光化学氧化有关。这些化学循环控制O3的产生速率。在这篇论文中，我描述了新颖的原位测量，旨在增进我们对影响从化学反应池中去除NO和NO2的化学的理解。描述了通过TD-LIF测量NO2，SigmaPNs，SigmaANs和HNO 3以及对测量精度的综合评估。使用第2章中的实验室和现场实验检查了TD-LIF入口中的二次化学作用。结果表明，可以在宽范围内以+/- 15--20％的精度获得SigmaPN，SigmaAN和HNO3的测量值。大气条件。第3章和第4章介绍了SigmaPNs和总可用反应性氮与其他测量值的比较。白天的测量值平均在6％以内，并且几乎始终在其合并的不确定性范围内（每次+/- 15％，+ /-总计-21％）。这三章提供了有力的证据，表明TD-LIF具有在地球上任何位置进行观测的能力都是准确的。在第5章中，我描述了SigmaAN的测量和分析。这些化合物在与O3相同的化学通道中形成。 TD-LIF测量是SigmaAN的首次观察。在拉波特（La Porte），SigmaANs的混合比几乎是先前在其他位置测量的SigmaRONO2，i的十倍，中位值为1.2 ppbv。 Ox和SigmaAN之间观察到的相关性具有从0900--1200 CDT时的29（R2 = 0.73）DeltaO x / DeltaSigmaANs到1400--1800 CDT时的41（R2 = 0.74）DeltaOx / DeltaSigmaANs的斜率增加。由同时进行的烃观测所限制的计算表明，基于报道的RO2 + NO反应中烷基硝酸盐形成的支化比，可以预期SigmaANs混合比的大小以及SigmaANs与Ox的相关性。第6章展示了气候变化对O3生产率的影响，特别强调了VOC和硝酸烷基酯生产的作用。

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