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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Atmospheric Oxidation of Toluene in a Large-Volume Outdoor Photoreactor: In Situ Determination of Ring-Retaining Product Yields
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Atmospheric Oxidation of Toluene in a Large-Volume Outdoor Photoreactor: In Situ Determination of Ring-Retaining Product Yields

机译：大型室外光反应器中甲苯的大气氧化：环保留产物收率的原位测定

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摘要

Experiments on the photooxidation of toluene/NO_x/air mixtures were performed in the European Photoreactor (EUPHORE), a large-scale outdoor reaction chamber located in Valencia/Spain. The objective of the study was the in situ determination of the yields of ring-retaining products by differential optical absorption spectroscopy (DOAS) and the elucidation of their formation pathways. The experiments were performed with toluene concentrations between 0.68 and 3.85 ppm and initial NO_x concentrations ranging from 3 to 300 ppb, i.e., down to the range actually observed in the lower atmosphere. The ring-retaining product yields were found to be 5.8 ± 0.8%, 12.0 ± 1.4%, 2.7 ± 0.7%, and 3.2 ± 0.6% for benzaldehyde, o-cresol, m-cresol, and p-cresol, respectively. Under the experimental conditions, no dependency of the yields on the NO_x concentration or the toluene/NO_x ratio could be found. The formation kinetics of the cresols are in line with a "prompt" formation mechanism, i.e., abstraction of a hydrogen atom from the toluene-OH adduct (toluene-OH + O_2 → cresols + HO_2). In addition, substantial evidence was found that reaction with NO_3 radicals represents an important sink for cresols in smog chamber studies conducted under conditions of NO_x concentrations above the range observed in the troposphere, possibly also under tropospheric conditions.
机译：甲苯/ NO_x /空气混合物的光氧化实验是在欧洲光反应器（EUPHORE）中进行的，该反应器是位于西班牙瓦伦西亚的大型室外反应室。该研究的目的是通过差示光吸收光谱法（DOAS）原位确定环保持产物的产率并阐明其形成途径。实验是在0.68至3.85 ppm的甲苯浓度和3至300 ppb的初始NO_x浓度范围内进行的，即低至在较低大气中实际观察到的范围。发现苯甲醛，邻甲酚，间甲酚和对甲酚的环保持产物产率分别为5.8±0.8％，12.0±1.4％，2.7±0.7％和3.2±0.6％。在实验条件下，没有发现产率对NO_x浓度或甲苯/ NO_x比率的依赖性。甲酚的形成动力学符合“迅速”的形成机理，即从甲苯-OH加合物（甲苯-OH + O_2→甲酚+ HO_2）中提取氢原子。另外，在NO_x浓度高于对流层范围内观察到的条件下（可能也在对流层条件下）进行的烟雾试验中，与NO_3自由基的反应代表了对甲酚的重要吸收。

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