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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Identification and Quantitation of Aerosol Products of the Reaction of β-Pinene with NO3 Radicals and Implications for Gas- and Particle-Phase Reaction Mechanisms
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Identification and Quantitation of Aerosol Products of the Reaction of β-Pinene with NO3 Radicals and Implications for Gas- and Particle-Phase Reaction Mechanisms

机译：β-PinENE反应的鉴定和定量β-Pine烯的反应，没有 3 气体和颗粒 - 相反应机制的影响

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Substantial amounts of gas- and particle-phase organic nitrates have been reported in field studies of atmospheric chemistry conducted around the world, and it has been proposed that a significant fraction of these may be formed from the nighttime reaction of monoterpenes with NO_(3) radicals. In the study presented here, β-pinene (a major global monoterpene emission) was reacted with NO_(3) radicals in an environmental chamber and the molecular and functional group composition of the resulting secondary organic aerosol (SOA) was determined using a variety of methods. Eight products, which comprised ～95% of the SOA mass, were identified and quantified. More than 90% (by mass) of these consisted of acetal heterodimers and heterotrimers that were apparently formed through acid-catalyzed reactions in phase-separated particles. The molar yield of the major oligomer was 16.7%, and the yields of the other six and the single monomer ranged from 1.1% to 2.9%, for a total yield of 30.7%. From these analyses it was determined that the yields of the two major monomer building blocks were 25.9% and 23.6%, and that those of the other four ranged from 2.0% to 4.8%, for a total monomer yield of 62.4%. The measured SOA mass yield was 88.9% and the O/C, N/C, and H/C ratios, molecular weight, and density of the SOA calculated from the results of functional group analysis of the bulk SOA were 0.40, 0.11, 1.79, 217 g mol~(–1), and 1.21 g cm~(–3), respectively, similar to values estimated from results of molecular analysis. The results demonstrate the combined importance of RO_(2)~(?) + RO_(2)~(?) reactions, alkoxy radical decomposition and isomerization, and acid-catalyzed particle-phase reactions in the NO_(3) radical-initiated oxidation of β-pinene and subsequent formation of SOA and should be useful for understanding reactions of other monoterpenes and for developing models for the laboratory and atmosphere.
机译：已经报道了大量的气体和颗粒 - 相硝酸盐在世界各地进行的大气化学研究中，并且已经提出了这些大部分可以从单口的夜间反应与NO_（3）形成自由基。在此提出的研究中，β-脊烯（主要全球单萜发射）与环境室中的NO_（3）基团反应，并且使用各种各样的方法测定所得的二次有机气溶胶（SOA）的分子和官能团组合物方法。鉴定和量化八种占SOA质量〜95％的产品。这些超过90％（质量）由缩醛异二聚体和杂偶联体组成，其明显通过相分离的颗粒中的酸催化反应形成。主要低聚物的摩尔产量为16.7％，另外六个和单体的产率为1.1％至2.9％，总收率为30.7％。从这些分析中，确定两个主要单体构建块的产量为25.9％和23.6％，另一个四个的产量为2.0％至4.8％，总单体产量为62.4％。测量的SOA质量产量为88.9％，SOA的O / C，N / C和H / C比率，分子量和密度从散装SOA的官能团分析结果计算的SOA为0.40,0.11,1.79 ，分别为217g mol〜（-1）和1.21g cm〜（-3），类似于来自分子分析结果估计的值。结果证明了RO_（2）〜（？）+ RO_（2）〜（2）反应，烷氧基分解和异构化的同一重要性，以及NO_（3）激发氧化中的酸催化的颗粒反应β-脊烯和随后形成SOA，也可用于了解其他单层的反应以及为实验室和大气开发模型。

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