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Impact of Criegee Intermediate Reactions with Peroxy Radicals on Tropospheric Organic Aerosol
ACS Earth and Space Chemistry ( IF 2.9 ) Pub Date : 2020-08-26 , DOI: 10.1021/acsearthspacechem.0c00147 Rabi Chhantyal-Pun 1 , M. Anwar H. Khan 1 , Nicholas Zachhuber 1 , Carl J. Percival 2 , Dudley E. Shallcross 1 , Andrew J. Orr-Ewing 1
ACS Earth and Space Chemistry ( IF 2.9 ) Pub Date : 2020-08-26 , DOI: 10.1021/acsearthspacechem.0c00147 Rabi Chhantyal-Pun 1 , M. Anwar H. Khan 1 , Nicholas Zachhuber 1 , Carl J. Percival 2 , Dudley E. Shallcross 1 , Andrew J. Orr-Ewing 1
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Peroxy radicals and carbonyl oxides (Criegee intermediates) are produced in the troposphere during OH and ozone-initiated oxidation of hydrocarbons. Reactions between these species have previously been shown to form highly oxidized molecules which can condense to form secondary organic aerosols. Here, cavity ring-down spectroscopy coupled with laser flash photolysis was used to measure directly rate coefficients for reactions of CH2OO with CH3O2 and CH3C(O)O2. The rate coefficients were found to be similar within the measurement uncertainties and only weakly dependent on temperature (in the range 243–310 K) and pressure (20–100 Torr, N2). A combined rate coefficient of k (CH2OO + RO2, RO2 = CH3O2/CH3C(O)O2) = (2.4 ± 1.2) × 10–11 cm3 molecule–1 s–1 was obtained under these conditions. Global modeling using STOCHEM-CRI, updated with monoterpene chemistry generating Criegee intermediates and supplemented by regional box modeling, shows that this class of Criegee intermediate + peroxy radical reactions can contribute up to ∼1.3% of secondary organic aerosol production in forested regions of the world.
中文翻译：
Criegee与过氧自由基的中间反应对对流层有机气溶胶的影响
在OH和臭氧引发的烃氧化过程中，对流层中会产生过氧自由基和羰基氧化物（Criegee中间体）。这些物质之间的反应先前已显示形成高度氧化的分子，这些分子可凝结形成二次有机气溶胶。在这里，腔衰荡光谱结合激光闪光光解法被用来直接测量CH 2 OO与CH 3 O 2和CH 3 C（O）O 2反应的速率系数。发现速率系数在测量不确定度内相似，仅在很小的程度上取决于温度（在243–310 K范围内）和压力（20–100 Torr，N 2）。综合费率系数为在这些条件下，得到的k（CH 2 OO + RO 2，RO 2 = CH 3 O 2 / CH 3 C（O）O 2）=（2.4±1.2）×10 –11 cm 3分子–1 s –1。使用STOCHEM-CRI进行的全球建模，通过生成萜烯中间体的单萜化学进行了更新，并通过区域盒式建模进行了补充，表明该类别的Criegee中间体+过氧自由基反应可占世界森林地区次级有机气溶胶产量的约1.3％ 。
更新日期：2020-10-16
中文翻译：
Criegee与过氧自由基的中间反应对对流层有机气溶胶的影响
在OH和臭氧引发的烃氧化过程中，对流层中会产生过氧自由基和羰基氧化物（Criegee中间体）。这些物质之间的反应先前已显示形成高度氧化的分子，这些分子可凝结形成二次有机气溶胶。在这里，腔衰荡光谱结合激光闪光光解法被用来直接测量CH 2 OO与CH 3 O 2和CH 3 C（O）O 2反应的速率系数。发现速率系数在测量不确定度内相似，仅在很小的程度上取决于温度（在243–310 K范围内）和压力（20–100 Torr，N 2）。综合费率系数为在这些条件下，得到的k（CH 2 OO + RO 2，RO 2 = CH 3 O 2 / CH 3 C（O）O 2）=（2.4±1.2）×10 –11 cm 3分子–1 s –1。使用STOCHEM-CRI进行的全球建模，通过生成萜烯中间体的单萜化学进行了更新，并通过区域盒式建模进行了补充，表明该类别的Criegee中间体+过氧自由基反应可占世界森林地区次级有机气溶胶产量的约1.3％ 。
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