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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Kinetics of the Gas Phase Reactions of the Criegee Intermediate CH2OO with O-3 and IO
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Kinetics of the Gas Phase Reactions of the Criegee Intermediate CH2OO with O-3 and IO

机译：用O-3和IO的Criegee中间体CH2OO气相反应的动力学

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摘要

The kinetics of the gas phase reactions of the Criegee intermediate CH2OO with O-3 and IO have been studied at 296 K and 300 Torr through simultaneous measurements of CH2OO, the CH2OO precursor (CH2I2), O-3, and IO using flash photolysis of CH2I2/O-2/O-3/N-2 mixtures at 248 nm coupled to time-resolved broadband UV absorption spectroscopy. Experiments were performed under pseudo-first-order conditions with respect to O-3, with the rate coefficients for reactions of CH2OO with O-3 and IO obtained by fitting to the observed decays of CH2OO using a model constrained to the measured concentrations of IO. Fits were performed globally, with the ratio between the initial concentration of O-3 and the average concentration of IO varying in the range 30-700, and gave k(CH)(2OO+)(O3)( )= (3.6 +/- 0.8) x 10(-13) cm(3) molecule(-1) s(-1) and k(CH)(2OO+)(IO) = (7.6 +/- 1.4) x 10(-11) cm(3) molecule(-1) s(-1) (where the errors are at the 2 sigma level). The magnitude of k(CH)(2OO+O3) has a significant effect on the steady state concentration of CH2OO in chamber studies. Atmospheric implications of the results are discussed.
机译：通过同时测量CH2OO，CH2OO前体（CH2I2），O-3和IO的同时测量使用闪光光解，在296k和300托的中，使用闪光光解的同时测量克莱通中间体CH2OO与O-3和IO的气相反应。 CH2I2 / O-2 / O-3 / N-2混合物在248nm时，耦合到时间分辨的宽带UV吸收光谱。在伪第一阶条件下进行实验，相对于O-3进行，通过使用约束的模型对所观察到的CH2OO的衰变而获得的CH2OO和IO的速率系数。 。在全球范围内进行拟合，其初始浓度与30-700范围内的I-3的平均浓度与IO的平均浓度之间的比率，并给予k（CH）（2oo +）（O3）（）=（3.6 +/- 0.8）×10（-13）厘米（3）分子（-1）S（-1）和K（CH）（2oo +）（IO）=（7.6 +/- 1.4）×10（-11）cm（3 ）分子（-1）s（-1）（误差在2个σ水平）。 K（CH）（2oo + O3）的幅度对腔室研究中CH2OO的稳态浓度有显着影响。讨论了结果的大气意义。

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