Kinetic studies of excited singlet oxygen atom O( 1 D) reactions with ethanol
Kinetic studies of excited singlet oxygen atom O( 1 D) reactions with ethanol
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激发态单线态氧原子O(1D)与乙醇反应的动力学研究
DOI：
10.1002/kin.21474
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发表时间：
2021
影响因子：
1.5
通讯作者：
Ju, Yiguang
中科院分区：
文献类型：
--
作者：
Zhong, Hongtao;Yan, Chao;Teng, Chu C.;Chen, Timothy Y.;Wysocki, Gerard;Ju, Yiguang
在光解流动反应器中，采用中红外法拉第旋转光谱（FRS）和紫外-红外直接吸收光谱（DAS），在297 K，反应器压力分别为60、120和150 Torr（He浴）的条件下，研究了激发态单重态氧原子与乙醇（O（1D）+C2 H5 OH（1））的多通道反应。在266 nm处，O3的光解产生了激发态单重态氧原子。基于O3耗尽的原位光化测量法测定了光子通量和O（1D）浓度。通过DAS信号监测OH和H2O的时间分布。3568.62和3568.29 cm-1，而HO 2的时间分布是通过大约3568.62和3568.29 cm-1的FRS信号测量的。1396.90 cm−1。目标反应（1）的分支比通过将时间曲线拟合到内部反应机制的模拟来确定。两个主要反应通道分别为CH 3CHOH + OH和CH 3 O + CH 2 OH，其分支比分别为0.46 ± 0.12和0.42 ± 0.11。在低温范围内，HO 2和O2 CH 2CH 2 OH（β-RO 2）之间的特定HO 2 + RO 2反应在本工作中被估计为HO 2 + O2 CH 2CH 2 OH产物，速率常数为7 × 10− 12 cm 3 molecule − 1 s −1。
The multichannel reaction of excited singlet oxygen atom with ethanol, O(1D) + C2H5OH (1), was studied in a photolysis flow reactor coupled with mid‐infrared Faraday rotation spectroscopy (FRS) and UV‐IR direct absorption spectroscopy (DAS) at 297 K with reactor pressures of 60, 120, and 150 Torr (bath He). The excited singlet oxygen atom was generated through the photolysis of O3at 266 nm. The photon flux and O(1D) concentrations were determined by in situ actinometry based on O3depletion. Temporal profiles of OH and H2O were monitored via DAS signals at ca. 3568.62 and 3568.29 cm−1, while temporal profiles of HO2were measured via FRS signals at ca. 1396.90 cm−1. The branching ratios of the target reaction (1) were determined by fitting temporal profiles to simulations from an in‐house reaction mechanism. Two major reaction channels were identified as CH3CHOH + OH and CH3O + CH2OH, and their branching ratios were determined as 0.46 ± 0.12 and 0.42 ± 0.11, respectively. A specific HO2+ RO2reaction between HO2and O2CH2CH2OH (β‐RO2) at the low‐temperature range is estimated in this work as HO2+ O2CH2CH2OH products with a rate constant of 7 × 10−12cm3molecule−1s−1.