摘要
本论文主要报道我们在自行设计搭建的红外化学发光的实验装置上,结合商用步进扫描的时间分辨傅立叶变换红外光谱(TR-FTIR)仪,对三种烷基亚硝酸(RONO)类分子(n-C_4H_9ONO,(CH_3)_2C_3H_5ONO,(CH_3)_3CONO)355nm光解动力学、氟甲苯(邻位、对位)的266 nm光解动力学,以及C_2自由基与O_2和CH自由基与醇类分子的反应动力学进行了研究。主要结果如下:
1)n-C_4H_9ONO,(CH_3)_2C_3H_5ONO和(CH_3)_3CONO的355 nm光解,获得了光解产物NO的时间分辨的红外发射谱,对于n-C_4H_9ONO和(CH_3)_2C_3H_5ONO两个分子光解产物NO的转动温度和相对振动布居几乎一致,它们的紫外吸收光谱以及产物NO的时间行为也几乎相同。我们的DT-DFT(B3LYP/6-311G(d,p))计算表明n-C_4H_9ONO中一个γ-H被甲基取代形成(CH_3)_2C_3H_5ONO,对这两个分子的光解动力学行为有着可以忽略的影响,计算结果和我们的实验符合的很好。对(CH_3)_3CONO其光解产物NO发射光谱的分析,获得了NO的转动温度和相对振动布居,并发现了振动布居的反转现象,总结这三个分子的光解实验,我们确认了光解产物NO的最大振动布居量子数(v)与光解光激发的母体分子中N=O伸缩振动的泛频跃迁(0→v~*)所涉及的振动量子数之间的关系是v=v~*-1。
2)邻位和对位氟甲苯的266 nm光解动力学,获得了转动分辨的HF(1≤v≤3)红外发射光谱,在光解邻位氟甲苯后获得的HF(1≤v≤3)的转动布居符合Boltzmann分布,转动温度为785±42K,通过外推得到初生时刻近乎无碰撞条件下的HF转动温度分别为1053±105K,平均转动能量为8.7±0.5KJ/mol。实验获得HF(1≤v≤3)的相对振动布居为:(v=1):(v=2):(v=3)=(0.73):(0.21):(0.06),相应的振动温度:3040±46K。通过Boltzmann分布外推出HF(v=O)的相对振动布居,得到光解产物HF的平均振动能量为29.27kJ/mol。对于对位氟甲苯同样的方法得到光解产物HF的平均转动能量为8.6±0.5 kJ/mol,平均振动能量为26.77kJ/mol。实验观测的相对振动布居:(v=1):(v=2):(v=3)=(0.77):(0.18):(0.05),振动温度为2635±40K。
3)C_2自由基与O_2反应的研究,首次在实验上观测到振动激发的反应产物CO和CO_2。确定了主要反应通道为C_2+O_2→C_2O_2→CO_2+C和C_2+O_2→C_2O_2→2CO。
4)CH自由基与醇类分子(甲醇CH_3OH,乙醇C_2H_5OH,环己醇C_6H_(11)OH)的反应研究,在三个反应中均首次观测到振动激发的产物CO,确定CH自由基与醇类的反应主要是一个插入反应,CH攻击醇中的OH基团,然后插入到O-H键中,主要反应通道为CH+R-OH→R·+CO+H_2.
We designed and set up an experimental equipment for studying the infrared emission of chemical reactions employing Step-Scan time-resolved Fourier Transform Infrared Spectroscopy(TR-FTIR). With TR-FTIR, first, the photodissociation dynamics of alky nitrites (n-C_4H_9ONO, (CH_3)_2C_3H_5ONO, (CH_3)_3CONO) and fluorotoluene (ortho, para) at 355 nm and 266 nm; second, the reaction dynamics of C_2 with O_2 and CH with alcohol (CH_3OH, C_2H_5OH, C_6H_(11)OH) in the gas phase have been studied in this dissertation. The main results are the followings.
1). Photodissociation dynamics of alky nitrites (n-C_4H_9ONO, (CH_3)_2C_3H_5ONO, (CH_3)_3CONO) at 355nm: Photodissociation dynamics study of n-C_4H_9ONO, (CH_3)_2C_3H_5ONO and (CH_3)_3CONO by means of time-resolved Fourier transform infrared (TR-FTIR) emission spectroscopy. The obtained TR-FTIR emission spectra of the nascent NO fragments produced in the 355-nm laser photolysis of the three alkyl nitrite species The nascent NO fragments of n-C_4H_9ONO and (CH_3)_2C_3H_5ONO showed an almost identical rotational temperature and vibrational distributions of NO. In addition, a close resemblance between the two species was also found in the measured temporal profiles of the IR emission of NO and the recorded UV absorption spectra. The experimental results are consistent with our ab initio calculations using the time-dependent density functional theory at the B3LYP/6-311G(d,p) level, which indicate that the substitution of one of the twoγ-H atoms in n-C_4H_9ONO with a methyl group to form (CH_3)_2C_3H_5ONO has only a minor effect on the photodissociation dynamics of the two molecules. By analyzing the observed TR-FTIR emission spectra of the NO fragments produced in the 355-nm laser photolysis of (CH_3)_3CONO), we obtained the rotational temperature and the relative vibrational distribution of NO. In addition, an inversion was found to occur in such a vibrational distribution. With the aid of n-C_4H_9ONO and (CH_3)_2C_3H_5ONO studies, we determined the v = v~* - 1 relationship between the vibrational quantum number of NO corresponding to its maximum vibrational distribution(v) and the vibrational quantum numbers(0→v*) relating to the overtone transitions of the parent molecule.
2). Photodissociation dynamics of o-fluorotoluene at 266 nm: Following the photodissociation of o-fluorotoluene at 266 nm, rotationally resolved emission spectra of HF(1≤v≤3)in the spectral region of 2500-4500 cm-1 are detected with a step-scan TR-FTIR, HF(1≤v≤3) shows nearly Boltzmann-type rotational distributions corresponding to a temperature 785±42K, a short extrapolation from data leads to a nascent rotational temperature of 1053±105K with an average rotational energy of 8.7±0.5KJ/mol The observed vibrational distribution of (v= 1): (v = 2) : (v = 3 ) = (0.73) : (0.21) : (0.06) corresponds to a vibrational temperature of 3040±46K, An average vibrational energy of 29.27 kJ/mol is derived based on the observed population of HF(1≤v≤3) and estimates of the population of HF (v = 0) by extrapolation. Experiments performed on p-fluorotoluene yielded similar results with an average rotational energy of 8.6±0.5 kJ/mol and vibrational energy of 26.77 kJ/mol for HF. The observed vibrational distribution of (v = 1): (v = 2): (v = 3 ) = (0.77): (0.18): (0.05) corresponds to a vibrational temperature of 2635±40K.
3). For the reaction of C_2 + O_2, primary vibrationally excited products CO_2 and CO were observed for the first time. The elementary reaction channels were identified and reaction mechanism was suggested as follows: C_2 + O_2→C_2O_2→CO_2 + C and C_2 + O_2→C_2O_2→2CO.
4). For the reaction of CH with alcohol (CH_3OH, C_2H_5OH, C_6H_(11)OH), primary vibrationally excited products CO were observed in the all reactions for the first time. The most feasible reaction pathway should be CH radical attacking on OH group in alcohol, followed by the insertion of CH into the O-H bond. The elementary reaction channels were: CH + R-OH→R+ CO + H_2
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