Faculty of Industrial Chemistry and Environmental Engineering, University "Politehnica" of Timişoara Bulevardul Vasile Pârvan Nr. 6, 300223 Timişoara, Romania.
Westfälische Hochschule Gelsenkirchen, Neidenburger Strasse 43, 45877 Gelsenkirchen, Germany.
Int J Mol Sci. 2019 Aug 26;20(17):4165. doi: 10.3390/ijms20174165.
The main aim of this work is to substantiate the mechanism of 1-propanol oxidation by ozone in aqueous solution when the substrate is present in large excess. Further goals are assessment of the products, their formation yields as well as the kinetic parameters of the considered reaction. The reaction of ozone with 1-propanol in aqueous solution occurs via hydride transfer, H-abstraction and insertion. Of these three mechanisms, the largest share is for hydride transfer. This implies the extraction of an hydride ion from the activated C-H group by O according to reaction: (CH)(H)(HO)C-H + O → [(CH)(H)(HO)C + HO] → (CH)(H)(HO)C + HO. The experimentally determined products and their overall formation yields with respect to ozone are: propionaldehyde-(60 ± 3)%, propionic acid-(27.4 ± 1.0)%, acetaldehyde-(4.9 ± 0.3)%, acetic acid-(0.3 ± 0.1)%, formaldehyde-(1.0 ± 0.1)%, formic acid-(4.6 ± 0.3)%, hydrogen peroxide-(11.1 ± 0.3)% and hydroxyl radical-(9.8 ± 0.3)%. The reaction of ozone with 1-propanol in aqueous media follows a second order kinetics with a reaction rate constant of (0.64 ± 0.02) M·s at pH = 7 and 23 °C. The dependence of the second order rate constant on temperature is described by the equation: l n k I I = ( 27.17 ± 0.38 ) - ( 8180 ± 120 ) × T - 1 , which gives the activation energy, Ea = (68 ± 1) kJ mol and pre-exponential factor, A = (6.3 ± 2.4) × 10 M s. The nature of products, their yields and the kinetic data can be used in water treatment. The fact that the hydride transfer is the main pathway in the 1-propanol/ozone system can probably be transferred on other systems in which the substrate is characterized by C-H active sites only.
这项工作的主要目的是在底物大量过剩的情况下,证实臭氧在水溶液中氧化 1-丙醇的反应机制。进一步的目标是评估产物、它们的生成产率以及所考虑反应的动力学参数。臭氧与水溶液中的 1-丙醇反应通过氢化物转移、H-抽提和插入进行。在这三种机制中,氢化物转移占据最大份额。这意味着 O 从活化的 C-H 基团中提取一个氢化物离子,根据反应式:(CH)(H)(HO)C-H + O → [(CH)(H)(HO)C + HO] → (CH)(H)(HO)C + HO。实验确定的产物及其相对于臭氧的总生成产率为:丙醛-(60 ± 3)%、丙酸-(27.4 ± 1.0)%、乙醛-(4.9 ± 0.3)%、乙酸-(0.3 ± 0.1)%、甲醛-(1.0 ± 0.1)%、甲酸-(4.6 ± 0.3)%、过氧化氢-(11.1 ± 0.3)%和羟基自由基-(9.8 ± 0.3)%。臭氧在水介质中与 1-丙醇的反应遵循二级动力学,在 pH = 7 和 23°C 时,反应速率常数为(0.64 ± 0.02) M·s。二级速率常数对温度的依赖性由方程描述:l n k I I = ( 27.17 ± 0.38 ) - ( 8180 ± 120 ) × T - 1 ,这给出了活化能 Ea = (68 ± 1) kJ mol 和指前因子 A = (6.3 ± 2.4) × 10 M s。产物的性质、产率和动力学数据可用于水处理。氢化物转移是 1-丙醇/臭氧体系中的主要途径,这一事实可能适用于其他底物仅具有 C-H 活性位点的体系。