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臭氧和羟基自由基氧化苯并三唑的动力学。

Kinetic of benzotriazole oxidation by ozone and hydroxyl radical.

机构信息

Université de Poitiers, CNRS, Laboratoire de Chimie et Microbiologie de l'Eau (UMR 6008), Ecole Supérieure d'Ingénieurs de Poitiers, 40 avenue du Recteur Pineau, 86022 Poitiers Cedex, France.

出版信息

Water Res. 2010 Mar;44(6):2058-66. doi: 10.1016/j.watres.2009.12.018. Epub 2009 Dec 16.

Abstract

Ozonation experiments were performed in batch reactors in order to determine the rate constants for the reaction of molecular ozone and OH radicals with benzotriazole (BT) at different pHs. The first group of ozonation experiments was carried out for the determination of the rate constant for the direct reactions between ozone and BT. Two different kinetic models were used for the determination of kinetic rate constants: (i) the log-reduction of BT with ozone in excess, (ii) the competition kinetic model. The second-order rate constants for BT with molecular ozone were determined to be 36.4+/-3.8M(-1) s(-1) and 18.4+/-0.8M(-1) s(-1) at pH 2 from the two methods respectively. With the competition method, the value at pH 5 was found to be 22.0+/-2.0M(-1) s(-1). In a following stage, the reaction of BT with OH radicals was investigated at pH values ranging from 2 to 10.2. Using a method involving two probe compounds during the ozonation, the second-order rate constants of the BT reaction with hydroxyl radicals were determined. The rate constants were found to vary from 6.2x10(9)M(-1) s(-1) at pH 10.2 to 1.7x10(10)M(-1) s(-1) at pH 2.

摘要

进行了一系列臭氧反应实验,以确定在不同 pH 值下分子臭氧与苯并三唑(BT)的反应的速率常数。第一组臭氧反应实验是为了确定臭氧与 BT 之间的直接反应的速率常数。使用了两种不同的动力学模型来确定动力学速率常数:(i)臭氧过量时 BT 的对数减少,(ii)竞争动力学模型。通过这两种方法,分别在 pH 2 下确定了与分子臭氧的 BT 的二级速率常数为 36.4+/-3.8M(-1) s(-1)和 18.4+/-0.8M(-1) s(-1)。使用竞争方法,在 pH 5 时发现的值为 22.0+/-2.0M(-1) s(-1)。在随后的阶段,在 pH 值范围从 2 到 10.2 时研究了 BT 与 OH 自由基的反应。通过在臭氧反应过程中使用两种探针化合物的方法,确定了 BT 与羟基自由基的反应的二级速率常数。发现这些速率常数从 pH 值为 10.2 时的 6.2x10(9)M(-1) s(-1)变化到 pH 值为 2 时的 1.7x10(10)M(-1) s(-1)。

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