Kinetics and mechanism of dissolved organic phosphorus (DOP) digestion by the UV/O3 process

IF 1.5 4区 化学 Q4 CHEMISTRY, PHYSICAL
Jialong Zhu, Kaixuan Fang, Mengdi Zhang, Huixuan Chen, Mengfei Zhou, Xiaofang Sun
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Abstract

In this study, the kinetics and mechanism of UV/O3 synergistic oxidative digestion of dissolved organic phosphorus (DOP) were investigated, focusing on the ozone direct oxidation and hydroxyl radical oxidation parts of glufosinate and triphenyl phosphate (TPhP). The p-chlorobenzoic acid (p-CBA) was selected as the probe compound, and two kinds of reaction kinetic models were proposed by competitive kinetic method with Rct according to the different scale of rate constants of hydroxyl radical oxidation. Under the condition of weakly alkaline (pH = 9.0) and weakly acidic environment (pH = 5.0), the second-order rate constants of glufosinate and TPhP was determined indirectly to be ko3/glufosinate = (2.903 ± 0.247)M−1s−1 and ko3/TPhP = (3.307 ± 0.204) M−1s−1 by ozone direct oxidation, and k·OH/glufosinate = (1.257 ± 1.031) × 109 M−1s−1 and k·OH/TPhP = (7.120 × 108 ± 0.963) M−1s−1 by hydroxyl radical oxidation, respectively. The comparison of the contribution levels of the two parts to the digestion process showed that the contribution levels in the digestion of glufosinate and TPhP processes both the contribution of ·OH were higher than those of ozone, 86.3% and 72.6%, respectively.

紫外线/O3 工艺消化溶解有机磷 (DOP) 的动力学和机理
本研究以草铵膦和磷酸三苯酯(TPhP)的臭氧直接氧化和羟基自由基氧化部分为研究对象,探讨了紫外/臭氧协同氧化消解溶解性有机磷(DOP)的动力学和机理。以对氯苯甲酸(p-CBA)为探针化合物,根据羟基自由基氧化速率常数的不同尺度,用 Rct 竞争动力学法提出了两种反应动力学模型。在弱碱性(pH = 9.0)和弱酸性(pH = 5.0)环境条件下,间接测定了草铵膦和 TPhP 的二阶速率常数为 ko3/glufosinate = (2.903 ± 0.247)M-1s-1 和 ko3/TPhP = (3.307 ± 0.204) M-1s-1 ;通过臭氧直接氧化法,k-OH/草铵膦 = (1.257 ± 1.031) × 109 M-1s-1 和 k-OH/TPhP = (7.120 × 108 ± 0.963) M-1s-1 ;通过羟基自由基氧化法,k-OH/草铵膦 = (1.257 ± 1.031) × 109 M-1s-1 和 k-OH/TPhP = (7.120 × 108 ± 0.963) M-1s-1 。两部分对消解过程的贡献水平比较表明,在草铵膦和 TPhP 的消解过程中,-OH 的贡献水平均高于臭氧,分别为 86.3% 和 72.6%。
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来源期刊
CiteScore
3.30
自引率
6.70%
发文量
74
审稿时长
3 months
期刊介绍: As the leading archival journal devoted exclusively to chemical kinetics, the International Journal of Chemical Kinetics publishes original research in gas phase, condensed phase, and polymer reaction kinetics, as well as biochemical and surface kinetics. The Journal seeks to be the primary archive for careful experimental measurements of reaction kinetics, in both simple and complex systems. The Journal also presents new developments in applied theoretical kinetics and publishes large kinetic models, and the algorithms and estimates used in these models. These include methods for handling the large reaction networks important in biochemistry, catalysis, and free radical chemistry. In addition, the Journal explores such topics as the quantitative relationships between molecular structure and chemical reactivity, organic/inorganic chemistry and reaction mechanisms, and the reactive chemistry at interfaces.
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