Photosensitizing and Inhibitory Effects of Ozonated Dissolved Organic Matter on Triplet-Induced Contaminant Transformation

化学 溶解有机碳 反应速率常数 磺胺 光化学 吸光度 磺胺嘧啶 发色团 激进的 转化(遗传学) 环境化学 有机化学 动力学 色谱法 生物化学 抗生素 物理 量子力学 基因
作者
Jannis Wenk,Michael Aeschbacher,Michael Sander,Urs von Gunten,Silvio Canonica
出处
期刊:Environmental Science & Technology [American Chemical Society]
卷期号:49 (14): 8541-8549 被引量:88
标识
DOI:10.1021/acs.est.5b02221
摘要

Dissolved organic matter (DOM) is both a promoter and an inhibitor of triplet-induced organic contaminant oxidation. This dual role was systematically investigated through photochemical experiments with three types of DOM of terrestrial and aquatic origins that were preoxidized to varying extents by ozonation. The inhibitory effect of DOM was assessed by determining the 4-carboxybenzophenone photosensitized transformation rate constants of two sulfonamide antibiotics (sulfamethoxazole and sulfadiazine) in the presence of untreated or preoxidized DOM. The inhibitory effect decreased with the increasing extent of DOM preoxidation, and it was correlated to the loss of phenolic antioxidant moieties, as quantified electrochemically, and to the loss of DOM ultraviolet absorbance. The triplet photosensitizing ability of preoxidized DOM was determined using the conversion of the probe compound 2,4,6-trimethylphenol (TMP), which is unaffected by DOM inhibition effects. The DOM photosensitized transformation rate constants of TMP decreased with increasing DOM preoxidation and were correlated to the concomitant loss of chromophores (i.e., photosensitizing moieties). The combined effects of DOM preoxidation on the inhibiting and photosensitizing properties were assessed by phototransformation experiments of the sulfonamides in DOM-containing solutions. At low extents of DOM preoxidation, the sulfonamide phototransformation rate constants remained either unchanged or slightly increased, indicating that the removal of antioxidant moieties had larger effects than the loss of photosensitizing moieties. At higher extents of DOM preoxidation, transformation rates declined, mainly reflecting the destruction of photosensitizing moieties.
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