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Phenols and Amine Induced HO~· Generation During the Initial Phase of Natural Water Ozonation

机译:天然水臭氧化初期苯酚和胺类诱导HO〜·的产生

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摘要

The initial phase of ozone decomposition in natural water (t < 20 s) is poorly understood. It has recently been shown to result in very high transient HO~· concentrations and, thereby, plays an essential role during processes such as bromateformation or contaminants oxidation. Phenols and amines are ubiquitous moieties of natural organic matter. Naturally occurring concentrations of primary, secondary, and tertiary amines, amino acids, and phenol were added to surface water, and ozone decomposition as well as HO~· generation were measured starting 350 milliseconds after ozone addition. Six seconds into the process, 5 μM of dimethylamine and phenol had generated ∫HO~·dt = 1 x 10~(-10) M·s and 1.8 x 10~(-10) M·s, respectively. With 10 μM dimethylamine and 1.5 mgO_3/L, R_(ct), (∫HO~·dt/ ∫O_3dt) reached 10~(-6), which is larger than in advanced oxidation processes (AOP) such as O_3/H_2O_2. Experiments in the presence of HO~·-scavengers indicated that a significant fraction of phenol-induced ozone decomposition and HO~· generation results from a direct electron transfer to ozone. For dimethylamine, the main mechanism of HO~· generation is direct formation of O_2~(·-) which reacts selectively with O_3 to form O_3~(·-). Pretreatment of phenol-containing water with HOCl or HOBr did not decrease HO~· generation, while the same treatment of dimethylamine-containing water considerably reduced HO~· generation.
机译:天然水中臭氧分解的初始阶段(t <20 s)了解甚少。近来已证明其导致非常高的瞬时HO-浓度,并因此在诸如溴酸酯化或污染物氧化的过程中起着至关重要的作用。酚和胺是天然有机物的普遍组成部分。将天然存在的伯,仲和叔胺,氨基酸和苯酚的浓度添加到地表水中,并在添加臭氧后的350毫秒内测量臭氧的分解以及HO〜·的产生。进入过程六秒钟,分别产生5μM的二甲胺和苯酚∫HO〜·dt = 1 x 10〜(-10)M·s和1.8 x 10〜(-10)M·s。在10μM二甲胺和1.5 mgO_3 / L下,R_(ct)的(∫HO〜·dt /∫O_3dt)达到10〜(-6),这比诸如O_3 / H_2O_2的高级氧化工艺(AOP)更大。在存在HO〜·清除剂的情况下进行的实验表明,苯酚诱导的臭氧分解和HO〜·的产生的很大一部分是由于电子直接转移到臭氧中所致。对于二甲胺,HO〜·生成的主要机理是直接形成O_2〜(·-),O_2〜(·-)与O_3选择性反应形成O_3〜(·-)。用HOCl或HOBr预处理含苯酚的水不会降低HO〜·的生成,而对含二甲胺的水进行相同的处理则可以大大减少HO〜·的生成。

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  • 来源
    《Environmental Science & Technology》 |2006年第9期|p.3057-3063|共7页
  • 作者单位

    Swiss Federal Institute of Aquatic Science & Technology (EAWAG), Uberlandstrasse 133, Postfach 611, CH-8600 Dubendorf, Switzerland;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 环境化学;
  • 关键词

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