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首页> 外文期刊>Environmental Science & Technology >Oxidation of Microcystins by Permanganate: pH and Temperature- Dependent Kinetics, Effect of DOM Characteristics, and Oxidation Mechanism Revisited
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Oxidation of Microcystins by Permanganate: pH and Temperature- Dependent Kinetics, Effect of DOM Characteristics, and Oxidation Mechanism Revisited

机译:高锰酸盐对微囊藻毒素的氧化作用:pH和温度依赖性动力学,DOM特性的影响以及氧化机理的重新研究

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摘要

Oxidative degradation of six representative microcystins (MCs) (MC-RR, -LR, -YR, -LF, -LW, and -LA) by potassium permanganate (KMnO_(4); Mn(VII)) was investigated, focusing on the temperature- and pH-dependent reaction kinetics, the effect of dissolved organic matter (DOM), and the oxidation mechanisms. Second-order rate constants for the reactions of the six MCs with Mn(VII) (k _(Mn(VII),MC)) were determined to be 160.4–520.1 M~(–1) s~(–1) (MC-RR > -LR ≈ -YR > -LF ≈ -LW > -LA) at pH 7.2 and 21 °C. The k _(Mn(VII),MC) values exhibited activation energies ranging from 15.1 to 22.4 kJ mol~(–1). With increasing pH from 2 to 11, the k _(Mn(VII),MC) values decreased until pH 5, and plateaued over the pH range of 5–11, except for that of MC-YR (which increased at pH > 8). Species-specific second-order rate constants were calculated using predicted pK _(a) values of MCs. The oxidation of MCs in natural waters was accurately predicted by the kinetic model using k _(Mn(VII),MC) and Mn(VII) exposure (∫[Mn(VII)]dt) values. Among different characteristics of DOM in natural waters, UV_(254), SUVA_(254), and the abundance of humic-like substances characterized by fluorescence spectroscopy exhibited good correlation with ∫[Mn(VII)]dt. A thorough product study of MC-LR oxidation by Mn(VII) was performed using liquid chromatography–mass spectrometry.
机译:研究了高锰酸钾(KMnO_(4); Mn(VII))对六种代表性微囊藻毒素(MCs)(MC-RR,-LR,-YR,-LF,-LW和-LA)的氧化降解,重点是温度和pH依赖的反应动力学,溶解有机物(DOM)的作用以及氧化机理。六个MC与Mn(VII)(k_(Mn(VII),MC))反应的二级速率常数确定为160.4–520.1 M〜(–1)s〜(–1 )(MC-RR> -LR≈-YR> -LF≈-LW> -LA)在pH 7.2和21°C下。 k_(Mn(VII),MC)值显示出的活化能范围为15.1至22.4 kJ mol〜(–1)。随着pH从2升高到11,k_(Mn(VII),MC)值降低到pH 5,并在5-11的pH范围内达到平稳,MC-YR除外(在pH> 8)。使用MC的预测p iK _(a)值计算特定于物种的二阶速率常数。通过动力学模型,使用k_(Mn(VII),MC)和Mn(VII)暴露(∫[Mn(VII)] dt)值​​,可以通过动力学模型准确预测天然水中MC的氧化。在自然水体中,DOM的不同特征中,UV_(254),SUVA_(254)以及以荧光光谱为特征的大量腐殖质物质与∫[Mn(VII)] dt表现出良好的相关性。使用液相色谱-质谱法对Mn(VII)氧化MC-LR进行了彻底的产物研究。

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  • 来源
    《Environmental Science & Technology》 |2018年第12期|7054-7063|共10页
  • 作者单位

    School of Urban and Environmental Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulju-gun, Ulsan 44919, Republic of Korea;

    School of Urban and Environmental Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulju-gun, Ulsan 44919, Republic of Korea;

    School of Urban and Environmental Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulju-gun, Ulsan 44919, Republic of Korea;

    School of Urban and Environmental Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulju-gun, Ulsan 44919, Republic of Korea;

    School of Urban and Environmental Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulju-gun, Ulsan 44919, Republic of Korea;

  • 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);
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