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二甲亚砜捕获-高效液相色谱测定天然水体中羟基自由基的光化学生成

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邰超, 韩丹, 阴永光, 赵同谦, 王静. 二甲亚砜捕获-高效液相色谱测定天然水体中羟基自由基的光化学生成[J]. 环境化学, 2015, 34(2): 212-218. doi: 10.7524/j.issn.0254-6108.2015.02.2014061202
引用本文: 邰超, 韩丹, 阴永光, 赵同谦, 王静. 二甲亚砜捕获-高效液相色谱测定天然水体中羟基自由基的光化学生成[J]. 环境化学, 2015, 34(2): 212-218. doi: 10.7524/j.issn.0254-6108.2015.02.2014061202
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TAI Chao, HAN Dan, YIN Yongguang, ZHAO Tongqian, WANG Jing. Determination of photogenerated hydroxyl radicals in natural water by high performance liquid chromatography after trapping with dimethyl sulfoxide[J]. Environmental Chemistry, 2015, 34(2): 212-218. doi: 10.7524/j.issn.0254-6108.2015.02.2014061202
Citation: TAI Chao, HAN Dan, YIN Yongguang, ZHAO Tongqian, WANG Jing. Determination of photogenerated hydroxyl radicals in natural water by high performance liquid chromatography after trapping with dimethyl sulfoxide[J]. Environmental Chemistry, 2015, 34(2): 212-218. doi: 10.7524/j.issn.0254-6108.2015.02.2014061202
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二甲亚砜捕获-高效液相色谱测定天然水体中羟基自由基的光化学生成

  • 1.

    河南理工大学资源环境学院, 焦作, 454000;

  • 2.

    环境化学与生态毒理学国家重点实验室, 中国科学院生态环境研究中心, 北京, 100085

  • 基金项目:

    国家自然科学基金(41371501, 21377156)

    河南省杰出青年(124100510003)

    河南理工大学杰出青年(HPUJ2013-04)资助.

Determination of photogenerated hydroxyl radicals in natural water by high performance liquid chromatography after trapping with dimethyl sulfoxide

  • 1.

    Insititute of Resources and Environment, Henan Polytechnic University, Jiaozuo, 454000, China;

  • 2.

    State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, 100085, China

  • Fund Project:

  • 摘要: 利用二甲亚砜捕获羟基自由基定量生成甲醛,甲醛与1,3-环己二酮和氨衍生反应,衍生产物在400 nm的激发波长下,在460 nm处具有特征荧光,建立了一个新的高效液相色谱分离、荧光检测水体中光学反应产生的羟基自由基的方法.考察了捕获剂用量、酸度、温度、时间以及衍生试剂用量对羟基自由基测定的影响,在优化的实验条件下,该方法对羟基自由基的定量下限为0.066 μmol·L-1.采用建立的方法对湖水、海水以及湿地水在氙灯模拟光源以及太阳光下羟基自由基光化学生成进行了初步研究,表明太阳光照下羟基自由基的生成速率约为氙灯光照下羟基自由基生成速率的两倍以上,说明羟基自由基在实际自然条件下的生成速率有可能被低估.天然水体中的羟基自由基的生成与水体成分密切相关,由铁和可溶性有机质(DOM)光照产生羟基自由基的机理较为复杂,DOM和铁的相互作用对天然水体中羟基自由基的光化学生成影响有待于进一步研究.
    Abstract: Hydroxyl radicals photochemically generated in natural water play an important role in the transformation of pollutants. A high performance liquid chromatography method for the determination of hydroxyl radicals was developed, based on trapping hydroxyl radicals with dimethyl sulfoxide to generate formaldehyde quantitatively. Formaldehyde then reacted with 1,3-cyclohexanedione and ammonia to producea derivative of formaldehyde, which was separated and analyzed by HPLC with fluorescence detector. Factors influencing the trapping of hydroxyl radical and derivation, such as trapping and derivatization reagent amount, pH, temperature and time, were investigated. Under the optimized condition, the lower limit at quantification reached 0.066 μmol·L-1. The method was applied to the determination of hydroxyl radicals generated in typical natural water (lake, sea and wetland water) under sunlight and Xenon lamp. The results showed that the photochemical generation of hydroxyl radicals under the natural condition was possibly underestimated. The generation of hydroxyl radical was closely related to the constituent in natural water, especially the interaction between DOM and iron.
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  • [1] 张彭义, 余刚. 蒋展鹏. 水中有机物与羟基自由基反应的QSAR分析[J]. 环境化学, 1999, 18(3): 232-237
    [2] Mostofa K M G, Yoshioka T, Mottaleb A, et al. Photobiogeochemistry of Organic Matter[M]. Heidelberg: Springer,2013, 209-272
    [3] Timko S A, Romera-Castillo C, Jaffé R, et al. Photo-reactivity of natural dissolved organic matter from fresh to marine waters in the Florida Everglades, USA[J]. Environmental Science: Processes & Impacts, 2014, 16(4): 866-878
    [4] 房豪杰, 邵春雷,陆晶,等. 水相中羟基自由基诱导二甲基硫氧化的研究[J]. 环境化学, 2006, 25(2): 133-136
    [5] Olasehinde E F, Hasan N. Adehuga O S, et al. Hydroxyl radical mediated degradation of diuron in river water[J]. Journal of American Science, 2013, 9(4): 29-34
    [6] Dong M M, Rosario-Ortiz F L. Photochemical formation of hydroxyl radical from effluent organic matter[J]. Environmental Science Technology, 2012, 46(7): 3788-3794
    [7] 张琳, 张喆,吴峰,等. 水中铁(Ⅲ)-草酸盐配合物光解产生羟基自由基的测定[J]. 环境化学, 2002, 21(1): 87-91
    [8] Boucheloukh H, Sehili T, Kouachi N, et al. Kinetic and analytical study of the photo-induced degradation of monuron by nitrates and nitrites under irradiation or in the dark[J]. Photochemical Photobiological Sciences, 2012, 11(8): 1339-1345
    [9] 李静, 刘延湘, 吴峰,等. 光照下高岭土悬浮液中产生羟基自由基的测定[J]. 环境化学, 2007, 26(5): 651-657
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出版历程
  • 收稿日期:  2014-06-12
  • 刊出日期:  2015-02-15

二甲亚砜捕获-高效液相色谱测定天然水体中羟基自由基的光化学生成

  • 1.  河南理工大学资源环境学院, 焦作, 454000;
  • 2.  环境化学与生态毒理学国家重点实验室, 中国科学院生态环境研究中心, 北京, 100085
  • 收稿日期:  2014-06-12
基金项目:

国家自然科学基金(41371501, 21377156)

河南省杰出青年(124100510003)

河南理工大学杰出青年(HPUJ2013-04)资助.

摘要: 利用二甲亚砜捕获羟基自由基定量生成甲醛,甲醛与1,3-环己二酮和氨衍生反应,衍生产物在400 nm的激发波长下,在460 nm处具有特征荧光,建立了一个新的高效液相色谱分离、荧光检测水体中光学反应产生的羟基自由基的方法.考察了捕获剂用量、酸度、温度、时间以及衍生试剂用量对羟基自由基测定的影响,在优化的实验条件下,该方法对羟基自由基的定量下限为0.066 μmol·L-1.采用建立的方法对湖水、海水以及湿地水在氙灯模拟光源以及太阳光下羟基自由基光化学生成进行了初步研究,表明太阳光照下羟基自由基的生成速率约为氙灯光照下羟基自由基生成速率的两倍以上,说明羟基自由基在实际自然条件下的生成速率有可能被低估.天然水体中的羟基自由基的生成与水体成分密切相关,由铁和可溶性有机质(DOM)光照产生羟基自由基的机理较为复杂,DOM和铁的相互作用对天然水体中羟基自由基的光化学生成影响有待于进一步研究.

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