海水环境中敌草隆的间接光降解影响

Study on Indirect Photodegradation Effect of Diuron in Seawater Environment

  • 摘要: 近岸海域腐殖酸主要来自径流输入,其性质、组成等受来源影响。以4种典型陆源腐殖酸为光敏剂研究了敌草隆(DIU)在海水中的间接光降解行为及机理,并分析了海水环境因子中盐度、pH和硝酸根离子(\mathrmNO^-_3 )对DIU间接光降解的影响。结果表明,有色溶解有机物(CDOM)是海水中DIU间接光降解的主要参与者,能显著促进DIU的间接光降解。在溶解有机碳(DOC)质量浓度相同情况下,腐殖酸JKHA(J&K腐殖酸)对DIU间接光降解的促进作用显著大于苏万尼河腐殖酸(SRHA)、苏万尼河天然有机物(SRNOM)和苏万尼河富里酸(SRFA)。CDOM在光照条件下可生成3CDOM*、·OH、1O2等活性中间体(RIs),其中3CDOM*是促进DIU间接光降解的主要活性中间体,对DIU间接光降解贡献率约61.0%。实验所用CDOM经解析获得4种荧光组分(C1~C4),C1、C3和C4荧光强度与3CDOM*的稳态浓度显著正相关(相关性系数均大于0.95),是3CDOM*的主要来源,在DIU的间接光降解中起着主要作用。陆源腐殖质组分C1、C3和C4在JKHA中的相对强度明显高于其他3种,所以对DIU间接光降解的促进作用比其他3种腐殖质强。盐度0~35.0时,DIU间接光降解速率随溶液盐度的增加先升高后降低。pH为(7.00±0.10)~(9.00±0.10)时DIU间接光降解速率随pH的升高而升高,在pH为(9.00±0.10)时最高。硝酸根离子对DIU的间接光降解也具有促进作用。

     

    Abstract: The humic acid mainly comes from the runoff input, its properties and composition are affected by its source. The indirect photodegradation behavior and mechanism of Diuron (DIU) in seawater were studied using four typical terrestrial humic acids as photosensitizers, and the effects of seawater environmental factors (salinity, pH and nitrate ions) on the indirect photodegradation of DIU were analyzed. The results showed that CDOM was the main participant in indirect photodegradation of DIU in seawater and it could significantly promote the indirect photodegradation of DIU. At the same dissolved organic carbon (DOC) mass concentration, JKHA promoted the indirect photodegradation of DIU significantly more than those of other three CDOMs. CDOM can generate 3CDOM*, ·OH, 1O2 and other active intermediates under the light conditions, among which 3CDOM* was the most effective reactive intermediates (RIs) that contributed 61% to indirect photodegradation of DIU. Four fluorescence components (C1~C4) were identified in the CDOMs used, and the fluorescence intensities of C1, C3 and C4 were significantly and positively correlated with the steady-state concentration of 3CDOM* (correlation coefficients were all greater than 0.95), which was the main source of 3CDOM* and played a major role in the indirect photodegradation of DIU. The relative intensities of terrestrial source humus fractions C1, C3 and C4 in JKHA were significantly higher than those of the other three CDOMs, resulting in a stronger promotion of indirect photodegradation of DIU by JKHA than by the other three humus fractions. The indirect photodegradation rate of DIU increased first and then decreased with the increase of salinity at salinity range from 0 to 35.0. In the range of pH from (7.00±0.10) to (9.00±0.10), the indirect photodegradation rate of DIU increased with the increase of pH, and its fastest degradation rate was found at pH (9.00±0.10). \mathrmNO_3^- could also promote the indirect photodegradation of DIU.

     

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