Characteristics, distribution and source of dissolved organic matter and its implications for antimony contamination in Zijiang River basin
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摘要:
溶解性有机质（dissolved organic matter, DOM）是影响重金属元素在水体中迁移转化的关键因素之一。资江是洞庭湖第三大支流，流域内锑矿开发导致资江江水中锑（Sb）的质量浓度处于较高水平。为了解析资江流域江水中DOM的特征及来源，探索DOM对Sb迁移的指示意义，研究对资江流域江水进行了三维荧光光谱分析，利用平行因子法分析了水体中DOM的组分和荧光特征以及各组分与Sb质量浓度的关联。结果表明：（1）资江流域江水中Sb质量浓度为1.50～62.20 μg/L，平均值为7.26 μg/L，其中有55.56%的采样点Sb质量浓度超过最低限制5 μg/L；（2）资江流域江水DOM有C1、C2和C3共3个组分，依次为陆源的类富里酸组分、类腐殖质组分以及可作为电子运输工具的醌类腐殖质组分，以C1和C2组分为主；（3） DOM主要通过2种方式影响Sb的迁移，一是水体中DOM的醌类基团作为电子传递体并参与有机质的氧化及铁氧化物的还原，二是富里酸基团与Sb进行络合形成DOM-Sb型复合物，2种方式协同促进了资江流域江水中Sb的富集，提高了Sb的迁移能力。研究结果将为资江流域江水Sb污染溯源和防治提供新的方向和理论依据。
Abstract:Dissolved organic matter (DOM) is critical to affecting heavy metal migration and transformation in water. Zijiang River, the third largest tributary of Dongting Lake in Hunan Province, has a high level of antimony (Sb) mass concentration due to the rapid development of the antimony mining and smelting. Excitation-emission matrix spectroscopy (EEMs) and parallel factor analysis (PARAFA)were used to analyze the source and characteristics of DOM in Zijiang River and its indicative significance on antimony migration. The results show that the mass concentration of antimony in the river water in Zijiang River ranges from 1.50 to 62.20 μg/L, with an average of 7.26 μg/L, of which 55.56% exceed the antimony minimum limit of 5 μg/L. DOM of Zijiang River consists of three different components (C1, C2, and C3), which are terrestrial sources, humic-like substance, and the quinone-like humic substance used as electron transport tool, respectively. DOM is mainly composed of C1 and C2. Antimony migration and transformation are influenced by DOM in two ways: The quinone-like humic component, as an electron transfer tools, participates in the reduction of DOM and iron oxide; the complexation of fulvic acid with antimony results in the formation of DOM-Sb complex. The two approaches synergistically enhance the enrichment and transport capabilities of antimony in the Zijiang River. This study will provide a new direction and theoretical basis for the source and prevention of river water antimony pollution in the Zijiang River.
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表 1 荧光光谱参数描述
Table 1. Description of fluorescence spectral parameter
荧光光谱参数 计算方法 意义 特征描述 荧光指数[28]
（fluorescence index，FI）k为370 nm时，j为470 nm与
520 nm的荧光强度之比微生物来源有机质占
总有机质的比例<1.4，陆源有机物； >1.9，微生物来源；
1.4～1.9，陆源内源混合来源；自生源指数[29]
（autochthonous index，BIX）k为310 nm时，j为380 nm与
430 nm的荧光强度之比微生物来源有机质和
外源有机质的比值，衡量自生来源
有机质的贡献率<0.6，自生来源贡献少；0.6～0.8，中度新近自
生来源特征；>0.8 较强的自生来源特征；腐殖化指数[30]
（ humification index，HIX）k为255 nm时，j为435～480 nm与
300～345 nm之间荧光强度之和的比值表征DOM腐殖化程度 1.5～4，具有弱腐质化特征；
4～6，具有较强腐质化特征；
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表 2 资江流域江水水质指标特征
Table 2. Characteristics of water quality index of the Zijiang River
水体 统计值 pH EC DO DOC 元素质量浓度 Sb As Cd Cr 上游段 范围 7.99～9.12 163.00～267.00 8.13～10.96 1.48～2.70 1.50～3.36 0.83～1.62 0.02～0.06 0.16～1.24 平均值 8.63 213.56 9.53 2.16 2.45 1.19 0.03 0.53 标准差 0.40 34.39 0.87 0.35 0.55 0.21 0.02 0.34 变异系数 0.05 0.16 0.09 0.16 0.22 0.17 0.52 0.64 中游段 范围 8.00～8.32 211.90～513.00 7.63～9.81 2.19～4.00 5.00～62.20 2.05～3.21 0.02～0.07 0.35～1.64 平均值 8.16 293.54 8.63 2.67 12.09 2.42 0.04 0.78 标准差 0.10 85.11 0.81 0.54 17.75 0.36 0.02 0.50 变异系数 0.01 0.29 0.09 0.20 1.47 0.15 0.38 0.64 下游段 范围 8.10～8.41 111.10～228.00 8.78～11.01 1.85～3.15 1.71～30.10 0.64～5.43 0.02～0.12 0.37～1.76 平均值 8.24 206.10 10.07 2.34 7.83 2.80 0.07 0.74 标准差 0.10 36.28 0.66 0.35 8.50 1.25 0.03 0.44 变异系数 0.01 0.18 0.07 0.15 1.09 0.45 0.41 0.59 总体 范围 7.99～9.12 111.10～513.00 7.63～11.01 1.48～4.00 1.50～62.20 0.64～5.43 0.02～0.12 0.16～1.76 平均值 8.33 238.49 9.35 2.39 7.26 2.08 0.05 0.67 标准差 0.33 69.24 0.98 0.48 11.96 1.00 0.03 0.44 变异系数 0.04 0.29 0.10 0.20 1.65 0.48 0.57 0.65 注：表中pH和变异系数为无量纲；EC单位为μS/cm；DO、DOC单位为mg/L；其他指标单位为μg/L。
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表 3 水体中3个荧光组分特征及其与确定组分的对比
Table 3. Characteristics of the three fluorescence components and their comparison with previous identified components
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表 4 三维荧光光谱指数分布情况
Table 4. Distribution of spectra indices based on EEMs
指标 最大值 最小值 平均值 变异系数/% 总体 FI 1.68 1.55 1.63 2.08 BIX 0.87 0.73 0.82 3.19 HIX 5.33 3.17 4.33 14.08 上游段 FI 1.67 1.55 1.62 2.35 BIX 0.85 0.80 0.83 2.27 HIX 4.55 3.17 3.93 14.14 中游段 FI 1.68 1.58 1.64 1.94 BIX 0.87 0.80 0.83 2.50 HIX 4.68 3.77 4.16 8.82 下游段 FI 1.65 1.57 1.62 1.77 BIX 0.82 0.73 0.80 3.62 HIX 5.33 4.38 4.93 6.60
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