EEMs Characteristics of Dissolved Organic Matter and Their Implication in High Arsenic Groundwater of Jianghan Plain
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摘要: 水体中溶解性有机质(dissolved organic matter, DOM)是含水层中砷释放的主控因素之一.江汉平原河湖众多、沟渠广布，地表水体与浅层地下水的交互作用使得DOM的组分特征及其强度有显著差异.为查明江汉平原地下水中溶解性有机质在砷迁移转化过程中的作用，对江汉平原地表水和浅层地下水进行三维荧光光谱分析，使用平行因子分析法提取水体中有机质的分子组成、功能特点和荧光特征，并分析各组分相对含量与地下水中砷与铁的关联.江汉平原水体中DOM包括3种主要组分，组分C1、C2为类腐殖质，C2是生物降解过程中产生的小分子，C3为类蛋白物质.地下水DOM以类腐殖质组分C1、C2为主，地表水以类蛋白类物质C3和小分子腐殖质C2为主.高砷地下水中DOM以陆源为主，主要通过两种途径促进As的迁移转化：(1) DOM的腐殖质组分充当微生物群落的电子运输工具，促进微生物作用下的有机质氧化和铁氧化物的还原，并伴随As的释放及大量溶解性有机碳(dissolved organic carbon, DOC)和HCO3-的产生；(2) As以铁等金属阳离子为桥接物与腐殖质结合，通过形成As-Fe-DOM络合物，导致地下水中砷的迁移.Abstract: Dissolved organic matter (DOM) is one of the key factors controlling the release of arsenic from sediment to groundwater. There are abundant surface water systems with rivers, lakes, streams and ponds in the Jianghan plain, densely covered by irrigation canals and ditches. The interactions between surface water and shallow groundwater may significantly affect the characteristics and strength of DOM in water. In order to elaborate the roles of DOM on arsenic mobilization in groundwater of Jianghan plain, this study analyzes surface water and groundwater samples using excitation-emission matrix spectroscopy (EEMs) and characterizes the dissolved organic matter of its functional groups, molecular, fluorescence using PARAFAC (parallel factor analysis). It is found that dissolved organic matter in Jianghan plain mainly includes three different components, of which C1 and C2 are humic-like substances and C3 is characterized by protein-like substances. The main components of dissolved organic matter in groundwater are C1 and C2, whilst the dissolved organic matter in surface water is mostly C2 and C3. Dissolved organic matter in groundwater dominated by terrestrial materials, promotes the mobilization of arsenic in two ways. (1) The humic substances act as an electron shuttle for microbial communities, promoting the microbially mediated oxidation of organic matter and reduction of Fe oxides with the release of arsenic and the production of large amounts of DOC (dissolved organic carbon)and HCO3-; (2) Complexation of As with DOM via the bridging of metal cations (such as Fe) enhances the mobility of As in groundwater.
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图 1 研究区及采样点分布
Fig. 1. Location of the study area and sampling sites for surface water and groundwater
图 2 平行因子鉴别出的3个荧光组分及其荧光特征
Fig. 2. Spectral characteristics of the 3 components model identified by EEM-PARAFAC
图 3 研究区地表水与浅层地下水中DOM各组分相对含量
Fig. 3. Distribution of DOM in groundwater and surface water of Jianghan plain
图 4 地下水中As含量与荧光指数的关系
Fig. 4. Relationship between As concentrations and f450/500 value of groundwater in Jianghan plain
图 5 江汉平原浅层地下水中DOC、HCO3-、Fe与As浓度的关系
Fig. 5. Relationships between As and DOC, HCO3-, Fe concentrations of groundwater in Jianghan plain
图 6 菱铁矿饱和指数(SI)与Fe浓度、Fe/As浓度比值关系
Fig. 6. The saturation index (SI=lg IAP/K) for siderite (FeCO3) versus the Fe concentration and the Fe/As (mM/μM) here M is mol/L, in the groundwater of the Jianghan plain
图 7 不同As浓度的地下水中天然有机物组分的Fmax与As之间的关系
Fig. 7. Relationship between As concentration and Fmax of groundwater in Jianghan plain
表 1 江汉平原主要河流沿程水化学指标
Table 1. Statistics for water chemistry of surface water in Jianghan plain
所属地表水系 pH DO
(mg/L)Ca2+
(mg/L)K+
(mg/L)Mg2+
(mg/L)Na+
(mg/L)Cl-
(mg/L)
SO42-
(mg/L)DOC
(mg/L)NH4-N
(mg/L)TDS
(mg/L)硬度CaCO3
(mg/L)水质
类别汉
江沙洋段 7.79 7.93 50.8 2.44 9.09 9.38 9.52 36.4 2.40 0.13 185 147 Ⅰ 潜江段 6.87 8.75 50.0 2.43 9.02 7.50 7.81 34.8 2.66 0.15 180 146 Ⅱ 通
顺
河泽口段 6.79 2.11 98.2 11.3 18.0 33.3 45.5 45.5 33.9 3.20 439 294 Ⅴ 毛咀段 6.69 1.74 79.7 6.87 14.3 27.6 32.9 32.9 31.6 7.05 345 232 Ⅴ 三伏潭段 6.65 1.86 80.1 7.40 13.6 17.7 34.5 34.5 27.3 4.28 326 232 Ⅴ 袁家市段 6.56 2.99 83.6 7.35 15.0 24.4 34.6 34.6 6.83 3.75 343 244 Ⅴ 彭场镇段 6.66 4.73 72.5 8.08 12.6 15.5 37.4 37.4 23.9 3.23 282 210 Ⅴ 沙湖镇段 6.71 3.00 67.2 7.49 11.7 14.5 33.5 33.5 8.09 3.18 258 195 Ⅴ 东
荆
河潜江段 6.72 8.66 49.2 2.40 8.86 7.79 8.33 34.8 5.50 0.11 181 144 Ⅰ 监利段 8.06 8.24 49.6 2.99 9.45 9.42 13.6 36.9 2.94 0.36 185 144 Ⅰ 黄家口段 7.59 5.14 48.2 3.87 9.74 10.2 18.9 36.5 3.79 0.48 192 141 Ⅲ 峰口镇段 7.71 5.08 46.4 3.53 8.94 9.06 16.2 36.0 3.53 0.59 183 132 Ⅲ 长
江江陵段 7.54 6.37 52.4 2.63 9.03 9.83 10.4 38.6 2.18 0.86 193 150 Ⅲ 监利段 7.68 6.37 54.0 2.68 9.42 9.31 10.1 38.5 2.38 0.54 197 155 Ⅲ 
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表 2 研究区地下水水化学指标统计
Table 2. Statistics for water chemistry of groundwater in Jianghan plain
水化指标 单位 浅层潜水 浅层承压水 最大值 最小值 平均值 最大值 最小值 平均值 pH 7.50 6.41 6.87 7.59 6.26 6.80 EC μS/cm 2 089 333 994 1 315 399 869 Eh mV 170 20 77 58 -207 -108 氨氮 mg/L 1.55 0.02 0.24 17.7 0.02 3.64 Fe mg/L 0.83 0.02 0.32 20.8 0.01 7.23 Mn mg/L 3.41 ＜0.001 0.77 8.20 ＜0.001 0.91 Ca2+ mg/L 217 58.7 123 170 59.8 116 Mg2+ mg/L 41.1 6.40 23.6 34.1 12.2 24.4 Na+ mg/L 128 6.93 35.6 36.3 6.54 18.5 K+ mg/L 47.6 0.62 10.1 20.0 0.51 2.29 Cl- mg/L 140 0.74 29.4 33.7 0.37 4.68 NO3- mg/L 91 0.32 35.1 9.97 0.04 0.73 SO42- mg/L 256 0.65 65.3 27.9 0.72 7.73 HCO3- mg/L 730 189 442 904 267 619 DOC mg/L 15.6 0.70 3.08 14.41 0.98 4.01 As μg/L 36.2 0.33 8.67 2 550 0.54 136 TDS mg/L 1 193 227 521 692 218 477 硬度 mg/L 713 174 407 556 204 393
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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. Descriptions of the three-component PARAFAC model of Ex/Em wavelengths data and their comparison with previous identified components
组分 Ex./Em.Max(nm) 荧光类型 文献报道 C1 245(340)/460~480 类腐殖质；分子量大；易与金属离子络合 237~260(300~370)/400~500(Coble, 1996; Hudson et al., 2007)
240/456(Holbrook et al., 2006)
225(330)/460(Carstea et al., 2014)
＜240~275(339~420)/434~520(Ishii and Boyer, 2012)C2 250(325)/420 陆源类腐殖质；生物降解过程中产生的最小分子 237~260(300~370)/400~500 (Coble, 1996; Hudson et al., 2007)
250(325)/416 (Stedmon et al., 2003)
325/428 (Stedmon and Markager, 2005a)
315/418 (Murphy and Stedmon, 2008)C3 240~250/340 类蛋白物质(类色氨酸)；对微环境的变化敏感 225~237/340~381 (Coble, 1996; Hudson et al., 2007)
275/340 (Coble, 1996; Hudson et al., 2007)
280/328 (Stedmon and Markager, 2005b)
240/338 (Murphy et al., 2008)注：Ex./Em.Max(nm)表示荧光强度最大处的激发/发射波长，基于平行因子分析；括号中数值为第2个波峰所对应的波长.
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