Inorganic-Organic Characteristics and Health Risk Assessment of Typical Underground River System in Southwest China
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摘要:
岩溶地下水为全球约25%的人口提供饮用水源，地下河作为主要岩溶地下水类型，是中国西南岩溶区重要供水水源，掌握其水质污染状况及人体健康风险，对岩溶区水资源保护与安全用水具有重要意义。本文以广西桂林会仙狮子岩地下河系统为例，采集地下河水样品22组(无机和有机样品各11组)，采用电感耦合等离子体质谱、离子色谱、气相色谱-质谱等方法测定11项无机离子、10项金属元素及41项有机指标的质量浓度，运用单指标污染标准指数法、健康风险评价模型揭示了研究区无机与有机指标分布、污染及健康风险。结果表明：①狮子岩地下河水中无机超标指标有NH4+(1.33倍)、Fe(1.2倍)、Al(1.5倍)和Mn(1.01倍)，超标点多位于地下河排泄区；检出18项有机物，其中挥发性有机物(VOCs)、半挥发性有机物(SVOCs)和有机氯农药(OCPs)检出率分别为18.75%、30.77%和91.67%，研究区存在普遍的农药残留(49.14~109.83ng/L)。②与地下水对照值相比，研究区受到10项无机指标的轻度~中度污染、14项有机指标的轻度污染，个别采样点受到NO3-、Fe、Al和Mn的较严重~严重污染，一处采样点遭受苯并[a]芘的极严重污染。③经饮用水和皮肤接触两种途径暴露的非致癌健康风险(成人9.98×10-3a-1，儿童1.09×10-2a-1)和致癌健康风险(成人1.33×10-7a-1，儿童2.82×10-7a-1)均在可接受范围内。本文认为研究区存在不同程度的无机和有机污染，但污染物指标对人体暂不构成非致癌和致癌健康风险。
Abstract:BACKGROUND Karst groundwater provides drinking water for about 25% of the world's population. As the main type of karst groundwater, underground rivers are an important water supply source for karst areas in Southwest China. It is of great significance to master the water quality, pollution status and human health risk for water resources protection and safety use in southern karst areas.
OBJECTIVES To reveal the chemical compositions, pollution degree and health risk of underground river water.
METHODS 22 groups of underground river water samples (half inorganic and half organic samples) from the underground river system of Shiziyan in Huixian, Guilin, Guangxi were collected. The concentrations and spatial distribution of 21 inorganic ions and 41 organic indices were analyzed by inductively coupled plasma-mass spectrometry (ICP-MS), ion chromatography (IC) and gas chromatography-mass spectrometry (GC-MS).The single index pollution standard index method was used to evaluate the pollution of 17 inorganic ions and 15 detected organic compounds. The health risk assessment model recommended by the United States Environmental Protection Agency (US EPA) was used to study the human health risk of 10 major pollutants.
RESULTS The results showed that: (1) Ca2+ and HCO3- were the dominant ions in the Shiziyan underground river. The concentrations of NH4+, Fe, Al and Mn in the underground river exceeded the groundwater quality standard by 1.33, 1.2, 1.5 and 1.01 times, respectively, and the exceeding points were mostly located in the discharge area of the underground river. 18 organic compounds were detected, of which the detection rates of volatile organic compounds (VOCs), semi volatile organics (SVOCs) and organochlorine pesticides (OCPs) were 18.75%, 30.77% and 91.67% respectively. (2) Compared with the groundwater background values, the underground river water in the study area was slightly-moderately polluted by 10 inorganic indicators and 14 organic compounds. Some sampling points were seriously polluted by NO3-, Fe, Al and Mn, and one sampling point (UR8) was extremely polluted by benzo [a] pyrene. (3) According to the results of health risk assessment, the non-carcinogenic health risks of being exposed to drinking water and for skin exposure were 9.98×10-3 per year for adults and 1.09×10-2 per year for children, and carcinogenic health risks were 1.33×10-7 per year for adults and 2.82×10-7 per year for children, which were within acceptable levels.
CONCLUSIONS There are various degrees of inorganic and organic pollution in the study area, but the pollutant indicators do not pose a non-carcinogenic or carcinogenic health risk to the population.
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表 1 狮子岩地下河有机测试指标和测试方法
Table 1. Statistics of organic indices and analytical methods in the Shiziyan underground river
有机指标类型 测试指标数 测试项目 测试方法 VOCs 16项 三氯甲烷、四氯化碳、苯、甲苯、二氯甲烷、1, 2-二氯乙烷、1, 1, 1-三氯乙烷、1, 1, 2-三氯乙烷、1, 2-二氯丙烷、三溴甲烷、氯乙烯、1, 1-二氯乙烯、四氯乙烯、乙苯、二甲苯、苯乙烯 气相色谱-质谱法 SVOCs 13项 1, 2-二氯苯、1, 4-二氯苯、1, 2, 4-三氯苯、2, 4-二硝基甲苯、2, 6-二硝基甲苯、萘、蒽、荧蒽、苯并[b]荧蒽、苯并[a]芘、双(2-乙己基)邻苯二甲酸酯、2, 4, 6-三氯苯酚、五氯苯酚 气相色谱-质谱法 OCPs 12项 总六六六、α-六六六、β-六六六、γ-六六六、δ-六六六、总DDT、六氯苯、七氯、艾氏剂、环氧七氯、狄氏剂、异狄氏剂 气相色谱法 
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表 2 单指标污染标准指数评价分级
Table 2. Single factor standard index grade
污染指数 污染等级 污染类别 Pi≤0 Ⅰ 未污染 Pi>(0~0.2) Ⅱ 轻污染 Pi>(0.2~0.6) Ⅲ 中污染 Pi >(0.6~1.0) Ⅳ 较重污染 Pi>(1.0~1.5) Ⅴ 严重污染 Pi>1.5 Ⅵ 极重污染
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表 3 健康风险评价模型相关参数取值
Table 3. Values of parameters related to health risk assessment
评价指标 参数 SF[(kg·d)/mg] RfD[mg/(kg·d)] PC
(cm/h)饮用水途径 皮肤入渗途径 饮用水途径 皮肤入渗途径 非致癌指标 NH4+ - - 0.97 0.97 0.001 NO3- - - 1.6 1.6 0.001 Al - - 0.14 0.14 0.01 Mn - - 0.046 0.0018 0.0001 Hg - - 0.0003 0.0003 0.0018 Fe - - 0.3 0.045 0.0001 异狄氏剂 - - 0.0003 0.0003 0.001 苯并[a]芘 7.3 37.47 - - 0.001 致癌指标 总六六六 1.8 1.8 - - 0.001 总DDT 0.34 0.34 - - 0.001 注：“-”表示无相应参考标准值。
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表 4 狮子岩地下河无机离子及金属元素化学特征统计
Table 4. Statistics of chemical characteristics of inorganic ions and metals in Shiziyan underground river
统计量 指标类型——无机离子 K+ Na+ Ca2+ Mg2+ NH4+ Cl- SO42- HCO3- NO3- NO2- F- 最大值(mg/L) 47.75 18.80 119.47 16.66 0.85▲ 25.81 41.47 390.37 72.01 0.12 0.09 最小值(mg/L) 0.16 0.65 64.53 1.12 nd 2.96 7.38 203.86 nd nd nd 平均值(mg/L) 9.20 4.89 82.39 5.16 0.09 7.59 17.08 252.95 14.64 0.03 0.06 标准差(mg/L) 15.27 6.26 17.38 4.59 0.25 7.00 12.86 54.96 23.85 0.04 0.03 变异系数 1.66 1.28 0.21 0.89 2.84 0.92 0.75 0.22 1.63 1.26 0.47 超标率(%) 0.00 0.00 0.00 0.00 9.09 0.00 0.00 0.00 0.00 0.00 0.00 统计量 指标类型——金属元素 Al Cu Pb Zn Cr Cd Mn As Hg Fe 最大值(μg/L) 300▲ 2.37 0.94 8.77 4.46 nd 101▲ 1.72 0.75 360▲ 最小值(μg/L) nd nd nd nd 1.95 nd 0.98 nd nd nd 平均值(μg/L) 81.76 0.36 0.16 1.67 2.89 / 43.03 0.97 0.41 102.18 标准差(μg/L) 91.70 0.70 0.29 2.97 0.75 / 38.18 0.49 0.34 122.95 变异系数 1.12 1.95 1.73 1.78 0.26 / 0.89 0.51 0.81 1.20 超标率(%) 9.09 0.00 0.00 0.00 0.00 / 9.09 0.00 0.00 9.09 注：nd表示未检出；“/”表示无参考值及相应计算值；标注“▲”数值表示此浓度超标。
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表 5 狮子岩地下河有机指标检出情况统计
Table 5. Detection of organics in Shiziyan underground river
有机指标类型 总检出率
(%)单项检出指标统计 标准限值
(ng/L)检出项目 检出率(%) 最小值(ng/L) 最大值(ng/L) 平均值(ng/L) 三氯甲烷 9.09 250.00 250.00 250.00 60000a VOCs 18.75 甲苯 18.18 610.00 890.00 750.00 700000a 二氯甲烷 54.55 550.00 910.00 778.00 20000a SVOCs 30.77 荧蒽 18.18 69.60 133.00 101.30 240000a 苯并[b]荧蒽 27.27 19.30 27.50 23.73 4000a 苯并[a]芘 9.09 60.50▲ 60.50▲ 60.50▲ 10a DEHP 36.36 207.00 573.00 404.33 8000a 总六六六 100.00 2.85 44.30 20.89 5000a α-六六六 27.27 3.65 13.40 7.96 / β-六六六 90.91 1.81 15.80 4.87 / γ-六六六 72.73 1.42 8.87 4.07 2000a δ-六六六 90.91 2.17 31.20 11.32 / OCPs 91.67 总DDT 100.00 7.24 20.20 16.92 1000a 六氯苯 54.55 2.48 5.75 3.34 1000a 七氯 18.18 5.40 9.91 7.66 400a 环氧七氯 63.64 1.35 4.62 2.28 30b 狄氏剂 18.18 1.48 5.51 3.50 30b 异狄氏剂 100.00 19.80 46.40 32.02 2000b 注：标注“▲”数值表示此浓度超标；a表示《地下水质量标准》(GB/T 14848—2017)Ⅲ类质量标准；b表示WTO《饮用水水质准则》限值；“/”表示无参考值。
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表 6 无机和有机污染物分别经饮用水途径和皮肤入渗途径产生的个人年健康风险值
Table 6. Per capita annual health risks caused by inorganic-organic pollutants though drinking and skin penetration pathway, respectively
致癌性 污染指标 个人年健康风险值(a-1) 饮用水途径 皮肤接触途径 合计 成人 儿童 成人 儿童 成人 儿童 非致癌物 NH4+ 1.06×10-4 1.15×10-4 5.48×10-7 3.85×10-7 1.06×10-4 1.16×10-4 NO3- 7.53×10-3 8.21×10-3 3.90×10-5 2.74×10-5 7.57×10-3 8.24×10-3 Fe 2.80×10-4 3.06×10-4 9.68×10-7 6.80×10-7 2.81×10-4 3.07×10-4 Al 3.36×10-4 3.67×10-4 1.74×10-5 1.22×10-5 3.54×10-4 3.79×10-4 Mn 4.90×10-4 5.34×10-4 6.49×10-6 4.55×10-6 4.96×10-4 5.39×10-4 Hg 1.14×10-3 1.24×10-3 1.06×10-5 7.44×10-6 1.16×10-3 1.23×10-3 异狄氏剂 2.79×10-5 6.10×10-5 2.90×10-7 2.03×10-7 2.82×10-5 6.12×10-5 总健康风险 9.91×10-3 1.08×10-2 7.54×10-5 5.29×10-5 9.98×10-3 1.09×10-2 致癌物 苯并[a]芘 1.16×10-7 2.52×10-7 6.15×10-9 4.32×10-9 1.23×10-7 2.57×10-7 总六六六 9.85×10-9 2.15×10-8 1.02×10-10 7.16×10-11 9.959×10-9 2.16×10-8 总DDT 1.51×10-9 3.29×10-9 1.56×10-11 1.10×10-11 1.52×10-9 3.30×10-9 总健康风险 1.27×10-7 2.77×10-7 6.27×10-9 4.40×10-9 1.33×10-7 2.82×10-7
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