Determination of Multiple Elements in Soils Surrounding Iron Deposits from Guyang County, Baotou City, and Health Risk Assessment
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摘要:
矿产的开发利用会向周边土壤释放重金属元素，当人体摄入或接触受污染的土壤则可能会产生健康危害。铁矿是中国分布最为广泛的矿种之一，但前人对铁矿区土壤重金属健康风险的研究较少，尤其是干旱区铁矿。干旱区生态脆弱，修复困难，因此需要更加科学地对土壤加强管理。本文以内蒙古包头市固阳县某铁矿区为研究对象，采集表层土壤101件，采用电感耦合等离子体质谱/发射光谱法和原子荧光光谱法测定了土壤中的重金属含量，研究元素的特征，并利用健康风险评价法评价重金属对人体的健康危害，提出土壤污染筛选值。结果显示：①研究区土壤中Cu、Cr、Ni变异系数大于0.5，平均含量明显高于河套平原背景值；②Cu的高值区主要分布于尾矿库与选矿厂周边，Cr、Ni的高值区主要分布于基岩山区；③健康风险评价结果表明各元素的危害商(HQ)均小于1，由大到小顺序为As>Cr>Ni>Cu>Cd>Zn>Hg，总危害商(HI)的平均值为0.542，有1个点HI大于1，位于矿区南部基岩区，Cr、Ni、As的贡献率分别为59%、25%、15%，总致癌风险指数(CR)均小于10-4；④基于人体健康计算提出研究区土壤Cr、Ni、As的污染筛选值为541、579、32.8mg/kg。本研究揭示了：①研究区Cr、Ni主要受到成土母质影响，Cu主要受到选矿活动影响；②土壤重金属总体上健康危害较低，受成土母质影响较大，但仍需关注尾矿库周边污染元素的累积情况，并避免经口摄入污染物；③不同地区或不同类型的铁矿中的伴生元素不同，仍需对各气候分区内不同类型的铁矿进一步开展研究。
Abstract:BACKGROUND The exploitation of minerals releases heavy metals into the surrounding soil, which can cause health hazards when biological entities are exposed to contaminated soil. Iron ore is one of the most widely distributed minerals in China, but there are few studies on the health risk of soil heavy metals in iron mines, especially in arid areas. The ecosystem of the arid area is fragile and difficult to repair once it has been polluted.
OBJECTIVES To perform environmental health risk assessment for topsoil surrounding iron deposits from Guyang County, Baotou City.
METHODS 101 topsoil samples were collected from an iron mine in Guyang County, Baotou City. Heavy metals were measured by inductively coupled plasma-mass spectrometry/optical emission spectrometry and atomic fluorescence spectrometry, to study element characteristics. The health risk assessment method was used to evaluate and calculate the screening value.
RESULTS The results showed that the variation coefficients of copper, chromium, and nickel in the study area were higher than 0.5, and the average contents of these elements were significantly higher than that in the Hetao Plain. The high value areas of copper were mainly distributed around tailings ponds and concentrators, while the high value areas of chromium or nickel were mainly distributed in bedrock mountains. The assessment of health hazards showed that the hazard quotient of all elements was less than 1, and the order was As>Cr>Ni>Cu>Cd>Zn>Hg. The average of total hazard quotient was 0.542. There was a sample in the bedrock mountain south of the iron mine, which had a total hazard quotient exceeding 1, and the contribution rates of chromium, nickel and arsenicwere 59%, 25%, and 15%, respectively. The carcinogenic hazard index of all elements was below 10-4. Soil screening levels of chromium, nickel and arsenic in the study area were 579mg/kg, 622mg/kg and 32.8mg/kg base on human health.
CONCLUSIONS Chromium and nickel in the study soil are mainly affected by parent materials of soil formation, while copper is mainly affected by mineral processing activities. In general, the health hazard of heavy metals in soil is relatively low, and is greatly influenced by the parent materials of soil formation. However, it is still necessary to pay attention to the accumulation of polluted elements in the areas around tailings ponds, and to avoid oral intake of pollutants. And it is also necessary to further study the feature of soil heavy metals from different kinds of iron mines and different regions that have not been studied before, because the associated elements of iron ore in different regions or types are not the same.
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表 1 健康风险评价模型暴露因子参数
Table 1. Exposure factor parameters of health risk assessment model
参数 具体描述 数值单位 参考值 OISERn 非致癌(致癌)效应下经口摄入土壤暴露量 - - DCSERn 非致癌(致癌)效应下皮肤接触土壤暴露量 - - PISERn 非致癌(致癌)效应下吸入土壤颗粒暴露量 - - OISR 每日摄入土壤量 mg/d 100Ⅰ ED 暴露时长 a 25Ⅰ EF 暴露频率 d/a 250Ⅰ ABS0 经口摄入吸收效率因子 无量纲 1Ⅰ BW 平均体重 kg 61.8Ⅰ ATn 非致癌(致癌)效应平均时长 d 27740Ⅰ(致癌), 9125Ⅰ(非致癌) DAIR 每日空气呼吸量 m3/d 14.5Ⅰ PM10 空气中可吸入悬浮颗粒物总量 mg/m3 0.07Ⅱ PIAF 吸入土壤颗粒物在体内滞留比例 无量纲 0.75Ⅰ fspo 室内空气中来自土壤的颗粒物所占比例 无量纲 0.8Ⅰ EFO 室内暴露频率 d/a 187.5Ⅰ fspi 室外空气中来自土壤的颗粒物所占比例 无量纲 0.5Ⅰ EFI 室外暴露频率 d/a 62.5Ⅰ SAE 皮肤暴露面积 cm2 3033Ⅲ SSAR 皮肤表面土壤黏附系数 mg/cm2 0.2Ⅰ ABSd 皮肤接触吸收效率因子 无量纲 0.001Ⅰ(镉)，0.03Ⅰ(砷) E 每日皮肤接触事件频率 次/d 1Ⅰ 注：标注Ⅰ的数据直接引自HJ 25.3—2019；Ⅱ为包头市政府公布数据；Ⅲ根据HJ 25.3—2019计算得出。 
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表 2 土壤重金属不同暴露途径的RfD和SF值
Table 2. RfD and SF values for different exposure pathways of heavy metals in soil
重金属元素 参考剂量[mg/(kg·d)] 致癌斜率因子[kg·d/mg] RfD0 数据来源 RfDi 数据来源来源 RfDd 数据来源来源 SF0 数据来源来源 SFi 数据来源来源 SFd 数据来源来源 Cr 3.00×10-3 Ⅲ - - - - - - 5.12×10-2 Ⅳ - - Ni 2.00×10-2 Ⅰ 2.11×10-5 Ⅱ - - - - 1.11 Ⅱ - - Zn 3.00×10-1 Ⅰ - - - - - - - - - - Cu 4.00×10-2 Ⅰ - - - - - - - - - - Cd 1.00×10-3 Ⅰ 2.35×10-6 Ⅱ 2.50×10-5 Ⅱ - - 7.67 Ⅱ - - As 3.00×10-4 Ⅰ 3.52×10-6 Ⅱ 3.00×10-4 Ⅱ 1.50 Ⅰ 18.3 Ⅱ 1.50 Ⅱ Hg 3.00×10-4 Ⅰ 7.04×10-5 Ⅱ - - - - - - - - 注：标注Ⅰ的数据直接引自HJ 25.3—2019；Ⅱ根据HJ 25.3—2019中外推公式引用Ⅰ计算得出；Ⅲ直接引自OSWER 9355.4-24；Ⅳ根据HJ 25.3—2019中外推公式引用Ⅲ计算得出。
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表 3 土壤重金属参数统计
Table 3. Parameter statistics of heavy metals in soil
重金属元素 最小值(mg/kg) 最大值(mg/kg) 平均值(mg/kg) 标准差(mg/kg) 变异系数 河套平原表层土壤背景值[38] (mg/kg) Cr 48 382 109 55 0.51 56 Ni 22 173 44 23 0.51 25 Zn 43.7 177.3 81.1 24.5 0.30 55.7 Cu 16.6 519.9 53.0 59.8 1.13 19.2 Cd 0.03 0.33 0.10 0.04 0.36 0.12 Pb 4.28 61.18 18.13 7.27 0.40 18.76 As 1.21 14.85 8.29 2.60 0.31 9.68 Hg 0.0032 0.0492 0.0214 0.0088 0.41 0.0249
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表 4 不同暴露途径土壤重金属危害商
Table 4. Hazard quotient of heavy metals in soil under different exposure pathways
参数 危害商 最小值 最大值 平均值 HQoisCr 8.95×10-2 7.05×10-1 2.01×10-1 HQoisNi 5.97×10-3 4.78×10-2 1.23×10-2 HQpisNi 3.12×10-2 2.50×10-1 6.45×10-2 HQoisZn 8.06×10-4 3.28×10-3 1.50×10-3 HQoisCu 2.30×10-3 7.20×10-2 7.34×10-3 HQoisCd 1.39×10-4 1.83×10-3 5.82×10-4 HQdcsCd 3.36×10-5 4.45×10-4 1.41×10-4 HQpisCd 3.25×10-4 4.31×10-3 1.37×10-4 HQoisAs 2.24×10-2 2.74×10-1 1.53×10-1 HQdcsAs 4.07×10-3 4.99×10-2 2.79×10-2 HQpisAs 1.05×10-3 1.29×10-1 7.20×10-2 HQoisHg 5.94×10-5 9.10×10-4 3.95×10-4 HQpisHg 1.40×10-6 2.14×10-5 9.28×10-6
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表 5 所有暴露途径土壤重金属危害商
Table 5. Hazard quotient of heavy metals in soil under all exposure pathways
参数 危害商 最小值 最大值 平均值 HQCr 8.95×10-2 7.05×10-1 2.01×10-1 HQNi 3.72×10-2 2.98×10-1 7.68×10-2 HQZn 8.06×10-4 3.28×10-3 1.50×10-3 HQCu 2.30×10-3 7.20×10-2 7.34×10-3 HQCd 4.98×10-4 6.59×10-3 2.09×10-3 HQAs 3.69×10-2 4.53×10-1 2.53×10-1 HQHg 6.08×10-5 9.31×10-4 4.04×10-4 HI 3.21×10-1 1.20 5.42×10-1
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表 6 土壤重金属致癌健康风险指数
Table 6. Carcinogenic hazard index of heavy metals in soil
参数 健康风险指数 最小值 最大值 平均值 CRoisAs 6.62×10-7 8.12×10-6 4.53×10-6 CRdcsAs 1.20×10-7 1.48×10-6 8.25×10-7 CRpisAs 4.46×10-8 5.48×10-7 3.06×10-7 CRAs 8.27×10-7 1.01×10-5 5.67×10-6 CRCr 4.99×10-9 3.93×10-8 1.12×10-8 CRNi 4.81×10-8 3.85×10-7 9.94×10-8 CRCd 3.86×10-10 5.11×10-9 1.62×10-9
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表 7 研究区土壤重金属筛选值
Table 7. Screening levels of heavy metals in soil from the study area
重金属元素 筛选值(mg/kg) 基于HQois 基于HQpis 基于HQdcs 基于HQ 基于CRois 基于CRpis 基于CRdcs 基于CR 建议筛选值 GB36600筛选值 Cr 5.41×102 - - 5.41×102 - 9.71×105 - 9.71×105 5.41×102 - Ni 3.61×103 6.90×102 - 5.79×102 - 4.48×104 - 4.48×104 5.79×102 9.00×102 Zn 5.41×104 - - 5.41×104 - - - - 5.41×104 - Cu 7.22×103 - - 7.22×103 - - - - 7.22×103 1.80×104 Cd 1.80×102 7.68×101 7.44×102 5.02×101 - 6.48×103 - 6.48×103 5.02×101 6.50×101 As 5.41×101 1.15×102 2.97×102 3.28×101 1.83×102 2.71×103 1.00×103 1.46×102 3.28×101 6.00×101 Hg 5.41×101 2.30×103 - 5.29×101 - - - - 5.29×101 3.80×101 注：“-”表示无相关风险，无需计算。
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