Heavy Metal Pollution Characteristics and Risk Assessment of Soil and Rice in Farmland around the Copper-Lead-Zinc Tailing, Western Hubei Province
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摘要:
农田土壤污染导致的粮食安全问题已引起广泛关注，客观评价尾矿库周边农田土壤和农作物污染状况对后期土壤污染防治和安全利用具有重要意义。为研究鄂西某铜铅锌尾矿库周边农田土壤-水稻重金属污染状况及风险，本文同步采集50个点位农田土壤及水稻稻穗样品，应用电感耦合等离子体质谱/发射光谱、原子荧光光谱等方法测定As、Cd、Cu、Pb、Zn、Hg、Ni和Cr八种重金属含量及土壤pH值，采用潜在生态风险指数法和健康风险评估模型评价生态风险和健康风险。结果表明：①研究区土壤As、Cd、Cu、Pb、Zn存在超标，Cd超标率20%最大。水稻仅Cd超标，超标率14%。②相关性分析显示土壤重金属有相同的污染源，渗滤液泄漏是可能的污染源；水稻重金属与土壤具有正相关性，Cd元素相关性最强，可能由于水稻对土壤Cd吸收能力强。③潜在生态风险评价结果表明土壤Cd、Pb、Zn、Cu显著富集，Cd富集系数达4.41，研究区处于中度风险，6%点位具有极强风险。④健康风险评价结果表明几乎全部点位土壤总致癌风险和总非致癌风险大于可接受水平，存在重金属致癌风险，As和Cd致癌风险较大。水稻总致癌风险全部大于可接受水平，最大贡献者为Cd；总非致癌风险全部在可接受水平内。综上，该尾矿库周边农田土壤和水稻已受到重金属污染，存在一定的生态风险，对当地居民健康造成的风险值得重视。
Abstract:BACKGROUND The food security problem caused by heavy metal pollution in farmland soil has attracted widespread attention. Objective pollution investigation and evaluation work is of great significance for the later pollution prevention and safe utilization of soil.
OBJECTIVES To fully understand the heavy metal contamination condition, ecological risk and human health risk of soil and rice in the farmland around the copper-lead-zinc tailing pond in Western Hubei Province.
METHODS 50 sites of topsoil and rice were investigated systematically. ICP-MS, ICP-OES and AFS were used to determine the contents of eight heavy metals (As, Cd, Cu, Pb, Zn, Hg, Ni, Cr), as well as the pH value of the soil. The potential ecological risk index method and human health risk assessment model were used to evaluate the potential ecological risk and health risk of soil and rice.
RESULTS The results indicate that: (1) The contents of As, Cd, Cu, Pb and Zn in the soil exceed the standard, with the maximum exceedance rate of Cd being 20%. Only Cd in rice exceeds the standard with the exceedance rate of 14%. (2) Correlation analysis shows that soil heavy metals have the same pollution source, and leachate leakage is a possible source of pollution. There is a positive correlation between the heavy metals in rice and the surface soil, with the strongest correlation for Cd, which may be related to the strong absorption capacity of rice for soil Cd. (3) The evaluation results of potential ecological risk index show that Cd, Pb, Zn and Cu are significantly enriched in the soil, with the Cd enrichment coefficient of 4.41. The overall ecological risk is moderate, with 6% of the sites having very strong potential ecological risk. (4) The results of the health risk assessment indicate that the total and non-total carcinogenic risks are greater than the acceptable level at almost all sites. There is an overall risk of heavy metal carcinogenicity in the soil, with As and Cd being the major contributors. The total non-carcinogenic risk for rice at almost all sites in the study area is greater than the acceptable level, with Cd being the largest contributor. The total non-carcinogenic risk for rice at all sites is within the acceptable level.
CONCLUSIONS The soil and rice in the vicinity of the tailings pond have been contaminated by heavy metals, posing a certain ecological risk, and the risks to the health of the local population should be taken into account.
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表 1 健康风险评价模型计算公式
Table 1. Calculation formula of health risk assessment model
参数 计算公式 经口摄入 $ C D I_{\text {ingestion-soil }}=\frac{C_{\mathrm{i}} \times I R_{\text {soil }} \times C F \times E F \times E D}{B W \times A T}$ 皮肤接触 $ C D I_{\text {dermal-soil }}=\frac{C_{\mathrm{i}} \times S A \times A F \times A B S_{\mathrm{d}} \times C F \times E F \times E D}{B W \times A T}$ 呼吸摄入 $ C D I_{\text {inhale-soil }}=\frac{C_{\mathrm{i}} \times I R_{\text {air }} \times E F \times E D}{P E F \times B W \times A T}$ 食物摄入 $ C D I_{\text {oral }-\text { crop }}=\frac{C_{\mathrm{i}} \times I R_{\text {crop }} \times C F \times E F \times E D}{B W \times A T}$ 致癌风险 $ C R_{\mathrm{i}}=\sum\limits_{j=1}^3 C D I_{\mathrm{ij}} \times S F_{\mathrm{ij}}$ $ T C R=\sum\limits_{i=1} C R_{\mathrm{i}}$ 非致癌风险 $ H Q_{\mathrm{i}}=\sum\limits_{\mathrm{j}=1}^3 C D I_{\mathrm{ij}} / R f D_{\mathrm{ij}}$ $ H I=\sum\limits_{\mathrm{i}=1} H Q_{\mathrm{i}}$ 
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表 2 健康风险评价暴露参数
Table 2. Health risk assessment exposure parameters
参数 参数含义 成人 儿童 BW 平均体重(kg) 61.8 19.2 IRsoil 经口摄入速率(mg/d) 100 200 IRair 空气摄入速率(m3/d) 14.5 7.5 IRcrop 食物摄入速率(mg/d) 328 198 CF 转换因子(kg/mg) 1.00×10-6 1.00×10-6 EF 暴露频率(d/a) 350 350 ED 暴露年限(a) 24 6 SA 暴露皮肤表面积(cm2) 5374 2484 AF 皮肤对土壤黏附系数(mg·cm2) 0.07 0.2 PEF 土壤颗粒物扩散因子(m3/kg) 1.55×107 1.55×107 ABSd 皮肤吸收因子 As(0.03), Cd(0.001) AT 平均暴露时间(d) 27740(致癌), 2190(非致癌) 注：IRcrop参数来源于Mao等[34]，其他参数均来源于HJ 25.3—2019。
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表 3 重金属不同暴露途径参考计量(RfD)和致癌斜率因子(SF)
Table 3. Reference dose (RfD) and cancer slope factor (SF) of heavy metals by different exposed ways
暴露途径 参数 非致癌暴露参考剂量和致癌斜率因子 Cu Ni Zn Pb Cd Cr Hg As 经口摄入 RfD[mg/(kg·d)] 4.00×10-2 2.00×10-2 3.00×10-1 3.50×10-3 1.00×10-3 3.00×10-3 3.00×10-4 3.00×10-4 SF[kg·d/mg] / / / 8.50×10-3 6.10 5.00×10-1 / 1.50 皮肤接触 RfD[mg/(kg·d)] / / / 2.50×10-5 / / 3.00×10-4 SF[kg·d/mg] / / / 8.50×10-3 2.44×102 2.00 / 1.50 呼吸摄入 RfD [mg/(kg·d)] 1.20×10-2 2.11×10-5 3.00×10-1 2.89×10-3 2.35×10-6 2.35×10-5 7.04×10-5 3.52×10-6 SF [kg·d/mg] 1.11 / / 7.67 5.11×101 / 1.83×101 食物摄入 RfD [mg/(kg·d)] 4.00×10-2 2.00×10-2 3.00×10-1 3.50×10-3 1.00×10-3 3.00×10-3 3.00×10-4 3.00×10-4 SF [kg·d/mg] / / / 8.50×10-3 6.10 5.00×10-1 / 1.50 注：“/”表示HJ 25.3—2019暂无参考值及相应计算值。
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表 4 研究区土壤重金属含量和pH值结果统计
Table 4. Statistics of heavy metals content and pH of farmland soil from the study area
参数 pH(无量纲) As Cd Cu Pb Zn Hg Ni Cr 平均值(mg/kg) 6.98 12.3 0.76 46.2 68.1 182 0.057 33.9 74.8 中位数(mg/kg) 7.02 10.6 0.21 28.2 35.2 80.2 0.057 33.6 74.2 最大值(mg/kg) 8.15 54.1 10.8 409 763 2151 0.109 44.5 90.3 最小值(mg/kg) 4.97 6.41 0.10 19.3 26.3 54.7 0.020 22.5 59.6 湖北省背景值[32](mg/kg) / 12.3 0.172 30.7 26.7 83.6 0.08 37.3 86.0 超筛选值点位数 / 2 10 4 4 5 0 0 0 超标率% / 4 20 8 8 10 0 0 0 注：“/”表示无标准限值及相应计算值。
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表 5 研究区水稻重金属含量特征
Table 5. Characteristics of heavy metal contents in rice from the study area
参数 As(mg/kg) Cd (μg/kg) Cu (mg/kg) Pb(mg/kg) Zn (mg/kg) Hg (μg/kg) Ni (mg/kg) Cr (mg/kg) 标准限值 0.5 200 / 0.2 / 20 / 1.0 平均值 0.29 197 3.85 0.075 22.2 3.48 0.26 0.18 中位值 0.31 60.7 3.59 0.077 21.8 3.60 0.22 0.15 最大 0.46 2078 8.95 0.196 34.3 6.27 0.78 0.58 最小值 0.13 10.3 2.18 0.050 15.1 0.50 0.11 0.11 超标数 0 7 / 0 / 0 / 0 超标率(%) 0 14.0 / 0 / 0 / 0 注：“/”表示无标准限值及相应计算值。
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表 6 农田土壤不同重金属富集系数(Cif)和潜在生态风险(Ei)评价结果
Table 6. Assessment of enrichment factor (Cif) and potential ecological risk (Ei) of different heavy metals in farmland soil
参数 As Cd Cu Pb Zn Hg Ni Cr 富集系数(Cif) 平均值 1.00 4.41 1.50 2.55 2.17 0.72 0.91 0.87 中位数 0.86 1.22 0.92 1.32 0.96 0.71 0.90 0.86 最大值 4.40 62.8 13.3 28.6 25.7 1.36 1.19 1.05 最小值 0.52 0.58 0.63 0.99 0.65 0.25 0.60 0.69 潜在生态风险(Ei) 平均值 10.0 132 7.52 12.8 2.17 28.7 4.54 1.74 中位数 8.58 36.6 4.59 6.58 0.96 28.3 4.50 1.73 最大值 44.0 1884 66.6 143 25.7 54.5 5.97 2.10 最小值 5.21 17.4 3.14 4.93 0.65 10.0 3.02 1.39
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表 7 农田土壤和水稻中不同暴露途径重金属致癌风险和非致癌风险
Table 7. Carcinogenic risk and non-carcinogenic risk of heavy metals via different pathways in farmland soil and rice
风险类别 暴露途径 Cu Ni Zn Pb Cd Cr Hg As 合计 致癌风险(CR) 经口摄入 / / / 7.40×10-7 5.92×10-6 / / 2.36×10-5 3.02×10-5 皮肤摄入 / / / / 7.57×10-7 / / 2.26×10-6 3.02×10-6 呼吸吸入 / 2.45×10-7 / / 3.79×10-8 / / 1.47×10-6 1.75×10-6 合计 / 2.45×10-7 / 7.40×10-7 6.71×10-6 / / 2.73×10-5 3.50×10-5 非致癌风险(HQ) 经口摄入 2.30×10-2 3.39×10-2 1.21×10-2 3.89×10-1 1.52×10-2 9.96×10-4 5.79×10-3 8.19×10-1 1.30 皮肤摄入 / / / / 1.73×10-3 / / 7.00×10-2 7.17×10-2 呼吸吸入 1.86×10-4 7.78×10-2 2.94×10-5 1.14×10-3 1.57×10-2 1.10×10-1 5.99×10-5 1.69×10-1 3.75×10-1 合计 2.32×10-2 1.12×10-1 1.21×10-2 3.90×10-1 3.26×10-2 1.11×10-1 5.85×10-3 1.06 1.74 致癌风险(CR) 水稻摄入 / / / 1.73×10-9 2.87×10-6 / / 1.05×10-6 3.92×10-6 非致癌风险(HQ) 水稻摄入 1.90×10-3 2.59×10-4 1.47×10-3 4.82×10-4 3.89×10-3 2.36×10-6 3.48×10-4 1.94×10-2 2.77×10-2 注：“/”表示无参考值及相应计算值。
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