Study on Migration and Enrichment Characteristics and Risk Assessment of Heavy Metals (Metalloids) in Rock-Parent Material- Soil: Taking Typical Rock-Soil Profiles in Three Gorges Reservoir Area as Examples
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摘要:
笔者选取长江重点生区三峡库区（重庆段）4条典型岩石−土壤剖面，分析风化成土过程中重（类）金属元素（Cu、Pb、Zn、Cr、Ni、Cd、As、Hg）的迁移富集特征，探索该地段的典型健康风险。结果表明：①研究区侏罗纪碎屑岩风化剖面土壤呈弱碱性，二叠纪碳酸盐岩风化剖面土壤呈酸性、弱酸性，二叠纪碳酸盐岩母质土壤中各种元素含量基本高于侏罗纪碎屑岩母质土壤，8种重（类）金属元素含量均值都没有超过管制值。②同类土壤剖面中多种元素具有相似的迁移富集特征，各种元素的迁移富集规律受到成土母岩自身特性、淋溶淀积作用、黏土矿物吸附作用、大气降尘、元素地球化学性质和pH等多重因素的影响。③内梅罗综合污染指数显示研究区TP0301、TP0302剖面整体状况良好，无污染。TP0501和TP0502剖面由于元素Cd和As轻度超标造成轻度污染。④健康风险评价表明，儿童比成人更容易受到重（类）金属元素威胁，通过手−口摄入是土壤污染元素对人体引起非致癌健康风险的主要途径，研究区致癌风险较低，但 Cr 的重金属致癌健康风险指数 CR接近 1×10−6 ，应当引起关注。综合分析评价认为，研究区土壤整体状况良好，但二叠纪碳酸盐岩风化土壤剖面存在轻微的污染现象，考虑到研究区内居民的生命健康安全，建议加强二叠纪碳酸盐岩风化剖面中的类金属As和重金属Cr的监测关注。
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关键词:
- 生态地质 /
- 侏罗纪碎屑岩风化剖面 /
- 二叠纪碳酸盐岩风化剖面 /
- 元素迁移富集特征 /
- 重庆
Abstract:Four typical rock-soil profiles in the key ecological area of the Yangtze River (Chongqing section) were selected to explore the migration and enrichment characteristics of heavy metal elements ( Cu, Pb, Zn, Cr, Ni, Cd, As, Hg ) in the process of weathering and soil formation, and to explore the typical health risks in this area. The results show that the soil in the Jurassic clastic rock weathering profile in the study area is weakly alkaline, and the soil in the Permian carbonate rock weathering profile is acidic and weakly acidic. The content of various elements in the Permian carbonate rock parent material soil is basically higher than that in the Jurassic clastic rock parent material soil, and the average content of eight heavy metal elements does not exceed the control value; Various elements in the same soil profile have similar migration and enrichment characteristics. The migration and enrichment of various elements are affected by multiple factors such as the characteristics of the parent rock, leaching and deposition, clay mineral adsorption, atmospheric dustfall, elemental geochemical properties and pH; The Nemero comprehensive pollution index shows that the TP0301 and TP0302 profiles in the study area are in good condition and pollution-free. The TP0501 and TP0502 profiles were slightly polluted due to the light exceeding of Cd and As; Health risk assessment showed that children were more susceptible to heavy metal elements than adults. Hand-mouth ingestion was the main way of soil pollution elements causing non-carcinogenic health risks. The carcinogenic risk in the study area was low, but the carcinogenic health risk index CR of Cr was close to 1 × 10−6, which should be concerned. According to the comprehensive analysis and evaluation, the soil in the study area is in good condition as a whole, but there is slight pollution in the weathering soil profile of Permian carbonate rocks. Considering the life and health safety of residents in the study area, it is suggested to strengthen the monitoring of metalloid As and heavy metal Cr in the weathering profile of Permian carbonate rocks. However, the carcinogenic health risk index of Cr is close to 1 × 10−6, which should be concerned.
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图 1 研究区地质背景及采样点位置图
Figure 1. Geological background and sampling point location map of study area
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图 2 研究区二叠纪碳酸盐岩和侏罗纪碎屑岩风化剖面图
Figure 2. Weathering profile of Permian carbonate rocks and Jurassic clastic rocks in study area
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图 3 研究区质量平衡系数与采样深度关系图
（a）.TP0501；（b）.TP0502为二叠纪碳酸盐岩-石灰土剖面；（c）.TP0301；（d）. TP0302为侏罗纪碎屑岩-紫色土剖面
Figure 3. Relation diagram of mass balance coefficient and sampling depth in study area
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图 4 基岩（a）和风化土壤（b）中元素富集系数
Figure 4. (a) Enrichment factor of elements in bedrock and (b) Enrichment factor of elements in weathered soil
表 1 质量平衡系数参数表
Table 1 Mass balance coefficient parameter table
项目 参数名称/单位 范围 含义 Ci, W 元素i在风化层的实测含量（mg/kg） Ti, Zr = −1 元素i已经被全部迁移殆尽 Ci, P 元素i在基岩的实测含量（mg/kg） Ti, Zr＜0 元素i在风化和蚀变过程中有迁移或者损失 CZr, W 惰性元素Zr在风化层的含量（mg/kg） Ti, Zr= 0 元素i相对于新鲜基岩没有任何迁移 CZr, P 惰性元素Zr在基岩的含量（mg/kg） Ti, Zr＞0 有外来i元素的加入 
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表 2 土壤污染风险值
Table 2 Soil pollution risk value
元素 风险筛选值（标准） 风险管制值 pH≤5.5 5.5＜pH≤6.5 6.5＜pH≤7.5 pH＞7.5 pH≤5.5 5.5＜pH≤6.5 6.5＜pH≤7.5 pH＞7.5 Cd 0.3 0.3 0.3 0.6 1.5 2 3 4 Hg 1.3 1.8 2.4 3.4 2 2.5 4 6 As 40 40 30 25 200 150 120 100 Pb 70 90 120 170 400 500 700 1000 Cr 150 150 200 250 800 850 1000 1300 Cu 50 50 100 100 — — — — Ni 60 70 100 190 — — — — Zn 200 200 250 300 — — — — 注：表中风险筛选值依据《土壤环境质量农用地土壤污染风险管控标准（试行）（GB 15618—2018）》（下文简称为国标）。筛选值单位为mg/ kg。—为未检出，下同。
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表 3 单因子指数与内梅罗综合指数评价标准
Table 3 Single factor index and Nemero comprehensive index evaluation standard
等级 单因子指数 内梅罗综合指数 范围 污染评价 范围 污染评价 Ⅰ Pi≤1 清洁 P综≤0.7 安全 Ⅱ 1＜Pi≤2 轻度污染 0.7＜P综≤1.0 警戒线 Ⅲ 2＜Pi≤3 中度污染 1.0＜P综≤2.0 轻度污染 Ⅳ Pi＞3 重度污染 2.0＜P综≤3.0 中度污染 Ⅴ P综＞3.0 重度污染
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表 4 重金属健康风险暴露参数
Table 4 Heavy metal health risk exposure parameters
项目 参数名称及单位 成人参考值 儿童参考值 IngR 手−口摄入土壤频率（mg/d） 100 200 EF 暴露频率（d/a） 350 350 ED 暴露时间（a） 25 6 BW 平均体重（kg） 56.8 15.9 AT 平均暴露时间（d） 致癌 26280 ，非致癌9125 致癌 26280 ，非致癌2190 InhR 呼吸频率（m3/d） 14.5 7.5 PEF 颗粒物排放因子（m3/kg） 1.36×109 1.36×109 SA 皮肤暴露表面积（ cm2） 2415 1295 SL 皮肤粘附系数（mg/（cm2·d）） 0.2 0.2 ABS 皮肤吸收因子 0.001 0.001
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表 5 土壤中重金属不同暴露途径RfD 和 SF
Table 5 Different exposure pathways of heavy metals RfD and SF in soil
元素 RfD（mg/kg·d-1） SF（kg·d/mg） 呼吸吸入 手-口摄入 皮肤接触 呼吸吸入 Cu 4×10−2 4×10−2 1.2×10−2 — Pb 3.5×10−3 3.5×10−3 5.25×10−4 — Zn 3×10−1 3×10−1 6×10−2 — Cr 2.86×10−5 3×10−3 6×10−5 42 Ni 2.06×10−2 2×10−2 5.4×10−3 0.84 Cd 1×10−3 1×10−3 3×10−5 6.3 As 3×10−4 3×10−4 1.23×10−4 15.1 Hg 3×10−4 3×10−4 2.1×10−5 —
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表 6 研究区风化剖面元素含量与pH一览表
Table 6 List of element content and pH of weathering profile in the study area
剖面 样品 深度（cm） Cu Pb Zn Cr Ni Cd As Hg Zr pH TP0301 A 0～10 21.70 28.00 76.30 54.60 33.60 0.360 6.97 0.033 202.00 8.03 B1 10～20 21.50 26.30 76.50 56.20 32.40 0.270 7.56 0.017 211.00 8.19 B2 20～30 20.90 22.90 67.70 57.20 30.80 0.120 5.45 0.011 268.00 8.40 B3 30～50 18.80 23.40 65.60 58.00 30.60 0.120 4.68 0.011 244.00 8.47 C1 50～65 18.10 32.20 82.80 65.00 41.30 0.320 6.22 0.010 130.00 8.58 C2 65～80 17.20 25.00 73.20 61.90 34.90 0.200 4.25 0.010 191.00 8.45 土壤均值 — 19.70 26.30 73.68 58.82 33.93 0.232 5.86 0.015 207.67 — R ＞80 14.00 19.40 40.40 44.40 21.40 0.120 2.35 0.009 172.00 — TP0302 A 0～10 31.60 30.80 74.40 54.50 30.90 0.390 7.39 0.025 212.00 8.00 B1 10～20 20.20 29.40 80.70 55.00 36.70 0.220 7.74 0.013 197.00 8.27 B2 20～30 18.70 32.00 84.10 60.60 35.80 0.140 8.26 0.008 178.00 8.26 C 30～40 16.00 21.60 58.70 51.40 25.60 0.089 4.33 0.005 224.00 8.59 土壤均值 — 21.63 28.45 74.48 55.38 32.25 0.210 6.93 0.013 202.75 — R ＞40 15.80 21.20 63.20 48.30 24.80 0.080 3.06 0.003 238.00 — TP0501 A1 0～7 30.80 46.60 110.00 96.70 34.40 0.580 26.80 0.160 252.00 5.53 A2 7～15 29.00 47.30 122.00 98.60 36.00 0.580 26.20 0.170 259.00 5.01 E1 15～25 24.80 49.40 143.00 95.00 34.50 0.780 21.80 0.230 227.00 5.28 E2 25～35 22.10 36.70 119.00 84.80 30.80 0.660 20.60 0.200 198.00 5.62 B1 35～45 21.40 29.40 93.50 79.00 27.30 0.370 22.50 0.160 182.00 5.86 B2 45～60 28.00 35.20 102.00 106.00 38.90 0.380 24.50 0.200 232.00 6.04 C1 60～85 27.20 44.20 122.00 100.00 37.50 0.490 26.20 0.170 271.00 5.39 C2 85～110 30.00 49.40 128.00 99.40 38.00 0.390 26.40 0.180 252.00 5.34 土壤均值 — 26.66 42.28 117.44 94.94 34.68 0.529 24.38 0.184 234.13 — R ＞110 0.96 0.27 2.29 6.65 0.24 0.038 0.50 0.002 6.90 — TP0502 A1 0～10 40.30 46.20 121.00 117.00 40.30 0.660 43.70 0.180 259.00 5.00 A2 10～20 31.50 45.30 120.00 129.00 43.00 0.520 46.50 0.190 264.00 5.27 E1 20～40 29.00 50.60 129.00 107.00 42.00 0.330 26.90 0.220 266.00 4.97 E2 40～60 28.70 48.90 129.00 108.00 37.90 0.460 23.30 0.220 238.00 4.96 B1 60～75 24.20 24.40 76.40 68.80 36.50 0.440 15.30 0.200 138.00 5.62 B2 75～90 36.50 32.20 105.00 88.70 54.70 0.620 18.00 0.270 149.00 6.74 C1 90～120 30.00 50.20 128.00 121.00 42.40 0.400 41.80 0.220 256.00 5.30 C2 120～150 30.80 50.90 131.00 121.00 41.80 0.360 31.50 0.190 258.00 5.14 土壤均值 — 31.38 43.59 117.43 107.56 42.33 0.474 30.88 0.211 228.50 — R ＞150 2.01 0.29 5.15 4.36 3.44 0.045 0.50 0.001 7.90 — 超管制值/% 0.00 0.00 0.00 0.00 0.00 0.000 0.00 0.000 — — 上地壳丰度（UCC） 28.00 17.00 67.00 92.00 47.00 0.090 4.80 0.050 — — 重庆土壤背景值 24.60 28.10 81.90 74.40 31.60 0.280 6.62 0.069 — — 中国土壤背景值 22.60 26.00 74.20 61.00 26.90 0.097 11.20 0.065 — — 世界土壤 30.00 19.00 90.00 40.00 20.00 0.350 — — — — 注：表中字母A代表腐殖层，E代表淋溶层，B代表淀积层，C代表母质层，R代表基岩层；元素的含量为mg/kg，PH无量纲。
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表 7 研究区剖面土壤重金属元素单因子指数和内梅罗指数评价结果
Table 7 The evaluation results of single factor index and Nemero index of heavy metal elements in soil profile of the study area
剖面 样品 PCu PPb PZn PCr PNi PCd PAs PHg Pave Pmax P综 等级 TP0301 A 0.217 0.165 0.254 0.218 0.177 0.600 0.279 0.010 0.204 0.600 0.317 安全 B1 0.215 0.155 0.255 0.225 0.171 0.450 0.302 0.005 B2 0.209 0.135 0.226 0.229 0.162 0.200 0.218 0.003 B3 0.188 0.138 0.219 0.232 0.161 0.200 0.187 0.003 C1 0.181 0.189 0.276 0.260 0.217 0.533 0.249 0.003 C2 0.172 0.147 0.244 0.248 0.184 0.333 0.170 0.003 TP0302 A 0.316 0.181 0.248 0.218 0.163 0.650 0.296 0.007 0.207 0.650 0.312 安全 B1 0.202 0.173 0.269 0.220 0.193 0.367 0.310 0.004 B2 0.187 0.188 0.280 0.242 0.188 0.233 0.330 0.002 C 0.160 0.127 0.196 0.206 0.135 0.148 0.173 0.001 TP0501 A1 0.616 0.518 0.550 0.645 0.491 1.933 0.670 0.089 0.666 2.600 1.335 轻度
污染A2 0.580 0.676 0.610 0.657 0.600 1.933 0.655 0.131 E1 0.496 0.706 0.715 0.633 0.575 2.600 0.545 0.177 E2 0.442 0.408 0.595 0.565 0.440 2.200 0.515 0.111 B1 0.428 0.327 0.468 0.527 0.390 1.233 0.563 0.089 B2 0.560 0.391 0.510 0.707 0.556 1.267 0.613 0.111 C1 0.544 0.631 0.610 0.667 0.625 1.633 0.655 0.131 C2 0.600 0.706 0.640 0.663 0.633 1.300 0.660 0.138 TP0502 A1 0.806 0.660 0.605 0.780 0.672 2.200 1.093 0.138 0.701 2.200 1.226 轻度
污染A2 0.630 0.647 0.600 0.860 0.717 1.733 1.163 0.146 E1 0.580 0.723 0.645 0.713 0.700 1.100 0.673 0.169 E2 0.574 0.699 0.645 0.720 0.632 1.533 0.583 0.169 B1 0.484 0.271 0.382 0.459 0.521 1.467 0.383 0.111 B2 0.365 0.268 0.420 0.444 0.547 2.067 0.600 0.113 C1 0.600 0.717 0.640 0.807 0.707 1.333 1.045 0.169 C2 0.616 0.727 0.655 0.807 0.697 1.200 0.788 0.146
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表 8 健康风险评价结果
Table 8 Health risk assessment results
剖面 元素 HQing HQinh HQderm HI CR 成人 儿童 成人 儿童 成人 儿童 成人 儿童 成人 儿童 TP0301 Cu 8.67×10−4 6.50×10−3 9.24×10−8 1.79×10−7 1.40×10−5 2.81×10−5 8.81×10−4 6.53×10−3 — — Pb 1.28×10−2 9.59×10−2 1.36×10−6 2.64×10−6 4.12×10−4 8.28×10−4 1.32×10−2 9.67×10−2 — — Zn 4.06×10−4 3.05×10−3 4.33×10−8 8.41×10−8 9.82×10−6 1.97×10−5 4.16×10−4 3.07×10−3 — — Cr 2.91×10−2 2.18×10−1 3.25×10−4 6.31×10−4 7.02×10−3 1.41×10−2 3.64×10−2 2.33×10−1 1.36×10−7 1.99×10−7 Ni 2.68×10−3 2.01×10−2 2.78×10−7 5.39×10−7 4.80×10−5 9.66×10−5 2.73×10−3 2.02×10−2 1.67×10−9 2.45×10−9 Cd 5.75×10−4 4.32×10−3 6.13×10−8 1.19×10−7 9.26×10−5 1.86×10−4 6.68×10−4 4.50×10−3 1.34×10−10 1.97×10−10 As 3.71×10−2 2.78×10−1 3.96×10−6 7.68×10−6 4.37×10−4 8.80×10−4 3.76×10−2 2.79×10−1 6.23×10−9 9.13×10−9 Hg 1.76×10−4 1.32×10−3 1.87×10−8 3.64×10−8 1.21×10−5 2.44×10−5 1.88×10−4 1.34×10−3 — — TP0302 Cu 1.26×10−3 9.47×10−3 1.35×10−7 2.61×10−7 2.03×10−5 4.09×10−5 1.28×10−3 9.51×10−3 — — Pb 1.41×10−2 1.05×10−1 1.50×10−6 2.91×10−6 4.53×10−4 9.11×10−4 1.45×10−2 1.06×10−1 — — Zn 3.96×10−4 2.97×10−3 4.23×10−8 8.20×10−8 9.57×10−6 1.92×10−5 4.06×10−4 2.99×10−3 — — Cr 2.90×10−2 2.18×10−1 3.25×10−4 6.30×10−4 7.01×10−3 1.41×10−2 3.64×10−2 2.32×10−1 1.35×10−7 1.98×10−7 Ni 2.47×10−3 1.85×10−2 2.56×10−7 4.96×10−7 4.42×10−5 8.88×10−5 2.51×10−3 1.86×10−2 1.54×10−9 2.25×10−9 Cd 6.23×10−4 4.67×10−3 6.65×10−8 1.29×10−7 1.00×10−4 2.02×10−4 7.24×10−4 4.88×10−3 1.45×10−10 2.13×10−10 As 3.94×10−2 2.95×10−1 4.20×10−6 8.14×10−6 4.64×10−4 9.33×10−4 3.98×10−2 2.96×10−1 6.60×10−9 9.68×10−9 Hg 1.33×10−4 9.99×10−4 1.42×10−8 2.75×10−8 9.19×10−6 1.85×10−5 1.42×10−4 1.02×10−3 — — TP0501 Cu 1.23×10−3 9.23×10−3 1.31×10−7 2.54×10−7 1.98×10−5 3.98×10−5 1.25×10−3 9.27×10−3 — — Pb 2.13×10−2 1.60×10−1 2.27×10−6 4.40×10−6 6.85×10−4 1.38×10−3 2.20×10−2 1.61×10−1 — — Zn 5.86×10−4 4.39×10−3 6.25×10−8 1.21×10−7 1.42×10−5 2.85×10−5 6.00×10−4 4.42×10−3 — — Cr 5.15×10−2 3.86×10−1 5.76×10−4 1.12×10−3 1.24×10−2 2.50×10−2 6.45×10−2 4.12×10−1 2.40×10−7 3.52×10−7 Ni 2.75×10−3 2.06×10−2 2.85×10−7 5.52×10−7 4.92×10−5 9.89×10−5 2.80×10−3 2.07×10−2 1.71×10−9 2.51×10−9 Cd 9.27×10−4 6.95×10−3 9.88×10−8 1.92×10−7 1.49×10−4 3.00×10−4 1.08×10−3 7.25×10−3 2.16×10−10 3.17×10−10 As 1.43×10−1 1.07×100 1.52×10−5 2.95×10−5 1.68×10−3 3.38×10−3 1.44×10−1 1.07×100 2.39×10−8 3.51×10−8 Hg 8.52×10−4 6.39×10−3 9.09×10−8 1.76×10−7 5.88×10−5 1.18×10−4 9.11×10−4 6.51×10−3 — — TP0502 Cu 1.61×10−3 1.21×10−2 1.72×10−7 3.33×10−7 2.59×10−5 5.21×10−5 1.64×10−3 1.21×10−2 — — Pb 2.11×10−2 1.58×10−1 2.25×10−6 4.36×10−6 6.79×10−4 1.37×10−3 2.18×10−2 1.60×10−1 — — Zn 6.45×10−4 4.83×10−3 6.87×10−8 1.33×10−7 1.56×10−5 3.13×10−5 6.60×10−4 4.87×10−3 — — Cr 6.23×10−2 4.67×10−1 6.97×10−4 1.35×10−3 1.51×10−2 3.03×10−2 7.81×10−2 4.99×10−1 2.91×10−7 4.26×10−7 Ni 3.22×10−3 2.42×10−2 3.33×10−7 6.47×10−7 5.76×10−5 1.16×10−4 3.28×10−3 2.43×10−2 2.00×10−9 2.94×10−9 Cd 1.05×10−3 7.91×10−3 1.12×10−7 2.18×10−7 1.70×10−4 3.41×10−4 1.22×10−3 8.25×10−3 2.46×10−10 3.61×10−10 As 2.33×10−1 1.75×100 2.48×10−5 4.81×10−5 2.74×10−3 5.51×10−3 2.36×10−1 1.75×100 3.90×10−8 5.72×10−8 Hg 9.59×10−4 7.19×10−3 1.02×10−7 1.98×10−5 6.62×10−5 1.33×10−4 1.03×10−3 7.33×10−3 — —
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