Potential Ecological and Human Health Risks of Heavy Metals in Soils in Selected Copper Mining Areas—A Case Study: The Bor Area
Abstract
:1. Introduction
2. Material and Methods
2.1. Sample Localization and Collection
2.2. Sample Preparation and Analytical Methods
2.3. Metal Analysis and Quality Control
2.4. Pollution Assessment
2.5. Human Health Risk Assessment
2.6. Data Analysis
3. Results and Discussions
3.1. Metal Levels and Pollution Assessment in Soils
3.2. Metal Levels in Plants
3.3. Metal Trasfer from Soil to Plants
3.4. Health Risk Assessment
4. Conclusions
- The highest and the lowest amounts of soil Zn, Cu, Fe, Mn, and Pb were regularly found at site S1 and site R, respectively. The measured values were below the benchmarks given in the relevant Serbian and European Directives, except for Cu. This metal was found at concentrations above the maximum allowable concentration (MAC) for Serbia at site S1, as well as above the threshold value (TV) for Serbia at sites S2 and S3. Application of different pollution indices revealed low-to-moderate contamination levels at sites S1, S2 and S3, with Cu—likely deriving from anthropogenic activities—being the main contaminant of environmental concern.
- No evidence of phytotoxicity could be found from the levels of Zn, Cu, Fe, Mn, and Pb in the spontaneous vegetation collected, indicating a relatively low ecotoxicological risk for sites analyzed in this work. The safe limit suggested by WHO/FAO for Cu (40 mg kg−1 dw) and Pb (0.3 mg kg−1 dw) in plant foodstuffs were respectively exceeded in leafy vegetables (dill, sorrel) and celery roots, and in most vegetables, excluding potatoes.
- Metal concentrations in aerial parts of spontaneous plant species were often significantly lower than the values determined in the corresponding soils. This trend was most consistent in dandelion and for Cu and Pb. Significantly reduced Pb, Fe, and Mn also tended to occur in vegetables. In contrast, Cu was found at significantly elevated levels in celery roots and sorrel leaves, whereas Zn tended to show similar values to that seen in soils.
- Assessment of non-carcinogenic risk associated with consumption of vegetables grown in relatively unpolluted soils from the Bor area was conducted using the current methodology (US EPA–WHO FAO) via calculating the target hazard quotients (THQs) and the total target hazard quotients (TTHQs), with RfDs for most metals being based on gastrointestinal tract irritation. It was found that consumption of celery roots and carrot roots in the case of females (1.41; 1.05) and carrot roots in the case of males (1.15; 1.02) might pose a long-term risk of non-carcinogenic effects, with the main potential contributors being Cu and Fe.
- Expansion of present research to other plant species (cereals, fruits, and other vegetables), locations, and routes of metal exposure, e.g., consumption of animal foods (meat, milk, and eggs), drinking water, or contact with air, is imperative for enlarging our understanding of populational risk associated with Cu mining and processing in the Bor area specifically, and other areas with a long history of non-ferrous metal pollution in general.
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
References
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Zn | Cu | Fe | Mn | Pb | Reference | |
---|---|---|---|---|---|---|
Concentration range in surface horizons (worldwide) | 17–125 | 1–140 | 1000–100,000 | 7–9200 | 1.5−176 | [1] |
Mean concentration in surface horizons (worldwide) | 64 | 14 | 45,000 | 437 | 25 | [2] |
Mean level in upper continental crust | 67 | 28 | - | 438.59 | 17 | [33] |
71 | 25 | - | - | 17 | [34] | |
Limit values in soils as per European Council Directive 86/278/EEC | 150–300 | 50–140 | 50–300 | - | - | [35] |
Threshold values (TV) for Serbia | 140 | 36 | - | - | 85 | [36] |
Maximum allowable concentrations (MAC) for Serbia | 300 | 100 | - | - | 100 | [36] |
Intervention values (IV) for Serbia | 720 | 190 | - | - | 530 | [36] |
Site R | 10.51 | 25.97 | 112.24 | 41.01 | 7.88 | |
Site S1 | 20.24 | 122.01 | 234.92 | 46.20 | 3.27 | |
Site S2 | 19.15 | 82.04 | 167.31 | 59.02 | 12.47 | |
Site S3 | 23.53 | 84.99 | 182.07 | 23.18 | 12.94 | |
Bor (16 sites) | 40–890 (240.1) | 440–3800 (1558.6) | 16,200–58,200 (29,462.5) | 55–900 (459.9) | 21–1700 (264.1) | [14] |
Bor (8 sites) | 43.4–465 | 9.2–1586 | 10,010–19,245 | - | 21.99–238.4 | [15] |
Bor (12 sites) | - | 220–2540 (913.33) | - | 460–1300 (1070) | 40–230 (86.67) | [12] |
Bor (5 sites) | 72–126 | 84–408 | - | - | 5.8–57.5 | [13] |
Moldova Nouă | 197.03 | 229.15 | 44,582.45 | 1,845.28 | 22.02 | [17] |
Phytotoxic values | 100–500 | 36–698 | - | - | 100–500 | [37] |
Zn | Cu | Fe | Mn | Pb | ||
---|---|---|---|---|---|---|
Igeo | Site S1 | −2.32 | 1.86 | −8.17 | −3.83 | −1.18 |
Site S2 | −2.40 | 1.29 | −8.66 | −3.47 | −3.59 | |
Site S3 | −2.90 | 1.34 | −8.53 | −4.82 | −3.30 | |
Site R | −3.26 | −0.37 | −9.23 | −4.00 | −1.14 | |
EF | Site S1 | 0.22 | 4.05 | 0.08 | 0.49 | |
Site S2 | 0.30 | 3.82 | 0.14 | 0.66 | ||
Site S3 | 0.19 | 3.64 | 0.05 | 0.63 | ||
Site R | 0.24 | 1.80 | 0.15 | 0.62 | ||
Pi | Site S1 | 0.30 | 5.46 | 0.005 | 0.11 | 0.66 |
Site S2 | 0.28 | 3.67 | 0.004 | 0.14 | 0.63 | |
Site S3 | 0.20 | 3.81 | 0.004 | 0.05 | 0.66 | |
Site R | 0.16 | 1.16 | 0.002 | 0.09 | 0.40 | |
PIN | Site S1 | 1.12 | ||||
Site S2 | 0.76 | |||||
Site S3 | 0.78 | |||||
Site R | 0.24 |
Zn | Cu | Fe | Mn | Pb | |
---|---|---|---|---|---|
Dandelion (site S1) | 15.04 (3.51) | 83.38 (9.46) | 71.05 (3.08) | 39.87 (2.69) | 4.04 (0.81) |
Dandelion (site S2) | 10.22 (0.86) | 61.05 (1.58) | 75.89 (3.16) | 41.17 (1.53) | 1.72 (0.25) |
Dandelion (site S3) | 7.18 (1.10) | 21.23 (2.01) | 17.28 (1.43) | 6.76 (0.73) | 0.37 (0.11) |
Coltsfoot (site S1) | 10.36 (1.01) | 34.84 (1.95) | 44.01 (3.89) | 4.36 (1.77) | 3.12 (0.75) |
Coltsfoot (site S2) | 15.15 (4.63) | 63.41 (2.31) | 148.52 (6.18) | 52.67 (4.19) | 1.58 (0.30) |
Coltsfoot (site S3) | 9.43 (1.87) | 69.39 (6.43) | 92.59 (2.99) | 3.65 (0.32) | 0.79 (010) |
Nettle (site S1) | 17.07 (1.65) | 56.69 (3.28) | 39.48 (1.33) | 42.34 (1.19) | 3.54 (0.38) |
Nettle (site S2) | 17.90 (2.36) | 45.19 (4.39) | 66.15 (5.58) | 46.03 (3.10) | 0.35 (0.11) |
Nettle (site S3) | 12.04 (0.34) | 16.64 (0.39) | 166.28 (12.91) | 8.37 (1.20) | 1.90 (0.13) |
Creeping buttercup (site S1) | 13.76 (1.06) | 35.64 (4.62) | 15.46 (2.62) | 15.11 (1.59) | 1.30 (0.26) |
Creeping buttercup (site S2) | 13.17 (1.75) | 68.45 (8.79) | 63.90 (2.11) | 55.98 (2.88) | 0.75 (0.12) |
Creeping buttercup (site S3) | 9.85 (2.17) | 42.65 (2.41) | 103.29 (5.49) | 6.58 (0.81) | 2.99 (0.84) |
Potatoes tubers (site R) | 6.22 (1.31) | 2.69 (0.55) | 4.33 (2.24) | 4.36 (2.44) | 0.11 (0.01) |
Onion bulbs (site R) | 5.48 (1.72) | 3.94 (0.27) | 6.68 (1.17) | 9.96 (2.48) | 0.45 (0.16) |
Garlic bulbs (site R) | 11.53 (2.59) | 6.76 (1.77) | 7.40 (1.23) | 3.82 (0.99) | 0.43 (0.14) |
Carrot roots (site R) | 22.30 (4.16) | 32.39 (5.50) | 33.74 (2.43) | 29.63 (2.67) | 0.69 (0.11) |
Parsley roots (site R) | 19.35 (3.48) | 19.48 (3.82) | 23.41 (4.89) | 34.63 (5.04) | 0.64 (0.12) |
Celery roots (site R) | 22.14 (4.61) | 53.69 (7.33) | 56.28 (9.15) | 26.55 (7.48) | 0.82 (0.13) |
Dill leaves (site R) | 13.21 1.47) | 44.34 (3.73) | 28.10 (3.41) | 14.04 (2.96) | 2.73 (1.05) |
Sorrel leaves (site R) | 19.88 (3.77) | 25.97 (5.31) | 12.75 (3.56) | 5.17 (1.62) | 1.84 (0.53) |
Zn | Cu | Fe | Mn | Pb | Reference | |
---|---|---|---|---|---|---|
Normal range in plants | 1–400 | 5–20 | 40–500 | 20–1000 | 0.2–20 | [37,42,43,44] |
Critical values in plants | 100–400 | 20–100 | - | 30–500 | 30–300 | [37,42,43,44] |
Phytotoxic values | 400 | 200 | - | 3000 | 100–500 | [1] |
Common dandelion (leaves) | 28.8–90.3 | 42.9–192.5 | - | - | 2.7–17.8 | [45] |
Nettle (leaves) | 32.1–60.8 | 85.9–171.6 | - | - | 3.4–17.3 | |
Soapwort (leaves) | 800 | 350 | 100 | 23 | 18 | [14] |
Soapwort (stems) | 280 | 150 | 90 | 10 | 9 | |
Orange mullein (leaves) | 1400 | 630 | 130 | 25 | 1400 | |
Orange mullein (stems) | 590 | 70 | 30 | 10 | 590 | |
Brown knapweed (leaves) | 380 | 200 | 60 | 14 | 9 | |
Brown knapweed (stems) | 390 | 70 | 30 | 5 | 8 | |
Parsley roots | 7.74 * | 6.88 * | 99.02 * | 8.10 * | 0.66 * | [17] |
Carrot roots | 3.18 * | 1.77 * | 31.89 * | 2.23 * | 0.09 * | |
Bulb onions | 2.01 * | 1.37 * | 4.65 * | 1.34 * | 0.13 * | |
Cabbage leaves | 8.51 * | 2.77 * | 31.53 * | 9.15 * | 0.25 * | |
Letuce leaves | 5.14 * | 2.22 * | 16.90 * | 4.12 * | 0.21 * | |
Parsley leaves | 10.44 | 4.79 * | 106.75 * | 9.72 * | 0.50 * | |
Potatoes (tuberized roots) | 4.14 | 7.36 * | 10.42 * | 3.92 * | 0.45 * | [21] |
FAO | 60 | 40 | 450 | 500 | 0.30 | [44] |
Sex | Vegetal Food | THQ (Zn) | THQ (Cu) | THQ (Fe) | THQ (Mn) | THQ (Pb) | Sum THQ |
---|---|---|---|---|---|---|---|
Male | Potatoes tubers | 0.04 | 0.02 | 0.03 | 0.03 | 0.00 | 0.13 |
Onion bulbs | 0.04 | 0.03 | 0.05 | 0.07 | 0.00 | 0.19 | |
Garlic bulbs | 0.08 | 0.05 | 0.05 | 0.03 | 0.00 | 0.22 | |
Carrot roots | 0.16 | 0.23 | 0.24 | 0.21 | 0.01 | 0.85 | |
Parsley roots | 0.14 | 0.14 | 0.17 | 0.25 | 0.00 | 0.70 | |
Celery roots | 0.16 | 0.39 | 0.41 | 0.19 | 0.01 | 1.15 | |
Dill leaves | 0.04 | 0.25 | 0.09 | 0.04 | 0.01 | 0.43 | |
Sorrel leaves | 0.06 | 0.14 | 0.04 | 0.02 | 0.01 | 0.26 | |
Female | Potatoes tubers | 0.05 | 0.02 | 0.04 | 0.04 | 0.00 | 0.16 |
Onion bulbs | 0.02 | 0.01 | 0.03 | 0.04 | 0.00 | 0.10 | |
Garlic bulbs | 0.10 | 0.06 | 0.07 | 0.03 | 0.00 | 0.26 | |
Carrot roots | 0.20 | 0.28 | 0.30 | 0.26 | 0.01 | 1.05 | |
Parsley roots | 0.17 | 0.17 | 0.21 | 0.31 | 0.01 | 0.86 | |
Celery roots | 0.20 | 0.47 | 0.50 | 0.23 | 0.01 | 1.41 | |
Dill leaves | 0.05 | 0.30 | 0.11 | 0.05 | 0.01 | 0.52 | |
Sorrel leaves | 0.08 | 0.17 | 0.05 | 0.02 | 0.01 | 0.32 |
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Filimon, M.N.; Caraba, I.V.; Popescu, R.; Dumitrescu, G.; Verdes, D.; Petculescu Ciochina, L.; Sinitean, A. Potential Ecological and Human Health Risks of Heavy Metals in Soils in Selected Copper Mining Areas—A Case Study: The Bor Area. Int. J. Environ. Res. Public Health 2021, 18, 1516. https://doi.org/10.3390/ijerph18041516
Filimon MN, Caraba IV, Popescu R, Dumitrescu G, Verdes D, Petculescu Ciochina L, Sinitean A. Potential Ecological and Human Health Risks of Heavy Metals in Soils in Selected Copper Mining Areas—A Case Study: The Bor Area. International Journal of Environmental Research and Public Health. 2021; 18(4):1516. https://doi.org/10.3390/ijerph18041516
Chicago/Turabian StyleFilimon, Marioara Nicoleta, Ion Valeriu Caraba, Roxana Popescu, Gabi Dumitrescu, Doina Verdes, Liliana Petculescu Ciochina, and Adrian Sinitean. 2021. "Potential Ecological and Human Health Risks of Heavy Metals in Soils in Selected Copper Mining Areas—A Case Study: The Bor Area" International Journal of Environmental Research and Public Health 18, no. 4: 1516. https://doi.org/10.3390/ijerph18041516