Skip to main content
SpringerLink
Log in

A new approach to evaluate toxic metal transport in a catchment

  • Published:
Environmental Monitoring and Assessment Aims and scope Submit manuscript

Abstract

Competitive sorption and desorption of Cd2+, Pb2+, and Hg2+ onto riverbank and sediment samples of an area impacted by pyritic residue in a Southern Brazilian catchment were evaluated. Although these ions are considered poorly mobile, a new approach has been proposed to assess their behavior and associated risk. In this sense, factorial design and three-dimensional surface methodology are proposed to describe the competitive sorption behavior of the metal ion in the environmental matrix, as well as an innovative mobilization factor (MF) to describe the desorption rate from the integration of the normalized difference of sorption-desorption fluorescence peaks. Sorption was carried out with a central composite factorial design (23) to estimate simultaneous effects of independent variables. Three-dimensional surface analysis indicated increasing Cd2+ equilibrium concentration (Ceq) with Hg2+ and Pb2+ initial concentration (Ci), showing synergistic effect and low Cd2+ affinity to the solid phase. Statistical analysis presented \(C_{i_{\text {Hg}}}\) as a significant variable for cadmium and lead dynamics, although \(C_{i_{\text {Pb}}}\) was also significant for Hg2+ releasing to the liquid phase. After integrating the sorption and desorption fluorescence peaks, the MF for Cd2+, Pb2+, and Hg2+ was around 0.2, 0.5, and 0.1 in riverbank sediment, and 0.3, 0.9, and 0.1 in sediment, respectively. Hence, consistent ion mobilization along the river was observed, with Pb2+ mobilizing 9 and 6 times more than Hg2+ and Cd2+, respectively. The transport of ions such as Pb2+ and Hg2+, usually considered immobile, has indeed occurred, causing contamination through the watershed and increasing environmental risk.

A new approach to determine toxic metal mobilization factor in a river catchment.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5

Similar content being viewed by others

References

  • Ahmadi, M., Vahabzadeh, F., Bonakdarpour, B., Mofarrah, E., Mehranian, M. (2005). Application of the central composite design and response surface methodology to the advanced treatment of olive oil processing wastewater using Fenton’s peroxidation. Journal of Hazardous Materials, 123(1), 187–195.

    CAS  Google Scholar 

  • Ali, H., Khan, E., Sajad, M. (2013). Phytoremediation of heavy metals - concepts and applications. Chemosphere, 91, 869–881.

    CAS  Google Scholar 

  • ATSDR. (2015). Priority List of Hazardous Substances. Agency for Toxic Substances and Disease Registry. U.S. Department of Health and Human Services. Public Health Service, Division of Toxicology and Human Health Sciences (proposed). Environmental Toxicology Branch (proposed). 1600 Clifton road NE. Mailstop f-62. Atlanta, Georgia 30333.

  • Baird, C. (2012). Environmental chemistry, 5th edn. New York: W.H. Freeman and Company.

    Google Scholar 

  • Bezerra, M., Santelli, E.R., Oliveira, E., villar, L., escaleira, L. (2008). Response surface methodology (RSM,) as a tool for optimization in analytical chemistry. Talanta, 76(5), 965–977.

    CAS  Google Scholar 

  • Bingol, D., Saraydin, D., Ozbay, D.S. (2015). Full factorial design approach to Hg(II) adsorption onto hydrogels. Arabian Journal for Science and Engineering, 40(1), 109–116.

    CAS  Google Scholar 

  • Bolan, N., Kunhikrishnanc, A., Thangarajana, R., Kumpiened, J., Parke, J., Makinof, T., Kirkhamg, M., Scheckelh, K. (2014). Remediation of heavy metal(loid)s contaminated soils - to mobilize or to immobilize?. Journal of Hazardous Materials, 266, 141–166.

    CAS  Google Scholar 

  • Box, G., Hunter, J., Hunter, W. (2005). Statistics for experimenters: design, innovation, and discovery, 2nd edn. New Jersey: Wiley-Interscience.

    Google Scholar 

  • Bui, A., Nguyen, H., Nguyen, M., Tran, T., Vu, T., Nguyen, C., Reynolds, H. (2016). Accumulation and potential health risks of cadmium, lead and arsenic in vegetables grown near mining sites in Northern Vietnam. Environmental monitoring and assessment, 188(9), 525.

    Google Scholar 

  • Butler, B. (2009). Effect of pH, ionic strength, dissolved organic carbon, time, and particle size on metals release from mine drainage impacted streambed sediments. Water Research, 43(5), 1392–1402.

    CAS  Google Scholar 

  • Cesar, R., Egler, S., Polivanov, H., Castilhos, Z., Rodrigues, A. (2011). Mercury, copper and zinc contamination in soils and fluvial sediments from an abandoned gold mining area in southern Minas Gerais State, Brazil. Environmental Earth Sciences, 64(1), 211–222.

    CAS  Google Scholar 

  • Cesareo, R. (2010). X-ray fluorescence spectrometry. Hoboken: Wiley Online Library.

    Google Scholar 

  • Cho, I., & Zoh, K. (2007). Photocatalytic degradation of azo dye (Reactive Red 120) in TiO 2/UV system: optimization and modeling using a response surface methodology (RSM) based on the central composite design. Dyes and Pigments, 75(3), 533–543.

    CAS  Google Scholar 

  • Chotpantarat, S., Ong, S., Sutthirat, C., Osathaphan, K. (2011). Competitive sorption and transport of Pb2+, Ni2+, Mn2+, and Zn2+ in lateritic soil columns. Journal of Hazardous Materials, 190(1), 391–396.

    CAS  Google Scholar 

  • Consani, S., Carbone, C., Dinelli, E., Balić-žunić, T., Cutroneo, L., Capello, M., Salviulo, G., Lucchetti, G. (2017). Metal transport and remobilisation in a basin affected by acid mine drainage: the role of ochreous amorphous precipitates. Environmental science and pollution Research, 1–13.

  • Constantino, L., Quirino, J., Monteiro, A., Abrao, T., Parreira, P., Urbano, A., Santos, M. (2017). Sorption-desorption of selenite and selenate on Mg-Al layered double hydroxide in competition with nitrate, sulfate and phosphate. Chemosphere, 181, 627–634.

    CAS  Google Scholar 

  • de Oliveira, L., Cabral, M., Vieira, C., Antoniazzi, M., Risso, W., dos Reis Martinez, C. (2016). Metals bioaccumulation and biomarkers responses in the neotropical freshwater clam anodontites trapesialis: implications for monitoring coal mining areas. The Science of the Total Environment, 571, 983–991.

    Google Scholar 

  • de Oliveira, L., Cabral, M., Risso, W., dos Reis Martinez, C. (2018a). Single and combined effects of Zn, Mn and Fe on the neotropical freshwater bivalve anodontites trapesialis: bioaccumulation and biochemical biomarkers. Ecotoxic. Environ. Safety, 161, 735–745.

    CAS  Google Scholar 

  • de Oliveira, L., Santos, C., Risso, W., dos Reis Martinez, C. (2018b). Triple-mixture of Zn, Mn, and Fe increases bioaccumulation and causes oxidative stress in freshwater neotropical fish. Environmental Toxicology and Chemistry, 37(6), 1749–1756.

    Google Scholar 

  • Dragovic, S., Mihailovic, N., Gajic, B. (2008). Heavy metals in soils: distribution, relationship with soil characteristics and radionuclides and multivariate assessment of contamination sources. Chemosphere, 72(3), 491–495.

    CAS  Google Scholar 

  • Echeverria, J., Morera, M., Mazkiaran, C., Garrido, J. (1998). Competitive sorption of heavy metal by soils. isotherms and fractional factorial experiments. Environmental Pollution, 101(2), 275–284.

    CAS  Google Scholar 

  • Eckert, D., & Sims, J. (1995). Recommended soil pH and lime requirement tests. Recommended soil testing procedures for the northeastern United States. Northeast Regional Bulletin, 493, 11–16.

    Google Scholar 

  • Embrapa. (1997). Handbook for methods of soil chemical analyses, 2nd edn. Rio de Janeiro: The Brazilian Company for Agricultural Research, National Center of Soil Research.

    Google Scholar 

  • Essington, M. (2015). Soil and water chemistry, 2nd edn. New York: CRC press.

    Google Scholar 

  • Fiol, N., & Villaescusa, I. (2009). Determination of sorbent point zero charge: usefulness in sorption studies. environmental Chemistry Letters, 7(1), 79–84.

    CAS  Google Scholar 

  • Gagnon, C., Arnac, M., Brindle, J.R. (1992). Sorption interactions between trace metals (Cd and Ni) and phenolic substances on suspended clay minerals. Water Research, 26(8), 1067–1072.

    CAS  Google Scholar 

  • Galunin, E., Ferreti, J., Zapelini, I., Vieira, I., Tarley, C., Abrao, T., Santos, M. (2014). Cadmium mobility in sediments and soils from a coal mining area on Tibagi River watershed: Environmental risk assessment. Journal of Hazardous Materials, 265, 280–287.

    CAS  Google Scholar 

  • Gernet, M., Melo, V., Dieckow, J., Lima, V., Silva, W. (2014). Genesis and occupancy of a shell midden on Paraná State coast. Brazilian Quaternary International, 352, 135–146.

    Google Scholar 

  • Hu, N., Liu, J., Huang, P., Yan, S., Shi, X., Ma, D. (2017). Sources, geochemical speciation, and risk assessment of metals in coastal sediments: a case study in the Bohai Sea, China. Environmental Earth Sciences, 76(8), 309.

    Google Scholar 

  • Kabata-Pendias, A. (2010). Trace elements in soils and plants, 4th edn. New York: CRC Press.

    Google Scholar 

  • Landis, W., & Yu, M. (2003). Introduction to environmental toxicology: impacts of chemicals upon ecological systems, 3rd edn. USA: Lewis Publisher.

    Google Scholar 

  • Li, Z., Ma, Z., van der Kuijp, T., Yuan, Z., Huang, L. (2014). A review of soil heavy metal pollution from mines in China: pollution and health risk assessment. Science of the Total Environment, 468, 843–853.

    Google Scholar 

  • Li, N., Tian, Y., Zhang, J., Zuo, W., Zhan, W., Zhang, J. (2017). Heavy metal contamination status and source apportionment in sediments of Songhua River Harbin region, Northeast China. Environmental Science and Pollution Research, 24(4), 3214–3225.

    CAS  Google Scholar 

  • Liao, J., Wen, Z., Ru, X., Chen, J., Wu, H., Wei, C. (2016). Distribution and migration of heavy metals in soil and crops affected by acid mine drainage: public health implications in Guangdong Province, China. Ecotoxicity and Environmental Safety, 124, 460–469.

    CAS  Google Scholar 

  • Liu, W., Wang, T., Borthwick, A., Wang, Y., Yin, X., Li, X., Ni, J. (2013). Adsorption of Pb2+, Cd2+, Cu2+ and Cr3+ onto titanate nanotubes: competition and effect of inorganic ions. Science of Total Environment, 456, 171–180.

    Google Scholar 

  • Lu, S., Wang, Y., Teng, Y., Yu, X. (2015). Heavy metal pollution and ecological risk assessment of the paddy soils near a zinc-lead mining area in Hunan. Environmental monitoring and assessment, 187 (10), 627.

    Google Scholar 

  • May, P., & Bulman, R. (1983). The present status of chelating agents in medicine. Progress in Medicinal Chemistry, 20, 225–336.

    CAS  Google Scholar 

  • McComb, J., Rogers, C., Han, F., Tchounwou, P. (2014). Rapid screening of heavy metals and trace elements in environmental samples using portable X-ray fluorescence spectrometer: a comparative study. Water, Air, & Soil Pollution, 225(12), 2169.

    Google Scholar 

  • Melquiades, F., & Appoloni, C. (2004). Application of XRF and field portable XRF for environmental analysis. Journal of radioanalytical and nuclear chemistry, 262(2), 533–541.

    CAS  Google Scholar 

  • Melquiades, F., Parreira, P., Appoloni, C., Silva, W., Lopes, F. (2011). Quantification of metals in river water using a portable EDXRF system. Applied Radiation and Isotopes, 69(2), 327–333.

    CAS  Google Scholar 

  • Ming, H., Naidu, R., Sarkar, B., Lamb, D., Liu, Y., Megharaj, M., Sparks, D. (2016). Competitive sorption of cadmium and zinc in contrasting soils. Geoderma, 268, 60–68.

    CAS  Google Scholar 

  • Mouni, L., Belkhiri, L., Bouzaza, A., Bollinger, J. (2017). Interactions between Cd, Cu, Pb, and Zn and four different mine soils. Arabian Journal of Geosciences, 10(4), 77.

    Google Scholar 

  • Nascimento, V., Almendros, G., Fernandes, F. (1992). Soil humus characteristics in virgin and cleared areas of the Paraná River basin in Brazil. Geoderma, 54(1), 137–150.

    CAS  Google Scholar 

  • Pansu, M., & Gautheyrou, J. (2007). Handbook of soil analysis: mineralogical, organic and inorganic methods. Springer Science & Business Media.

  • Pareja-Carrera, J., Mateo, R., Rodríguez-estival, J. (2014). Lead (Pb) in sheep exposed to mining pollution: implications for animal and human health. Ecotoxicology and environmental safety, 108, 210–216.

    CAS  Google Scholar 

  • Park, J., Ok, Y., Kim, S., Cho, J., Heo, J., Delaune, R., Seo, D. (2016). Competitive adsorption of heavy metals onto sesame straw biochar in aqueous solutions. Chemosphere, 142, 77–83. Biochars multifunctional role as a novel technology in the agricultural, environmental, and industrial sectors.

    CAS  Google Scholar 

  • Pérez-Serradilla, J., & de Castro, M. (2007). Integrated sorption-energy-dispersive X-ray fluorescence detection for automatic determination of lead and cadmium in low-concentration solutions. Analytical and bioanalytical chemistry, 389(5), 1541–1547.

    Google Scholar 

  • Santos, M.J. (2018). Dataset: metal mobilization factor modeling. Mendeley Data Set. Available at http://data.mendeley.com/datasets/kmpv8s7nbk/1.

  • Santos, M., Tarley, C., Cunha, I., Zapelini, I., Galunin, E., Bleinroth, D., Vieira, I., Abrao, T. (2015). Leachability of major and minor elements from soils and sediments of an abandoned coal mining area in southern Brazil. Environmental Monitoring and Assessment, 187(3), 83.

    Google Scholar 

  • Sarkar, D. (2005). Physical and chemical methods in soil analysis. New Age International.

  • Selim, H. (2012). Competitive sorption and transport of heavy metals in soils and geological media. CRC Press.

  • Seo, D., Yu, K., DeLaune, R. (2008). Comparison of monometal and multimetal adsorption in Mississippi River alluvial wetland sediment: batch and column experiments. Chemosphere, 73(11), 1757–1764.

    CAS  Google Scholar 

  • Serrano, S., O Day, P., Vlassopoulos, D., García-gonzález, M., Garrido, F. (2009). A surface complexation and ion exchange model of Pb and Cd competitive sorption on natural soils. Geochimica et Cosmochimica Acta, 73(3), 543–558.

    CAS  Google Scholar 

  • Silbergeld, E.K., Waalkes, M., Rice, J.M. (2000). Lead as a carcinogen: experimental evidence and mechanisms of action. American Journal Industrial Medicine, 38(3), 316–323.

    CAS  Google Scholar 

  • Silva, L., de Vallejuelo, S., Martinez-Arkarazo, I., Castro, K., Oliveira, M., Sampaio, C., de Brum, I., De leao, F., Taffarel, S., Madariaga, J. (2013). Study of environmental pollution and mineralogical characterization of sediment rivers from Brazilian coal mining acid drainage. Science of the total environment, 447, 169–178.

    CAS  Google Scholar 

  • Simate, G., & Ndlovu, S. (2014). Acid mine drainage: challenges and opportunities. Journal of Environmental Chemical Engineering, 2(3), 1785–1803.

    CAS  Google Scholar 

  • Tagami, K., Twining, J.R., Wasserman, M. (2012). Tropical radioecology, chapter Terrestrial radioecology in tropical systems, (pp. 155–230). Amsterdam: Elsevier.

    Google Scholar 

  • Tan, K. (2010). Principles of soil chemistry. Boca Raton: CRC press.

    Google Scholar 

  • Tansel, B., & Dizge, N. (2011). Competitive effects and interactions during sorption of SMP fractions on activated carbon: response surface approach for visualization of sorption profiles. Journal of Environmental Management, 92, 596– 602.

    CAS  Google Scholar 

  • USDA. (2017a). Soil Survey Manual. Soil Science Division Staff, 4th edn. Washington: United States Department of Agriculture. Handbook No. 18.

    Google Scholar 

  • USDA. (2017b). Soil Texture Calculator. Natural Resources Conservation Service Soils. United States Department of Agriculture.

  • Verma, H. (2007). Atomic and nuclear analytical methods: XRF, mössbauer, XPS, NAA and B63Ion-Beamspectroscopic Techniques. Berlin: Springer.

    Google Scholar 

  • Vidal, M., Santos, M., Abrao, T., Rodríguez, J., Rigol, A. (2009). Modeling competitive metal sorption in a mineral soil. Geoderma, 149(3), 189–198.

    CAS  Google Scholar 

  • Waalkes, M. (2003). Review cadmium carcinogenesis. Mutation Research, 533, 107–120.

    CAS  Google Scholar 

  • Witek-Krowiak, A., Chojnacka, K., Podstawczyk, D., Dawiec, A., Pokomeda, K. (2014). Application of response surface methodology and artificial neural network methods in modelling and optimization of biosorption process. Bioresource Technology, 160, 150–160.

    CAS  Google Scholar 

  • Wuana, R.A., & Okieimen, F. (2011). Heavy metals in contaminated soils: a review of sources, chemistry, risks and best available strategies for remediation. Isrn Ecology.

  • Yu, M., Tsunoda, H., Tsunoda, M. (2016). Environmental toxicology biological and health effects of pollutants, 3rd edn. Routledge: Taylor & Francis Group.

    Google Scholar 

  • Zhao, H., Xia, B., Fan, C., Zhao, P., Shen, S. (2012). Human health risk from soil heavy metal contamination under different land uses near Dabaoshan Mine, Southern China. Science of the Total Environment, 417, 45–54.

    Google Scholar 

  • Zuluaga Rodríguez, J., Gallego Rios, S., Ramírez Botero, C. (2015). Content of Hg, Cd, Pb and As in fish species: a review. Vitae, 22(2), 148–149.

    Google Scholar 

Download references

Acknowledgments

The authors would like to thank prof. A. Urbano from Physics Department, Universidade Estadual de Londrina, for the insightful discussions on the X-ray diffraction.

Funding

This study received financial support and fellowships from the Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq, Brazil), under Grants 309927/2015-3 and 304066/2015-0 (Researcher grant), Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (Capes), and Fundação Araucária (FAP-FA, Brazil) under Grant 507/2014 (Researcher grant).

Author information

Authors and Affiliations

  1. Chemistry Department, Universidade Estadual de Londrina, Rod. Celso Garcia Cid-PR445, Londrina, Parana, 86051-990, Brazil

    Emilli Frachini, Leonel Vinicius Constantino & Maria Josefa Santos

  2. Electrical Engineering Department, Universidade Estadual de Londrina, Rod. Celso Garcia Cid-PR445, Londrina, Parana, 86051-990, Brazil

    Taufik Abrao

Authors
  1. Emilli Frachini
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Leonel Vinicius Constantino
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Taufik Abrao
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Maria Josefa Santos
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Maria Josefa Santos.

Ethics declarations

Conflict of interest

The authors declare that they have no conflict of interest.

Additional information

Publisher’s note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Highlights

1. Competitive sorption by applying factorial design and EDXRF was evaluated;

2. 3-D surface model indicates Cd2+ and Pb2+ synergistic effect on Hg2+ mobilization;

3. EDXRF analysis indicated high Pb2+ mobilization through the basin;

4. Innovative mobilization factor determined from the fluorescence peaks integration;

5. Even with specific interactions, Hg2+ ions were mobilized.

Electronic supplementary material

Below is the link to the electronic supplementary material.

(PDF 1.00 MB)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Frachini, E., Constantino, L.V., Abrao, T. et al. A new approach to evaluate toxic metal transport in a catchment. Environ Monit Assess 192, 234 (2020). https://doi.org/10.1007/s10661-019-7950-x

Download citation

  • Received:

  • Accepted:

  • Published:

  • DOI: https://doi.org/10.1007/s10661-019-7950-x

Keywords

Search

Navigation