Skip to main content
SpringerLink
Log in

Arsenic release from pyrite ash waste over an active hydrogeological system and its effects on water quality

  • Research Article
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

Arsenic is a potentially toxic element of concern for environmental compartments, and it is a frequent pollutant in many abandoned industrial sites. In this study, geochemical and hydrogeological tools were used to determine the long-term effects of As-rich pyrite ash disposal (83,000 m3 as estimated by geostatistical tools) in a brownfield located over a quaternary alluvial aquifer. Throughout the site, soil pollution and water table oscillation led to leachates in the form of both run-off and infiltration waters, thereby reducing (ground)water quality (e.g. pH, electrical conductivity) and, in particular, increasing the concentration of arsenic (average approx. 4000 μg/l for one hydrological year). By means of laboratory and in situ measurements, the main mechanisms through which the sulphide remaining in the pyrite ash leaches were identified. In addition, to evaluate the effects of the polluted groundwater on the nearby main river, a mathematical approach using the Domenico analytical groundwater transport model revealed potential concentrations of 49 μg/l of arsenic in the junction between the study aquifer and the river, equivalent to an annual quantity of 49 kg of this element.

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
Fig. 6
Fig. 7
Fig. 8

Similar content being viewed by others

Abbreviations

EC:

Electrical conductivity

ICP-MS:

Inductively coupled plasma mass spectrometry

IDA:

Isotopic dilution analysis

TCLP:

Toxicity characteristic leaching procedure

DEM:

Digital elevation model

IDW:

Inverse distance weighted

RBCA:

Risk base correction action

SI:

Saturation index

References

  • Abadi M, Zamani A, Parizanganeh A, Khosravi Y, Badiee H (2018) Heavy metals and arsenic content in water along the southern Caspian coasts in Iran. Environ Sci Pollut Res 25:23725–23735. https://doi.org/10.1007/s11356-018-2455-7

    Article  CAS  Google Scholar 

  • Ahmaruzzaman M (2011) Industrial wastes as low-cost potential adsorbents for the treatment of wastewater laden with heavy metals. Adv Colloid Interf Sci 166:36–59

    Article  CAS  Google Scholar 

  • Aide M, Beighley D, Dunn D (2016) Arsenic in the soil environment: a soil chemistry review. Int J Appl Agric Res 11:1–28

    Article  Google Scholar 

  • Alekseenko VA, Bech J, Alekseenko AV, Shvydkaya NV, Roca N (2018) Environmental impact of disposal of coal mining wastes on soils and plants in Rostov Oblast, Russia. J Geochem Explor 184:261–270. https://doi.org/10.1016/j.gexplo.2017.06.003

    Article  CAS  Google Scholar 

  • Álvarez-Ayuso E, Abad-Valle P, Murciego A, Villar-Alonso P (2016) Arsenic distribution in soils and rye plants of a cropland located in an abandoned mining area. Sci Total Environ 542:238–246. https://doi.org/10.1016/j.scitotenv.2015.10.054

    Article  CAS  Google Scholar 

  • Boente C, Sierra C, Rodríguez-Valdés E, Menéndez-Aguado JM, Gallego JR (2017) Soil washing optimization by means of attributive analysis: case study for the removal of potentially toxic elements from soil contaminated with pyrite ash. J Clean Prod 142:2693–2699. https://doi.org/10.1016/j.jclepro.2016.11.007

    Article  CAS  Google Scholar 

  • Boente C, Albuquerque MTD, Fernández-Braña A, Gerassis S, Sierra C, Gallego JR (2018) Combining raw and compositional data to determine the spatial patterns of potentially toxic elements in soils. Sci Total Environ 631–632:1117–1126. https://doi.org/10.1016/j.scitotenv.2018.03.048

    Article  CAS  Google Scholar 

  • Botey R, Guijarro JA, Jiménez A (2013) Valores Normales de Precipitación Mensual 1981- 2010. Ministerio de Agricultura, Alimentación y Medio Ambiente-Agencia Estatal de Meteorología. http://www.aemet.es/es/conocermas/recursos_en_linea/publicaciones_y_estudios/publicaciones/detalles/Valores_mensuales_1981_2010. Accessed September 2019

  • de Meyer CMC, Rodríguez JM, Carpio EA, García PA, Stengel C, Berg M (2017) Arsenic, manganese and aluminum contamination in groundwater resources of Western Amazonia (Peru). Sci Total Environ 607–608:1437–1450. https://doi.org/10.1016/j.scitotenv.2017.07.059

    Article  CAS  Google Scholar 

  • Domenico PA (1987) An analytical model for multidimensional transport of a decaying contaminant species. J Hydrol 91(1-2):49–58. https://doi.org/10.1016/0022-1694(87)90127-2

    Article  CAS  Google Scholar 

  • Drahota P, Knappová M, Kindlová H, Culka A, Majzlan J, Mihaljevič M, Rohovec J, Veselovský F, Fridrichová M, Jehlička J (2016) Mobility and attenuation of arsenic in sulfide-rich mining wastes from the Czech Republic. Sci Total Environ 557–558:192–203. https://doi.org/10.1016/j.scitotenv.2016.03.079

    Article  CAS  Google Scholar 

  • Evangelou VP (2012) Pyrite chemistry: the key for abatement of acid mine drainage. Acidic Mining Lakes:197–222

  • Falta RW (2008) Methodology for comparing source and plume remediation alternatives. Ground Water 46:272–285. https://doi.org/10.1111/j.1745-6584.2007.00416.x

    Article  CAS  Google Scholar 

  • Fedje KK, Sierra C, Gallego JR (2017) Enhanced soil washing for the remediation of a brownfield polluted by pyrite ash. Soil Sediment Contam 26:377–390. https://doi.org/10.1080/15320383.2017.1319335

    Article  CAS  Google Scholar 

  • Flaková R, Ženišová Z, Krčmár D et al (2017) Occurrence of antimony and arsenic at mining sites in Slovakia: implications for their mobility. Carpathian J Earth Environ Sci 12(1):41–48

    Google Scholar 

  • Gallego JR, Esquinas N, Rodríguez-Valdés E, Menéndez-Aguado JM, Sierra C (2015) Comprehensive waste characterization and organic pollution co-occurrence in a Hg and As mining and metallurgy brownfield. J Hazard Mater 300:561–571. https://doi.org/10.1016/j.jhazmat.2015.07.029

    Article  CAS  Google Scholar 

  • Gallego JR, Rodríguez-Valdés E, Esquinas N, Fernández-Braña A, Afif E (2016) Insights into a 20-ha multi-contaminated brownfield megasite: an environmental forensics approach. Sci Total Environ 563–564:683–692. https://doi.org/10.1016/j.scitotenv.2015.09.153

    Article  CAS  Google Scholar 

  • Gan M, Deng Q, Shen G, Fan X, Wen H, Chen X (2013) Research on the lead removal from pyrity cinder. In: 4th International Symposium on High-Temperature Metallurgical Processing. pp 587–593

  • González-Fernández B, Rodríguez-Valdés E, Boente C, Menéndez-Casares E, Fernández-Braña A, Gallego JR (2018) Long-term ongoing impact of arsenic contamination on the environmental compartments of a former mining-metallurgy area. Sci Total Environ 610–611:820–830. https://doi.org/10.1016/j.scitotenv.2017.08.135

    Article  CAS  Google Scholar 

  • Gutiérrez-Claverol M, Luque-Cabal C (1995) Geología de Asturias. Trea SL. Recur. Geológicos, Gijón, pp 187–202

    Google Scholar 

  • Hageman PL, Seal RR, Diehl SF, Piatak NM, Lowers HA (2015) Evaluation of selected static methods used to estimate element mobility, acid-generating and acid-neutralizing potentials associated with geologically diverse mining wastes. Appl Geochem 57:125–139. https://doi.org/10.1016/j.apgeochem.2014.12.007

    Article  CAS  Google Scholar 

  • Jiménez A, Prieto M, Salvadó MA, García-Grand S (2004) Structure and crystallization behavior of the (Ba, Sr) HAsO4· H2O solid-solution in aqueous environments. Am Mineral 89(4):601–609

    Article  Google Scholar 

  • Lara-Gonzalo A, Kruge MA, Lores I, Gutiérrez B, Gallego JR (2015) Pyrolysis GC-MS for the rapid environmental forensic screening of contaminated brownfield soil. Org Geochem 87:9–20. https://doi.org/10.1016/j.orggeochem.2015.06.012

    Article  CAS  Google Scholar 

  • Li W, Zhang M, Wang M, Han Z, Liu J, Chen Z, Liu B, Yan Y, Liu Z (2018) Screening of groundwater remedial alternatives for brownfield sites: a comprehensive method integrated MCDA with numerical simulation. Environ Sci Pollut Res 25:15844–15861. https://doi.org/10.1007/s11356-018-1721-z

    Article  Google Scholar 

  • Lopez-Arce P, Garcia-Guinea J, Garrido F (2017) Chemistry and phase evolution during roasting of toxic thallium-bearing pyrite. Chemosphere 181:447–460. https://doi.org/10.1016/j.chemosphere.2017.04.109

    Article  CAS  Google Scholar 

  • Lu H, Yu S (2019) Pollutant source analysis and tempo-spatial analysis of pollutant discharge intensity in a transboundary river basin. Environ Sci Pollut Res 26:1336–1354. https://doi.org/10.1007/s11356-018-3574-x

    Article  Google Scholar 

  • Martínez-Santos P, Martínez-Alfaro PE, Sanz E, Galindo A (2010) Daily scale modelling of aquifer–river connectivity in the urban alluvial aquifer in Langreo, Spain. Hydrogeol J 18:1525–1537. https://doi.org/10.1007/s10040-010-0613-1

    Article  Google Scholar 

  • Mesa V, Gallego JLR, González-Gil R, Lauga B, Sánchez J, Méndez-García C, Peláez AI (2017) Bacterial, Archaeal, and Eukaryotic Diversity across Distinct Microhabitats in an Acid Mine Drainage. Frontiers in Microbiology 8

  • Ministerie van Volkshuisvesting (2000) Circular on target values and intervention values for soil remediation - Dutch Target and Intervention Values. Netherlands Goverment Gazette

  • Olías M, Cánovas CR, Basallote MD, Macías F, Pérez-López R, González RM, Millán-Becerro R, Nieto JM (2019) Causes and impacts of a mine water spill from an acidic pit lake (Iberian Pyrite Belt). Environ Pollut 250:127–136. https://doi.org/10.1016/j.envpol.2019.04.011

    Article  CAS  Google Scholar 

  • Oliveira MLS, Ward CR, Izquierdo M, Sampaio CH, de Brum IAS, Kautzmann RM, Sabedot S, Querol X, Silva LFO (2012) Chemical composition and minerals in pyrite ash of an abandoned sulphuric acid production plant. Sci Total Environ 430:34–47. https://doi.org/10.1016/j.scitotenv.2012.04.046

    Article  CAS  Google Scholar 

  • O'Reilly SE, Strawn DG, Sparks DL (2001) Residence time effects on arsenate adsorption/desorption mechanisms on goethite. Soil Sci Soc Am J 65(1):67–77

    Article  CAS  Google Scholar 

  • Otaegi N, Cagigal E (2017) NanoRem pilot site – Nitrastur, Spain: remediation of arsenic in groundwater using nanoscale zero-valent iron. NanoRem Bull 12

  • Parkhurst DL, Appelo CA (1999) User’s guide to PHREEQC (version 2) - a computer program for speciation, batch-reaction, one-dimensional transport and inverse geochemical calculations; U.S. Geological Survey Water Resources Investigations Report 99-4259, U.S. Geological Survey, 310 pp. Washington, DC

  • Pigna M, Krishnamurti GSR, Violante A (2006) Kinetics of arsenate sorption–desorption from metal oxides. Soil Sci Soc Am J 70(6):2017–2027

    Article  CAS  Google Scholar 

  • Plaza F, Wen Y, Liang X (2018) Acid rock drainage passive remediation using alkaline clay: Hydro-geochemical study and impacts of vegetation and sand on remediation. Sci Total Environ 637–638:1262–1278. https://doi.org/10.1016/j.scitotenv.2018.05.014

    Article  CAS  Google Scholar 

  • Rodríguez JD, Jiménez A, Prieto M, Torre L, García-Granda S (2008) Interaction of gypsum with As (V)-bearing aqueous solutions: surface precipitation of guerinite, sainfeldite, and Ca2NaH (AsO4) 2· 6H2O, a synthetic arsenate. Am Mineral 93(5-6):928–939

    Article  Google Scholar 

  • Sierra C, Gallego JR, Afif E, Menéndez-Aguado JM, González-Coto F (2010) Analysis of soil washing effectiveness to remediate a brownfield polluted with pyrite ashes. Journal of Hazardous Materials 180 (1–3):602–608

  • Smedley PL, Kinniburgh DG (2002) A review of the source, behaviour and distribution of arsenic in natural waters. Appl Geochem 17:517–568

    Article  CAS  Google Scholar 

  • Sun J, Tang C, Wu P (2013) Migration of Cu, Zn, Cd and As in epikarst water affected by acid mine drainage at a coalfield basin, Xingren, Southwest China. Environ Earth Sci 69:2623–2632. https://doi.org/10.1007/s12665-012-2083-3

    Article  CAS  Google Scholar 

  • UNE-EN 12457-4 (2003) Characterisation of waste - Leaching - Compliance test for leaching of granular waste materials and sludges - Part 4: One stage batch test at a liquid to solid ratio of 10 l/kg for materials with particle size below 10 mm (without or with size reduction).

  • USEPA, US Environmental Protection Agency (1992) Method 1311: toxicity characteristic leaching procedure. https://www.epa.gov/hw-sw846/sw-846-test-method-1311-toxicity-characteristic-leaching-procedure. Accessed October 2019

  • Wang Z, Guo H, Xiu W, Wang J, Shen M (2018) High arsenic groundwater in the Guide basin, northwestern China: distribution and genesis mechanisms. Sci Total Environ 640–641:194–206. https://doi.org/10.1016/j.scitotenv.2018.05.255

    Article  CAS  Google Scholar 

  • Wcisło E, Bronder J, Bubak A, Rodríguez-Valdés E, Gallego JR (2016) Human health risk assessment in restoring safe and productive use of abandoned contaminated sites. Environ Int 94:436–448. https://doi.org/10.1016/j.envint.2016.05.028

    Article  CAS  Google Scholar 

  • Wilkin RT, Lee TR, Beak DG, Anderson R, Burns B (2018) Groundwater co-contaminant behavior of arsenic and selenium at a lead and zinc smelting facility. Appl Geochem 89:255–264. https://doi.org/10.1016/j.apgeochem.2017.12.011

    Article  CAS  Google Scholar 

  • Yang C, Chen Y, Peng P, Li C, Chang X, Wu Y (2009) Trace element transformations and partitioning during the roasting of pyrite ores in the sulfuric acid industry. J Hazard Mater 167:835–845. https://doi.org/10.1016/j.jhazmat.2009.01.067

    Article  CAS  Google Scholar 

  • Yang Q, Li Z, Lu X, Duan Q, Huang L, Bi J (2018) A review of soil heavy metal pollution from industrial and agricultural regions in China: pollution and risk assessment. Sci Total Environ 642:690–700

    Article  CAS  Google Scholar 

  • Zhang D, Guo H, Xiu W, Ni P, Zheng H, Wei C (2017) In-situ movilization and transformation of iron-oxides-adsorbed arsenate in natural groundwater. J. Hazard Mater 321:228–237. https://doi.org/10.1016/j.jhazmat.2016.09.021

    Article  CAS  Google Scholar 

Download references

Funding

This work was partially supported by the project I+DARTS (LIFE11 ENV/ES/000547, EC). We would also like to thank the Environmental Assay Unit of the Scientific and Technical Services of the University of Oviedo for their support. Diego Baragaño and Carlos Boente obtained a grant from the “Formación del Profesorado Universitario” programme, financed by the “Ministerio de Educación, Cultura y Deporte de España”.

Author information

Authors and Affiliations

  1. INDUROT and Environmental Technology, Biotechnology and Geochemistry Group, C/Gonzalo Gutiérrez Quirós s/n, 33600, Mieres, Asturias, Spain

    Diego Baragaño, Carlos Boente, Eduardo Rodríguez-Valdés, Alicia Fernández-Braña & José Luis R. Gallego

  2. Departamento de Explotación y Prospección de Minas, Universidad de Oviedo, C/Independencia, 13, 33004, Oviedo, Asturias, Spain

    Beatriz González-Fernández

  3. Departamento de Geología, Universidad de Oviedo, C/ Jesús Arias de Velasco, s/n, 33005, Oviedo, Asturias, Spain

    Amalia Jiménez

Authors
  1. Diego Baragaño
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Carlos Boente
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Eduardo Rodríguez-Valdés
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Alicia Fernández-Braña
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Amalia Jiménez
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. José Luis R. Gallego
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Beatriz González-Fernández
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Beatriz González-Fernández.

Additional information

Responsible editor: Stuart Simpson

Publisher’s note

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

Electronic supplementary material

ESM 1

(DOCX 1746 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Baragaño, D., Boente, C., Rodríguez-Valdés, E. et al. Arsenic release from pyrite ash waste over an active hydrogeological system and its effects on water quality. Environ Sci Pollut Res 27, 10672–10684 (2020). https://doi.org/10.1007/s11356-019-07120-8

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-019-07120-8

Keywords

Search

Navigation