Contribution of mine wastes to atmospheric metal deposition in the surrounding area of an abandoned heavily polluted mining district (Rio Tinto mines, Spain) Sonia Castillo a, ⁎, Jesús D. de la Rosa a, b , Ana M. Sánchez de la Campa a , Yolanda González-Castanedo a , Juan C. Fernández-Caliani a, b , Isabel Gonzalez c , Antonio Romero c a Associate Unit CSIC-University of Huelva “Atmospheric Pollution”, Centre for Research in Sustainable Chemistry (CIQSO), Campus of Excellence CeiA3, University of Huelva, E27071 Huelva, Spain b Department of Geology, Faculty of Experimental Sciences, University of Huelva, E21071 Huelva, Spain c Department of Crystallography, Mineralogy and Agricultural Chemistry, Faculty of Chemistry, University of Seville, 41071 Seville, Spain HIGHLIGHTS ► Metal dust appears in areas exposed to dust-bearing winds flowing from Rio Tinto mine. ► PM deposited is characterized by enrichment in potentially toxic metals/metalloids. ► Mine waste source made up of elements such as Cu, Zn, As, Sb, Ba, Pb, Sn, Cd and Bi. ► A decrease in deposition fluxes is observed as we move away from the waste deposits. ► Particle grain segregation is observed during metal dust transport from mine waste. abstract article info Article history: Received 20 October 2012 Received in revised form 24 January 2013 Accepted 25 January 2013 Available online 26 February 2013 Keywords: Atmospheric deposition Mine wastes Metals Insoluble fraction Soluble fraction Rio Tinto mines The present study seeks to estimate the impact of abandoned mine wastes on the levels and chemical profile of total atmospheric deposition in one of the oldest and largest mining districts in Europe (Rio Tinto mines, Iberian Pyrite Belt), on the basis of a complete geochemical characterization of particulate matter samples periodically collected in five sampling stations located around the mining district between March 2009 and February 2011. The annual levels of total bulk deposition (soluble and insoluble fractions) registered in the Rio Tinto Mining District ranged between 18 and 43 g/m 2 depending on the distance from the sampling station with regard to the mine waste deposits. As a general pattern in the area, high mass levels of Zn and Cu were deposited in a range of 9–62 mg/m 2 not only in the insoluble but also in the soluble fraction. Other potentially toxic trace elements such as As, Sb, Ba, Pb, Sn and Bi showed greater deposition fluxes in the locations closest to the mine waste deposits. A principal component analysis with a Multilinear Regression Analysis certifies the presence of two common sources in the mining area: 1) a mineral factor composed mainly of elements derived from silicate minerals (Al, Ca, Sr, Ti, Li, Mg, Mn, K, Na and Fe), mixed with other anthropogenic species (NH 4 + , SO 4 2- , NO 3 - ) within the village closest to the mine; and 2) a marine factor composed of Na, Cl, Mg, SO 4 2- and Sr. In addition, a mine waste factor made up of toxic elements (Cu, Zn, Ga, As, Sb, Ba, Pb, Sn, Cd and Bi) has been recognized in the sampling sites exposed to dust-bearing winds downwind of the mining area, suggesting that mine wastes are a relevant source of heavy-mineral particles with potentially adverse environmental effects to sur- rounding soils, plants and humans. © 2013 Elsevier B.V. All rights reserved. 1. Introduction In ancient mining districts with long histories of mining and met- allurgical activity, mine wastes represent one of the main sources of pollution to soils, water, air and biota (Hudson-Edwards et al., 2011; Csavina et al., 2011, 2012). Oxidation of sulphide minerals in mine wastes (Nordstrom, 2011) generates acid water loaded with dissolved iron, sulphates and potentially toxic elements (As, Se, Cu, Zn, Cd, Hg, and more), which are discharged into proximal fluvial and estuarine systems adversely affecting water and soil quality (Galán et al., 2003). However, this is not the only possible cause of water and soil contami- nation. The atmospheric dispersion of particulate matter (PM) by air is also a significant contributor of contaminants to the environment. Particle resuspension from open-cast mining, metallurgical activities Science of the Total Environment 449 (2013) 363–372 ⁎ Corresponding author. Tel.: +34 959219821. E-mail address: sonia.castle@gmail.com (S. Castillo). 0048-9697/$ – see front matter © 2013 Elsevier B.V. All rights reserved. http://dx.doi.org/10.1016/j.scitotenv.2013.01.076 Contents lists available at SciVerse ScienceDirect Science of the Total Environment journal homepage: www.elsevier.com/locate/scitotenv