Elsevier

Atmospheric Research

Volume 238, 1 July 2020, 104878
Atmospheric Research

2009–2017 trends of PM10 in the legendary Riotinto mining district of SW Spain

https://doi.org/10.1016/j.atmosres.2020.104878Get rights and content

Highlights

  • Geochemical of sulphide related elements in PM10 has been studied in open pit mine.

  • High concentrations have been detected during the reopening of the mine.

  • Mining source using PMF increase during the activity period of the mine.

  • The efficacy of implementation of best abatement technologies has been corroborated.

Abstract

This study is the first to perform a chemical characterization and source contribution of particulate matter (PM10) occurring through the abandonment and reopening of a historical sulphide mine. This long-range analysis covers the period 2009–2017 in the Riotinto mining district (Iberian Pyrite Belt, Southwestern Spain), which is a mining district of world-class importance. This mine represents a susceptible anthropogenic emission source of toxic sulphide-associated elements in atmospheric particulate matter, which affects the air quality of the nearby areas. A total of 567 samples of 24 h were collected from 2009 to 2017 in a rural station. The filters were analysed to determine Organic and elemental carbon, mayor and trace elements, and water soluble compounds of PM10.

The trends of PM10 and geochemical characterization were studied considering the following periods: mine abandonment (2009–2014) and the mine's state during (2015–2016) and after (2017) implementation of new emission abatement technology at this mine. The results revealed relatively high concentrations of Cu, Zn, Pb, As, Sb, and Bi during 2015–2016. A reduction of 42–59% was observed after 2017 for the same elements in PM10. Five sources were identified: regional, mining, aged sea salt, combustion + traffic and crustal, using positive matrix factorization model (PMF5). The contribution of the mining factor was higher in the reopening period (4.2 μg m−3, 16%). These results have been confirmed by As speciation analysis, in which the low extraction percentage obtained is related to the origin of the metalloids associated with sulphide ores.

The reduction of emissions of atmospheric particulate matter in the mining processes is the main objective in the implementation of measures considering the technological progress for cleaner and sustainable mining. In the case of reopening of historical mines, with low ore grade and greater extraction of ore and rock, a major effort must be made in order to avoid a negative influence on the environment and human health.

Introduction

Mining activity and mainly open pit operations are considered the major sources of particulate emission to atmosphere (Nriagu and Pacyna, 1988), highlighting the operations of exploitation, transport, abandonment of mining and waste accident in coal, and metallic and no metallic ore (Table S1). Fugitive atmospheric particles matter (APM) exert a considerable influence on the concentration, toxicity (Bell et al., 2001; Plumlee and Morman, 2011) and the human health (Magas et al., 2007; Wild et al., 2009; WHO, 2013; Patra et al., 2016) (Table S1). These APM inside open mine regions show high levels of heavy metals and metalloids (Tsai and Cheng, 2004; Park and Kim, 2005) that can be transported to near areas, which affects the quality of air and human health Recently, Csavina et al. (2012) considered the transport of heavy metals and metalloids by APM to be an important pathway for their redistribution in the environment. Hence, these pollutants can reach long distances before being finally deposited on the ground or inhaled (Rasmussen, 1998; Zota et al., 2009; Wai et al., 2016). However, studies on the dispersion of metals and metalloids in APM with mining activities are scarce, although the associated environmental and health risks are known (Brotons et al., 2010; Taylor et al., 2010; Csavina et al., 2011, Table S1).

Mining of Cu resources are taking high relevance in the current world due to the depletion of mineral resources and economic growth (Valenta et al., 2019). The reopening of metallic historical mining with low ore grade implies a greater extraction, movement and treatment of ore and rock (Lagos et al., 2018), and in consequence, a negative influence on the environment (Valenta et al., 2019).

In the last decade, in the Iberian Pyrite Belt (SW Iberian Peninsula), a resurgence of metallic mining has occurred owing to increases in prices, especially for Cu, which favours the opening of new mines (e.g. Cobre las Cruces Mine) or reopening of other legendary ones such as the Riotinto mining district. The process of reopening has been undertaken by Atalaya mining project in 2015.

Relevant geochemical anomalies of APM related to mining processes in Las Cruces Mine, Seville province, has been interpreted in Sánchez de la Campa et al. (2015). They found higher concentrations of Cu and As than those in other urban and rural Spanish areas in which high concentrations of As, Se, Bi, Cd, and Pb have been described. However, arsenic speciation studies in PM10 have established differences in its contribution, in which the average extraction efficiency of As in PM10 samples depends on the origin of the APM. The toxicity of As is dependent on its chemical form, oxidation state, and physical state of gas versus in solution (Pershagen et al., 1982; Viraraghavan et al., 1992).

In Riotinto, past mining, mineral processing, and smelting industries have generated great amounts of hazardous mining residues from its exploitation since pre-Roman times. Recently, the levels and chemical compositions of PM10 (particles with aerodynamic diameter below or equal to 10 μm) and depositional particles in this area have been defined by Sánchez de la Campa et al. (2011) and Castillo et al. (2013), respectively.

In this work, we study a chemical characterization and source contribution of PM10 occurring through the abandonment and reopening of the Riotinto historical mine, one of the more important open pit Cu mines of Europe. Our study focuses on the trend evolution of PM10 and sulphide-associated elements concentrations regarding the monitoring of fugitive emission implemented at a Cu mine in the Riotinto mining district, SW Spain. The concentration of tracer elements such as As, Pb, and Zn occurring through mining activity has been determined in PM10 during the period 2009–2017 in Nerva town, a rural zone located near the open pit. For trend analyses, three periods have been distinguished: mine abandonment (2009–2014) and during (2015–2016) and after (2017) the implementation of emission abatement technology at the Cu mine. The As speciation analysis as well as the extraction percentage obtained will permit to know the origin of As associated to PM10. The reduction of emissions of APM in the mining processes is a main objective in the application of measures considering the technological progress for cleaner and sustainable mining.

Section snippets

The study area

The Riotinto mining district is one of the world's principal sulphide geochemical anomalies (Fig. 1) (Leistel et al., 1998). This region is of great historic interest and is considered as one of the largest volcanogenic massive sulphide outcrops worldwide, which has been exploited dating back to pre-Roman times (Davis Jr. et al., 2000). Its intense activity has been reflected in the notable environmental degradation of the area (Galán et al., 2003; Lottermoser, 2010). Mining operation in this

Results and discussion

The mean concentrations and chemical composition of PM10 from 2009 to 2017 are shown in Table 1 considering the three periods established in this study: prior to abandonment and during and after the implementation of emission abatement technology. To describe and evaluate the statistically significant trends of all periods, the long-terms trend of PM10 and its components were assessed by using the Theil–Sen approach (Table 1).

Conclusions

Geochemical anomalies in toxic sulphide-associated elements in PM10 have been identified in the case of the historical Riotinto mine (Iberian Pyrite Belt, Spain) during 2009–2017. In the abandoned mine period (2009–2014), low concentrations of sulphide-associated elements and PM10 were found (Cu: 6.1 ng m−3, Zn: 23.2 ng m−3, Pb: 4.8 ng m−3 and As: 1.1 ng m−3) compared to the reopening period, mainly in 2016 (Cu: 25.3 ng m−3, Zn: 49.1 ng m−3, Pb: 11.5 ng m−3 and As: 4.5 ng m−3). In the periods

Declaration of Competing Interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgments

The authors are grateful to various public administrations for financial support: Department of the Environment (project 10/2013/PC/00) and Department of Innovation, Science and Enterprise (project 2009-RNM 5163M and 2011 RNM 7800) of the Autonomous Government of Andalusia and Project CGL2008-06270-C02/CLI of the Spanish Educational Ministry. In addition, the environmental technicians at Atalaya Mining and Nerva Town Hall are thanked for providing assistance with the sampling.

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