Evaluation of the Potential Risks of Heavy Metal Contamination in Rice Paddy Soils Around an Abandoned Hg Mine Area in Southwest China
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Acta Geochim (2020) 39(1):85–95 https://doi.org/10.1007/s11631-019-00364-8 ORIGINAL ARTICLE Evaluation of the potential risks of heavy metal contamination in rice paddy soils around an abandoned Hg mine area in Southwest China 1,2 1,2 1,2 3 Bayou Adlane • Zhidong Xu • Xiaohang Xu • Longchao Liang • 1,3 1 Jialiang Han • Guangle Qiu Received: 8 January 2019 / Revised: 12 June 2019 / Accepted: 12 July 2019 / Published online: 18 July 2019 Ó Science Press and Institute of Geochemistry, CAS and Springer-Verlag GmbH Germany, part of Springer Nature 2019 Abstract To assess the potential ecological and health Keywords Heavy metals Á Ecological risk index Á risks of trace elements (Hg, Cd, As, Mn, Sb, Pb, Cu, Ni, Cr, Wanshan Hg mining area and Zn), a total of 138 soil samples from rice paddies were collected during the rice harvest season in the Wanshan mining area, Guizhou Province, Southwest China. Factors 1 Introduction of the pollution load index (PLI), geo-accumulation index (I-Geo), enrichment factor (EF), and risk index (RI) were Mercury (Hg), characterized by its high toxicity, is known determined. High concentrations of Hg, Sb, As, Zn, Cd, to be a global pollutant that presents high exposure risk Cu, and Mn were observed in the soils. The PLI, I-Geo, and (Clarkson 1998; Schroeder and Munthe 1998; Lindqvist EF results all showed high levels of contamination by Hg et al. 1991). Due to the massive consumption of energy and and Sb and moderate levels of contamination by As, Pb, resources required by China’s rapid economic develop- Zn, Cu, Cd, and Mn. There was no significant contami- ment, many areas across the country have suffered from nation from Ni and Cr. The RI was very high, with Hg as environmental impacts caused by Hg. According to pre- the dominant pollutant, as expected, indicating that the liminary studies, more than 80% of the Hg emissions historical large-scale Hg mining, as well as artisanal min- released into the atmosphere have been caused by two main ing, has had a significant impact on the Wanshan area. sources: nonferrous metal smelting and coal combustion Moreover, coal combustion, manganese factories, and the (Wu et al. 2006; Li et al. 2012, 2015; Fan et al. 2017; Xu use of agrochemicals by the local population could also et al. 2016, 2017). Of the estimated 402 tons of atmo- have an impact on the soil through the introduction of spheric mercury emissions from China in 1995, coal heavy metal loads. To address the current state of con- combustion was estimated to contribute 145 tons, or 36.1% tamination, pollutant remediation and the regulation con- (Feng 2005). In 2000, the smelting of zinc, lead, and trol of the anthropogenic activities in Wanshan are urgently copper contributed an estimated 222.1 tons to the atmo- needed. spheric mercury emissions (Wu et al. 2006). The Wanshan Hg mining region in Guizhou Province was the largest Hg-producing region in China (Qiu et al. 2005). Approximately 22,000 tons of metal Hg and & Guangle Qiu 6000 tons of cinnabar were extracted from the Wanshan [email protected] mining area, resulting in large quantities of mine waste 1 (Liu 1998). Approximately 125.8 million tons of calcines State Key Laboratory of Environmental Geochemistry, 3 Institute of Geochemistry, Chinese Academy of Sciences, and 20.2 billion m of Hg-containing exhaust gas were Guiyang 550081, China released into the surrounding ecosystems of the Wanshan 2 University of Chinese Academy of Sciences, Beijing 100049, Hg mining region from 1949 to early 1990 (Liu 1998). China Because of the environmental strain caused by the massive 3 College of Resources and Environmental Engineering, mining production, the Wanshan Hg mine was closed in Guizhou University, Guiyang 550003, China 2004 under a national strategy to address environmental 123 86 Acta Geochim (2020) 39(1):85–95 issues. Severe Hg contamination has occurred in several 2 Materials and methods environmental compartments of Wanshan including rivers, sediments, soil, vegetation, and the atmosphere (Feng et al. 2.1 Study area 2003; Feng and Qiu 2008; Qiu et al. 2005, 2009; Li et al. 2008; Xu et al. 2019). Rice is the main food staple of the The Wanshan district (27.518022°N, 109.213663°E) is local population, and human health exposure to located in the eastern part of Guizhou Province, South- methylmercury (MeHg) through rice consumption has also western China. The study area covers 169.47 km2, been documented (Feng et al. 2008). including Wanshan town, Aozhai ethnic town, and Xiaxi Cinnabar ore, often associated with other toxic elements ethnic town (Fig. 1). such as antimony (Sb), arsenic (As), copper (Cu), man- The study area is a typical mountainous karst terrain ganese (Mn), zinc (Zn), and lead (Pb), can also be released with an elevation ranging from 205 to 1150 m a.s.l. It is into surrounding areas during the activities of ore pro- characterized by a subtropical humid climate with abun- cessing and retorting. In addition to the mining industry, dant precipitation (1200–1400 mm year-1) and mild tem- agricultural activities also contribute to the trace presence peratures (* 17 °C). The major rivers, the Xiaxi and of these metals. The long-term use of land accompanied by Aozhai rivers, drain the Wanshan catchment (WSC) with the frequent application of agrichemicals can lead to the their headwaters, and both rivers originate from Hg mining accumulation of various trace metals, such as Cu, Zn, sites (Fig. 1). Large quantities of low-grade ores and cal- nickel (Ni), and cadmium (Cd) in the region’s soil (Romic´ cines are stockpiled in their upstream banks and/or flood and Romic´ 2003). To date, very few studies examining plains. Numerous artisanal Hg retorting units exist in large toxic elements other than Hg have been systematically swaths north of the Aozhai River. The production of rice is conducted, particularly regarding the paddy soils in the the main activity of the local population of the Wanshan Wanshan Hg mining region. area. As this area was exposed to large-scale of Hg mining, The key to any environmentally corrective strategy in the exposure of the ecosystem (soil, water, and atmo- any given area, pertaining to the management of soil and its sphere) to Hg pollution and human health risks have been quality, is reliable and comparative data that examines reported at high levels (Søvika et al. 2011; Lin et al. many different environmental factors. Society must take 2011a). numerous aspects into consideration before proceeding toward actions that will effectively produce a sustainable 2.2 Sampling and measurement environment. Developing a plan for soil that is free from heavy metal pollution is no different. The first step is to The sampling campaign was conducted during the rice identify and quantify the source points of the heavy metals harvest season in September 2014. Two subsamples were that are known to present a risk to human health and the collected from each site. All soil samples were collected environment and to identify the specific areas in which and stored in sealed polyethylene bags to avoid cross- high levels of these metals indicate a proven risk to human contamination and then transported to the laboratory, health and the ecosystem (Zhang et al. 2007). A systematic where all samples were air dried, ground in a ceramic disc and thorough investigation of all heavy metals in the mill, and sieved through 150 mesh. The sampling sites are Wanshan mining region is urgently needed to accurately shown in Fig. 1. assess these risks. Studies that focus on only the risk caused Approximately 0.1–0.3 g of solid soil samples were by Hg do not provide a complete picture of the environ- digested in the mixed acid solution of HNO3–HF, and the mental impacts suffered by the region and therefore do not concentrations of Cd, Sb, Cr, Ni, Cu, Zn, Pb, Mn, As, and allow for the creation of a complete corrective strategy to Ti in the digests were determined by inductively coupled address the existing damages. plasma mass spectrometry (ICP-MS, Element, Finnegan The aim of this study was to measure the concentrations MAT Co.). For Hg, appropriate amounts of 0.3–0.5 g dry of Hg, Cd, As, Mn, Sb, Pb, Cu, Ni, Cr, and Zn in paddy samples were determined using a Lumex instrument, RA- soils near the abandoned mine areas of Wanshan to eval- 915? (Lumex Ltd., Russia). uate the current status of the pollution and to provide an Method blanks, duplicates, and certified reference assessment of the potential risks caused by the presence of materials were used for quality assurance and quality these metals if found. control. The recovery of the certified reference material (GBW07405) for all elements ranged between 97.63% and 110.76% (Table 1). All chemical analyses were carried out at the Institute of Geochemistry, Chinese Academy of Sciences. 123 Acta Geochim (2020) 39(1):85–95 87 Fig. 1 Map location of the study area and sampling sites Table 1 Concentrations of the different elements in the reference materials used in the present study and the results obtained (mg/kg) Element Certified reference material (GBW07405) (SEPAC) Hg Sb Cr Cd Pb Zn Cu As Ni Mn Tl Mean of measured value (mg/kg) 0.28 37.47 120.44 0.47 611.39 535.44 150.85 452.91 42.26 0.14 1.53 Certified value (mg/kg) 0.29 35 118 0.45 552 494 144 412 40 0.136 1.60 Recovery (%) 97.63 107.17 102.07 105.36 110.76 108.39 104.76 109.93 105.66 103.2 95.62 1r Standard deviation 0.02 2.52 8.02 00.06 36.6 33.30 9.65 24.62 3.75 0.01 0.12 n (Measurement times) 24 14 14 14 14 14 14 14 14 14 14 2.3 Statistical analysis where CF is contamination and; n is the number of metals.