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Mercury and Methylmercury in Riparian Soil, Sediments, Mine-Waste Calcines, and Moss from Abandoned Hg Mines in East Guizhou Province, Southwestern China

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Mercury and Methylmercury in Riparian Soil, Sediments, Mine-Waste Calcines, and Moss from Abandoned Hg Mines in East Guizhou Province, Southwestern China Applied Geochemistry Applied Geochemistry 20 (2005) 627–638 www.elsevier.com/locate/apgeochem Mercury and methylmercury in riparian soil, sediments, mine-waste calcines, and moss from abandoned Hg mines in east Guizhou province, southwestern China Guangle Qiu a,b, Xinbin Feng a,*, Shaofeng Wang a,b, Lihai Shang a,b a State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550002, PR China b Graduate School of the Chinese Academy of Sciences, Beijing 100039, PR China Received 14 April 2004; accepted 10 September 2004 Editorial handling by J.E. Gray Abstract Concentrations of total Hg and methylmercury (MMHg) in riparian soil, mine-waste calcine, sediment, and moss samples collected from abandoned Hg mines in Wanshan district, Guizhou province, China, were measured to show regional dispersion of Hg-contamination. High total Hg and MMHg concentrations obtained in riparian soils from mined areas, ranged from 5.1 to 790 mg kgÀ1 and 0.13 to 15 ng gÀ1, respectively. However, total Hg and MMHg con- centrations in the soils collected from control sites were significantly lower varying from 0.1 to 1.2 mg kgÀ1 and 0.10 to 1.6 ng gÀ1, respectively. Total Hg and MMHg concentrations in sediments varied from 90 to 930 mg kgÀ1 and 3.0 to 20 ng gÀ1, respectively. Total Hg concentrations in mine-waste calcines were highly elevated ranging from 5.7 to 4400 mg kgÀ1, but MMHg concentrations were generally low ranging from 0.17 to 1.1 ng gÀ1. Similar to the high Hg con- centrations in soil and sediments, moss samples collected from rocks ranged from 1.0 to 95 mg kgÀ1 in total Hg and from 0.21 to 20 ng gÀ1 in MMHg. Elevated Hg concentrations in mosses suggest that atmospheric deposition might be an important pathway of Hg to the local terrestrial system. Moreover, the spatial distribution patterns of Hg con- tamination in the local environment suggest derivation from historic Hg mining sites in the Wanshan area. Ó 2004 Elsevier Ltd. All rights reserved. 1. Introduction mental concerns. The primary concern about Hg mines is the biological accumulation of Hg, namely the conver- Mercury as a toxic element poses environmental con- sion from inorganic to organic Hg, such as methylmer- cerns, especially in historical Hg-mining districts. There cury (MMHg). Generally, historical mine-waste are many large Hg mines worldwide abandoned recently calcines (retorted ore) produced by inefficient roasting because of lower demand for Hg and increasing environ- of Hg ore contain abundant soluble Hg compounds, such as the elemental Hg and Hg salts (Kim et al., 2000, 2004). * Corresponding author. Tel.: +86 851 5891356; fax: +86 851 Such toxic Hg compounds are transferred to environ- 5891609. mental compartments, such as water, soil and sediments, E-mail addresses: [email protected], Xinbin@ and can be converted into organic compounds, which hotmail.com (X. Feng). eventually enter the human body through food chains. 0883-2927/$ - see front matter Ó 2004 Elsevier Ltd. All rights reserved. doi:10.1016/j.apgeochem.2004.09.006 628 G. Qiu et al. / Applied Geochemistry 20 (2005) 627–638 The Wanshan Hg deposit located in the eastern part 2.2. Hydrology and hydrogeology of Guizhou province, southwestern China, was ranked as the largest Hg-producing district in China. Mining The study area includes the Xiaxi, Aozhai, Hua- at Wanshan was initiated in the Qin Dynasty (221 ngdao and Gaolouping Rivers and covers an area of B.C.), but ceased in 2001. Approximately 22,000 ton approximately 174 km2 (Fig. 1). Meizixi stream, a tribu- of Hg, 6000 ton of cinnabar and large quantities of tary of the Aozhai River, flows through the discharges of mine-wastes have been produced at Wanshan. Between mine adits and mine-waste calcines. The upper tributary 1949 and the early 1990s, for instance, approximately of the Xiaxi River, named Dashuixi, flows through an 125.8 million tons of calcines and 20.2 billion m3 of ex- area where retorts are located and it is characterized haust gases containing Hg had been dispersed into adja- by high water pH ranging from 8.2 to 11.8 (Wu, cent ecosystems (Liu, 1998). Significant quantities of 2002). The Aozhai and Xiaxi River have an average base calcines were piled near old mine processing sites and stream flow from 0.25 to 0.45 m3 sÀ1 and an annual run- retorts. off of 131 million m3. Longjiang Reservoir, located Few geochemical studies relating Hg contamination along the Huangdao River, receives surface waters ema- to the local environment have been conducted at Wan- nating from mine-waste calcines. Geological outcrops in shan (Feng et al., 2003; Horvat et al., 2003; Wu, the drainage basin comprise limestone, dolomite and 2002). Total Hg concentrations in surface water emanat- sandstone with intercalated shale. ing from calcines were recently reported to be up to 580 ng LÀ1 (Feng et al., 2003) and 10,580 ng LÀ1 (Horvat 2.3. Mining and metallurgical activities et al., 2003), respectively. Total Hg concentrations in soil collected from the vicinity of a retort in the Wanshan There are many historical retorts and mining adits area are as high as up to 165 mg kgÀ1 (Wu, 2002). The distributed along or nearby the headwaters of both authors measured Hg in soil, sediment, and moss sys- Dashuixi and Meizixi streams (Fig. 1). The Guizhou tems in Wanshan to evaluate Hg contamination, distri- Hg retort, the largest Hg processing facility in the bution and the potential environmental risk to the Wanshan district, lies at the headwaters of Dashuixi ecosystem related to historical Hg mining. stream. Dashuixi Dam, which was built to receive drainage and mine-wastes discharged from the plant, is located at the upper end of the stream. A collection 2. Description of study area pond is located on a creek about 1100 m downstream from Dashuixi Dam. This pond was constructed in the The Wanshan Hg mining district is hilly and karstic, vicinity of a collapsed retort and a mining pit. Signif- ranging in elevation from 1149 to 270 m. The study area icant quantities of calcines and gangue were piled in has a sub-tropical humid climate characterized by abun- spoil heaps around this pond. Sources of water for dant precipitation and mild temperatures. Average the collection pond are the combination of mine yearly rainfall is of 1200–1400 mm. The annual average waters flowing through the surrounding calcines and minimum and maximum temperatures are 13 and 17 °C, mine water discharge. Similar to Dashuixi stream, cal- respectively, with the highest temperature of 33.5 °C cines were stock piled at the headwaters of Meizixi occurring in July. Most of the Hg mines and retorts in stream. Large quantities of rejected materials of waste this region are scattered in valleys. rocks, low-grade ores, and calcines are found in the stream banks or its flood plain. In addition, significant 2.1. Geology and mineralization quantities of calcines found at retort sites are located in the upper reach of Longjiang Reservoir. Mercury mines in the Wanshan area are primarily associated with thin-layered and laminated fine-grained dolomite or limestone beds of the Middle unit of Cam- 3. Sampling and analytical methods brian age. Surrounding rocks have undergone intensive alteration of silicification, dolomitization, calcification, Riparian soil, mine-waste calcine, sediment, and subordinately bituminization and pyritization (Hua moss samples were systematically collected from the and Cui, 1995). The primary ore mineral in the Wanshan Wanshan Hg mining district in November 2002 (Fig. deposits is cinnabar, with minor metacinnabar. Elemen- 1, Tables 1 and 2). tal Hg and Se-rich minerals occurring either as HgSe or Hg (Se,S) is found locally. Bitumen is common in the 3.1. Sampling and sample preparation Wanshan Hg ore bodies, but pyrite and other metal sul- fide minerals, which are significant acid–water produc- The authors collected riparian soils from rice pad- ing minerals (Gray et al., 2002a), are rare. Gangue dies and cornfields within or nearby a river channel- minerals are mostly quartz, calcite, dolomite and barite. bed. All soil sites are down gradient from Hg mining G. Qiu et al. / Applied Geochemistry 20 (2005) 627–638 629 M7 X10-11 r X9 Beijing Rive hai Aoz L12 Aozhai Guizhou Province L15 Study area Baiguoshu L14 M6 Xiaxi M4-5 er iv M1-2 R C1-3 xi L4-5 ia L6/11 X2-3 X6 L13 X M3 X4-5 N X1 P1 Guizhou Collection pond L9-10 X7-8 Hg Retort Dashuixi Dam Wanshan Town L1 C6 X12 r L8 C4 P2 e H 0 2.0km v u i L7 an R C5 L2-3 gd g a n o i Longjiang Reservior R p iv Mining adit Control sites u er o l Mine-waste calcines Moss o a Riparian soil Sediment profile G Fig. 1. Location of the sampling sites (see also Tables 1 and 2). areas. Soils collected distant from mined areas are re- 3.2. Analytical methods ferred to as ‘‘control sites.’’ Mine-waste calcines were collected as grab samples from discarded heaps. Depth For total Hg analysis, all samples were digested with a profile sampling was used in a large calcine pile to mixture of HNO3 and H2SO4 acids in a microwave oven. show the vertical distribution of Hg. Similarly, depth Then a suitable aliquot of digested sample solution was profile sampling at the shoreline of Dashuixi Dam measured using cold-vapor atomic absorption spectrom- and Longjiang Reservoir, both downstream of retorts etry (CV-AAS), with a detection limit of 0.01 lgkgÀ1.
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