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Bull Environ Contam ToxicolDOI 10.1007/s00128-016-1976-3

Persistent Mercury Contamination in Shooting Range Soils: The

Legacy from Former Primers

M. Staufer1 · A. Pignolet1 · J. A. Corcho Alvarado1 

Received: 8 June 2016 / Accepted: 16 November 2016 © Springer Science+Business Media New York 2016

and Rieder 2013) and its high persistence in soils (Schuster 1991; UNEP 2002; Jiskra et al. 2015), little is known about the contamination of shooting range soils with this metal. This may be due to the fact that Hg-containing ammuni-tion were replaced by formulations without Hg more than ifty years ago (Beck et al. 2007). However, Hg fulminate [Hg(CNO)2] was used in primers for rile and handgun ammunition for more than 100 years (Beck et  al. 2007). The thermal decomposition of this compound produces CO2, N2 and Hg (Garner and Hailes 1933; Zeichner et al. 1992). Numerous studies have shown that a large fraction of Hg (up to 86%) is vaporized after the irearm discharge (Zeichner et al. 1992; Wallace 1998). We may expect then that, after shooting, a major part of the released Hg will deposit near the iring line; but non negligible amounts may be transported longer distances.

In Switzerland, the use of Hg fulminate in ammunition started in the nineteenth century and continued until the 1960s. These ammunition were mainly used in shooting ranges for the regular shooting practice of civilian militia and sports clubs. Due to the long use of this type of ammu-nition, a signiicant deposition of Hg in the shooting ranges may be expected. Once deposited onto the soil, Hg strongly binds to soil constituents (Schuster 1991; Ravichandran 2004; Rieder et al. 2014; Rodríguez and Nanos 2016). Hg can exist in three valence states (0, I, II); however Hg(0) and Hg(II) are the dominant species in the soil (Schuster 1991). Plant uptake is normally extremely low and can gen-erally be neglected (Pant et al. 2010).

Hg in the soil may be nonetheless further mobilized by biogeochemical or physical processes (UNEP 2002; Jiskra et al. 2014). Redox conditions and pH are the most important factors controlling its aqueous speciation and transport in groundwater (Schuster 1991; Bavec and Gosar 2016). Other factors like dissolved organic matter (DOM)

Abstract Mercury (Hg) compounds were used in the past in primers for rile and handgun ammunition. Despite its toxicity, little is known about the contamination of shooting-range soils with this metal. We present new data about the Hg contamination of surface soils from numerous shooting ranges of Switzerland. Our study demonstrates that Hg is measurable at high levels in surface soils from the shooting ranges. In three of the investigated ranges, concentrations above the maximum Swiss guidance value of Hg in soil of 500 µg kg−1 were measured. Since the use of mercury-containing ammunition was stopped in the 1960s, our results demonstrate the high persistence of Hg in soils and their slow recovery by natural mechanisms.

Keywords Mercury contamination · Soils · Shooting ranges · Switzerland

Shooting ranges are known for their elevated contamina-tion in heavy metals from gunshot residues (Knechten-hofer et al. 2003; Hartikainen and Kerko 2009; Sanderson et al. 2012a, b; Okkenhaug et al. 2013; Islam et al. 2016). Lead (Pb) and antimony (Sb) are among the most investi-gated metals, mainly due to their high release in shooting ranges (Knechtenhofer et  al. 2003; Vantelon et  al. 2005; Scheinost et al. 2006; Wilson et al. 2006; Hartikainen and Kerko 2009; Okkenhaug et  al. 2013; Islam et  al. 2016). Despite the high toxicity of Hg (UNEP 2002; Dua and Gupta 2005; Rieder et al. 2011; Fernandes et al. 2012; Frey

* J. A. Corcho Alvarado jose.corcho@babs.admin.ch

1 Physics Division, Spiez Laboratory, Federal Oice for Civil Protection, Austrasse, 3700 Spiez, Switzerland

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may play an important role as well (Lodenius et al. 1987; Ravichandran 2004; Jiskra et  al. 2014). Strong interac-tions of Hg with the organic matter have been observed in soils (Lodenius et al. 1987; Schuster 1991; Yin et al. 1997; Jiskra et  al. 2014). Sorption and ixation of Hg is highest in soils containing elevated concentrations of molecules with thiol groups and fulvic and humic acids. Hg in the soil can however be transformed by methylating microbes (e.g. sulfate- and iron-reducing bacteria) into more mobile and toxic methylated forms such as monomethyl mercury (Munthe et  al. 2001; Ullrich et  al. 2001; Skyllberg et  al. 2006; Rieder et  al. 2011; Donovan et  al. 2016). This last compound is for example readily accumulated by biota and may thus pose a threat to soil microorganisms, animals and humans (Ullrich et al. 2001; Rieder et al. 2011).

The irst and main objective of this study is to obtain baseline information about the Hg contamination in surface soils from selected shooting ranges of Switzerland (Fig. 1). This is to our knowledge the irst time that such inves-tigation is carried out in shooting ranges. Other common ammunition contaminants (e.g. Pb, Sb, Cu and Zn) are as well determined in order to compare them with Hg. A last objective of this work was to obtain information about the potential role of the soil organic matter on the Hg ixation.

The information from this study will provide the basis knowledge for both: (a) an assessment of the long term risk of the Hg contamination in shooting ranges, and (b) deine the lines for future studies (e.g. speciation of Hg) in shoot-ing range soils.

Materials and Methods

Four shooting ranges, which are managed or its use is shared by the Swiss Federal Government, were selected for this study based on their construction year (Table 1; Fig. 1). The selected shooting ranges are located in Schwybogen, Mormont, Schollenholz and Sichtern (Fig.  1). The shoot-ing practice at the sites consist primarily of rile and hand-gun training with diferent types of bullets (e.g. calibers 7.5 × 55  mm GP11 and 5.6 × 45  mm GW Pat 90 for rile, and 9 and 7.65  mm Para/Luger for handgun); but other small calibers (<5.56 mm) are as well used. The soil in the shooting ranges is essentially covered by grass. Near the shooting ranges, soils are forested; but some areas are used for agricultural practices. The main characteristics of the shooting ranges and some information about the soils are given in Table 1.

Fig. 1 Map of Switzerland with the location of the shooting ranges managed by the Swiss Confederation (in red and yellow color). In red color are shown the sites investigated within this study. (Color igure online)

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Based on previous studies (Zeichner et  al. 1992), we expected to have a high Hg contamination limited to a small area near the shooter. It is expected as well that the Hg con-tamination will decrease with the distance from the iring point. Hence, soil samples (top 20 cm layer) were taken at 1 or 3 m increments from the iring point (see Fig. 2). Each sample (about 1  kg) was a composite of 16–25 subsam-ples taken at equidistant points from the shooter position

(Fig. 2). At the shooting ranges of Schwybogen and Mor-mont, samples were taken at 1 m distance increments from the shooter position (see example depicted in Fig. 2). For the shooting ranges of Schollenholz and Sichtern, a 3  m distance increment was used. A reference background soil sample was taken at each investigated site. The reference soils were collected outside and away from the shoot-ing ranges in order to estimate the natural background

Table 1 Description of the investigated shooting ranges with some properties of the soil

OM organic matter content in percent

Site Canton Swiss coordinates Distance from iring line (m)

Construction year Main use Hg-Fulminate primers

Soil type (m) OM (%)

Schwybogen, Stans, Nidwalden

670 650, 202 600 50 m300 m

1926/1986 Before military now civilian training

Heavily used Luvisol 9.9–20.9

Mormont, Bure, Jura

569 050, 254 700 50 m300 m

1968/1990 Military training Never used Calcosol 7.1–9.9

Schollenholz, Frau-enfeld, Thurgau

708 425, 267 230 2 × 25 m2 × 50 m2 × 300 m

1909 Military and civil-ian training

Heavily used Luvisol 5.2–9.2

Sichtern, Liestal, Biel

620 104, 259 235 25 m50 m2 × 300 m

1871/1972 Military and civil-ian training

Heavily used Cambisol 10.9–11.2

Fig. 2 Sampling protocol used for the 50  m shooting range of Schwybogen. a Side view with the position of each sample at 1  m increments from the iring point. b Above view with a rough location

of the subsamples (brown points in the lines) composing each sample. The sample N, for example, is a composite of N subsamples collected at 30 m from the iring point. (Color igure online)

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concentration of Hg in the soils (e.g. Hg from geogenic and/or atmospheric deposition origin). The reference sam-ple was collected at distances from the shooting range vary-ing from 165 m in Mormont to 600 m in Schollenholz.

The samples were analysed within 1 week after the collection date. Soils were characterized for organic mat-ter content by using the loss of ignition method. The soil samples were dried at 40°C and then sieved (2  mm frac-tion) to remove stones and litter. After a homogenization step in a tubular mixer, the total Hg content in the soil was determined according to EPA method 7473 by a direct Hg analyzer (DMA-80, Milestone). The DMA-80 has a wide working range up to 10′000 µg kg−1, with a detection limit as low as 0.1  µg  kg−1 Hg. The expanded measurement uncertainty (95%) was estimated to be at ±20%. The per-formance of the method was veriied with the certiied ref-erence materials for Hg in soil CGL-303 and CGL-304, which were supplied by the Central Geological Laboratory of Mongolia. The results of the standard reference mate-rials where within the certiied ranges of these materials. Three replicates of each sample were analyzed. The con-tinuous calibration veriication (CCV) was applied during all runs. The analysis of was lead (Pb), copper (Cu), zinc (Zn) and antimony (Sb) was conducted by Inducted Cou-pled Plasma Mass Spectrometry (ICP-MS) after a total digestion, according to the EPA method 200.8. The quality control of the measurement (e.g. calibration, internal stand-ards, CCV, blanks, etc.) was conducted as described on the EPA method. A generic detection limit of 0.1 mg kg−1 was achieved.

Results and Discussion

The concentration of Hg in the background soils, assumed to represent the natural background conditions at the sites, vary largely with values as low as 44 µg kg−1 in Mormont, 84 µg kg−1 in Schollenholz, 102 µg kg−1 in Sichtern and up to 315 µg kg−1 in Schwybogen (Fig. 3). As these reference samples were taken not far from the shooting ranges (165–600  m), a slight contamination with Hg originated from shooting activities cannot completely be excluded. The Hg concentrations in background soils are nonetheless similar to the ones observed in non-disturbed surface soils of Swit-zerland. For example, Hg concentrations varying from 70 up to 360 µg kg−1 have been reported in undisturbed forest soils of Switzerland (Ernst et al. 2008; Rieder et al. 2011, 2014). Hg is naturally found in the earth’s crust at an aver-age level of 50 µg kg−1 (John et  al. 1975; Schlüter 1993; Gustin and Lindberg 2005). Elevated concentrations of Hg above 6000 µg kg−1 have been reported for anthropogeni-cally contaminated sites (Inácio et al. 1998; Neculita et al.

2005; Arbestain et al. 2009; Fernández et al. 2015; Bavec and Gosar 2016).

The concentration of Hg in soils from the shooting ranges as a function of the distance from the iring line is shown in the Fig. 3. Hg concentrations well above the con-centrations measured in the background soils were found in 11 of the 14 shooting ranges. Elevated concentrations, above the maximum Swiss guidance value concentration of Hg in soil of 500  µg  kg−1 (OIS 1998), were measured in Schollenholz (at the 300 m old and 25 m Elo ranges) and Schwybogen (at the 50 m range). However, in Switzerland, there is no threshold value for treatment and/or remediation of Hg in undisturbed soils (Frey and Rieder 2013).

An exponential decrease of the concentration of Hg along the distance from the iring line was observed in most of the investigated sites (Fig.  3). In soils from the 25  m Elo range at Schollenholz and the 50 m range at Schwybo-gen, the concentration of Hg did not show any trend to decrease along the distance (Fig. 3a, b). The Schollenholz range is known to have been modernized several times in the past. For this site, it is documented that the soil level of the 300 m range was lowered and that in parallel the 25 m range was constructed. It is then suspected that the old soil from the 300 m range was used in the construction of the 25 m range. This may be the explanation for the extremely high concentrations of Hg in soils from the handgun 25 m range at Schollenholz. This would explain as well the low variability of the concentration of Hg in soils from the 25 m range.

The 50  m range at Schwybogen was constructed in 1986. The elevated concentrations of Hg found at this stand may possibly be explained by the use of old contaminated soils for the construction of the new stand. A less probable explanation might be that Hg-fulminate ammunition was used after their oicial replacement with more eicient and less toxic primers. In any case, due to the lack of suicient information, it is diicult to verify any of the hypotheses. For the 300 m old range at Schollenholz, the Hg concen-trations fall below the guidance value of 500  µg  kg−1 (OIS 1998) at a distance of 9 m from the shooter position (Fig. 3b).

For the rest of the ranges, where intermediate Hg con-centrations (above 50 and below 500  µg  kg−1) where measured in the soil, a decreasing trend along the dis-tance is observed. Due to the old age of the 300 m range at Sichtern, elevated Hg levels were expected at this site (Fig. 3c). The almost hundred years younger 50 m handgun range at Sichtern showed higher Hg concentrations than the older 300 m ranges. This may be attributed to reported construction activities that may have relocated the contami-nated soils in the new ranges.

The two ranges at Mormont, which were constructed after replacement of the Hg-fulminate primers, showed

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no Hg contamination (Fig. 3d). The concentrations of Hg in surface soils from the Mormont ranges varied between 28 and 51  µg  kg−1, very close to the concentration of 44 µg kg−1 found in the background soil. This site can be taken then as a reference site free of contamination with Hg-fulminate decomposition products.

Soils from the studied ranges showed a large variabil-ity in the content of organic matter (OM) in the range of 5%–21% of the total dry weight (Table 1). The highest val-ues were observed at the site of Schwybogen (9.9%–20.9%).

No relationship was observed between the content of OM and the concentration of Hg in the soils. This may be due to the fact that the spatial distribution of the Hg contamina-tion is mainly controlled by the release and deposition of Hg near the iring line. Moreover, construction activities in the past may have perturbed the upper layer of the soil and consequently the original Hg distribution.

Taking into account that range at Schollenholz is one of the oldest and that elevated Hg concentrations were found in the soil, a detailed analysis of other trace metals was

Fig. 3 Hg concentration in soils (in µg kg−1) as a function of the distance from the iring point. a Shooting range of Schwybogen, b shooting range of Schol-lenholz, c shooting range of Sichtern and d shooting range Mormont. The average, maxi-mum and minimum concentra-tions are given. The maximum recommended concentration of Hg in soils (500 µg kg−1) and the concentration of Hg in the reference soils are also indicated

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conducted at this site. Our analysis shows that soils in the Schollenholz ranges are slightly contaminated with Pb, Cu, Zn and Sb (Fig.  4). The concentration of Pb, Cu and Zn in soils from the 25 and 300 m ranges show rather similar exponential decreasing trend from the shooter position than the one observed for Hg. The concentrations of Pb and Sb are below the maximum threshold value concentration in soil (Pb: 2000 ppm, Sb: no threshold value) (OIS 1998). At the 50 m range, Cu and Zn show elevated concentrations in the irst few meters from the shooter, above the threshold

values (Cu: 1000 ppm; Zn: 1000 ppm). This may be caused by the frequent use of small caliber arms (<5.56  mm) at those kinds of ranges. Tombac (an alloy of Cu and Zn) is used in bullet jackets of that ammunition and can there-fore be found as abrasion product in front of the shooters position.

A similar deposition efect is observed for anthropogenic Pb and Sb. However, since Pb and Sb are usually alloyed as core of the projectile, the emission usually only occurs at the rear of the core due to the high temperature during the

Fig. 4 Trace metal concen-tration in soil (in mg kg−1) from the shooting range of Schollenholz as a function of the distance from the shooter position: a Pb, b Cu, c Zn and d Sb. The average, maximum and minimum concentrations are given. The concentration in the reference soil is also indicated

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ignition process. This may leads to lower concentrations in the soil compared to Cu and Zn. The concentrations of these elements show strong decreasing trends in the irst few meters from the shooting ranges. Contrary to Hg, the elements Pb, Cu, Zn and Sb are not easily volatized. We expect then to have the contamination localized near the shooter and the targets. Our results support the hypothesis that these elements are originated by shooting.

This study demonstrates that decomposition products of Hg-fulminate, compound used in primers until the 1960s, are measurable in surface soils from several shooting ranges in Switzerland. Further investigation of old shoot-ing ranges are needed to assess the level of anthropogenic Hg in the soils and its impact. This study further demon-strates the high persistence of Hg in soils and their slow recovery by natural mechanisms. In such anthropogenic contaminated sites, enhanced Hg concentrations may per-sist and therefore they provide ideal conditions to study the behavior of Hg and its species. Hg species are known to be highly toxic for microorganism, animals and humans (UNEP 2002; Dua and Gupta 2005; Rieder et al. 2011; Fer-nandes et al. 2012; Frey and Rieder 2013). Shooting ranges provide therefore an interesting scenario (polluted soils) for further investigating pathways of long term exposure to Hg from soil, groundwater and its bioaccumulation (e.g. earth-worms, mushrooms, etc.). The relatively poor knowledge of former building activities on old shooting ranges and the inconsistent or lack of data about the amount of shots ired from a range may nonetheless be important constraints.

Acknowledgements We acknowledge the support of Armasuisse for this project. We would like to also thank the technical support pro-vided by Hans Sahli (Radioactivity Branch) and the collaborators of the Environmental Testing Group.

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