You are on page 1of 20

Environ Geochem Health (2011) 33:311329

DOI 10.1007/s10653-011-9381-7

ORIGINAL PAPER

Contaminated lead environments of man: reviewing


the lead isotopic evidence in sediments, peat, and soils
for the temporal and spatial patterns of atmospheric
lead pollution in Sweden
Richard Bindler

Received: 28 June 2010 / Accepted: 17 October 2010 / Published online: 22 March 2011
Springer Science+Business Media B.V. 2011

Abstract Clair Patterson and colleagues demonstrated already four decades ago that the lead cycle
was greatly altered on a global scale by humans.
Moreover, this change occurred long before the
implementation of monitoring programs designed to
study lead and other trace metals. Patterson and
colleagues also developed stable lead isotope analyses
as a tool to differentiate between natural and pollutionderived lead. Since then, stable isotope analyses of
sediment, peat, herbaria collections, soils, and forest
plants have given us new insights into lead biogeochemical cycling in space and time. Three important
conclusions from our studies of lead in the Swedish
environment conducted over the past 15 years, which
are well supported by extensive results from elsewhere
in Europe and in North America, are: (1) lead
deposition rates at sites removed from major point
sources during the twentieth century were about 1,000
times higher than natural background deposition rates
a few thousand years ago (*10 mg Pb m-2 year-1 vs.

R. Bindler (&)
Department of Ecology and Environmental Science,
Umea University, 901 87 Umea, Sweden
e-mail: richard.bindler@emg.umu.se

0.01 mg Pb m-2 year-1), and even today (*1 mg Pb


m-2 year-1) are still almost 100 times greater than
natural rates. This increase from natural background to
maximum fluxes is similar to estimated changes in
body burdens of lead from ancient times to the
twentieth century. (2) Stable lead isotopes (206Pb/207Pb
ratios shown in this paper) are an effective tool to
distinguish anthropogenic lead from the natural lead
present in sediments, peat, and soils for both the
majority of sites receiving diffuse inputs from long
range and regional sources and for sites in close
proximity to point sources. In sediments[3,500 years
and in the parent soil material of the C-horizon,
206
Pb/207Pb ratios are higher, 1.3 to [2.0, whereas
pollution sources and surface soils and peat have lower
ratios that have been in the range 1.141.18. (3) Using
stable lead isotopes, we have estimated that in southern
Sweden the cumulative anthropogenic burden of
atmospherically deposited lead is *25 g Pb m-2
and *1 g Pb m-2 in the pristine north. Half of this
cumulative total was deposited before industrialization. (4) In the vicinity of the Ronnskar smelter in
northern Sweden, a major point source during the
twentieth century, there is an isotopic pattern that
deviates from the general trends elsewhere, reflecting
the particular history of ore usage at Ronnskar, which
further demonstrates the chronological record of lead
loading recorded in peat and in soil mor horizons.
Keywords Lead isotopes  Lake sediments 
Peat  Soil  Atmospheric pollution

123

312

Introduction
Already 45 years ago in his landmark paper, Contaminated and natural environments of man, Patterson (1965) concluded:
The industrial usage of lead is so massive
today that the amount of lead mined and
introduced into our relatively small urban
environments each year is more than 100
times greater than the amount of natural lead
leached each year from soils by streams and
added to the oceans over the entire earth.
There are indications that about nine tenths of
the lead in the upper mixed zones of the open
oceans in the northern hemisphere originates
from lead mines, and that the atmosphere
contains about 1,000 times more than natural
amounts of lead.
Patterson was a renowned geochemist who was
instrumental in developing the analytical techniques
required for the precise isotopic measurement of lead
in minerals at trace levels to date the age of the earth
(Patterson et al. 1955). In so doing, he was confronted
with the critical issue of a widespread contamination
of lead that added to the challenges of his work. In
pursuing this new interest in understanding the scope
of lead contamination, he and his colleagues laid the
foundation for a whole field of research aimed at
understanding the anthropogenic influence on lead
biogeochemistry.
Three components of Patterson and colleagues
research that are essential here are that he understood
that there was a long-term component to metal
contamination in the environment, which extends
back through antiquity and into pre-history (Patterson
1971, 1972; Settle and Patterson 1980). He viewed
this from the perspective of lead production with
time, but also its relationship to human health from
the perspective of exposure to lead (Ericson et al.
1975). Second, he and colleagues recognized that
there was an important long-range component,
whereby an initial link was made between increases
in lead concentrations in glacial ice from northern
Greenland and industrialization and metal emissions
from areas at lower latitudes (Murozumi et al. 1969).
Third, he transformed lead isotope analyses as a
technique to be used in dating the age of the earth and
the continents into a tool that could be used to

123

Environ Geochem Health (2011) 33:311329

distinguish the lead naturally present in soils from the


lead added to the environment that is derived from
lead-bearing ores (e.g., Chow and Patterson 1962;
Patterson and Hirao 1974; Shirahata et al. 1980). As a
geochemist, Patterson was well versed in the natural
heterogeneity in lead composition of different minerals, but he recognized that the lead naturally present
in soils and lake sediments could be isotopically
distinguished from the ore-derived lead being added
to the environment by human activities, such as
mining and the addition of alkyl lead to gasoline.
This combination of considering time, distance,
and isotopic composition when studying lead in lake
sediments, peat, boreal forest soils, and the overlying
vegetation has been central to research done by our
group at Umea University and quite a number of
other groups working elsewhere in Europe (e.g.,
Bacon et al. 1995, 1996; Farmer et al. 1996; Shotyk
et al. 1998; Weiss et al. 1999; Farmer et al. 2002; Le
Roux et al. 2005; Steinnes et al. 2005b; Bacon et al.
2006; Graham et al. 2006; Cloy et al. 2008) and
North America (e.g., Kaste et al. 2003; Watmough
et al. 2004; Watmough and Dillon 2007). Based on
these results, as I will summarize later, Pattersons
estimate in 1965 of a 1,000-fold increase in atmospheric levels of lead as compared to the natural
environment has proved fairly accurate for remote
areas removed from emission point sources but
exposed to long-range sources and diffuse local/
regional atmospheric sources (e.g., car and industrial
emissions).
The title of this paper intentionally harkens back to
Pattersons 1965 paper, and there are a few initial
premises that are best stated here in the beginning.
Firstas I think is quite evident from the data that I
present in this reviewis that based on the results of
research I have been involved in over the past
15 years, I am convinced that human activities have
greatly altered the biogeochemical cycling of lead in
the environment. Furthermore, this impact has
occurred not only over a period of decades or over
the centuries constituting the industrial era, but over a
few to several millennia. However, although it is
reasonable to argue that there is a very broad
consensus that recognizes the long-term input of lead
to the environment and its significance related to lead
cycling in the present-day environment, it is important to acknowledge that this is not a unanimous
consensus. For example, recent papers by Reimann

Environ Geochem Health (2011) 33:311329

et al. (2008c, 2009a) have engendered a number of


comment and review exchanges (Bindler 2008; Le
Roux et al. 2008; Reimann et al. 2008a, b, 2009b;
Shotyk 2008; Steinnes 2009), which have provided
productive discussions for a range of important
factors, particularly the influence of geologybut
with rather contrary interpretations and conclusions
from the different sides of the debate. Reimann et al.
make a valuable point in emphasizing the importance
of geology as a controlling factor for the distribution
of metals at continental and global scales, but at such
large scales important information on other factors at
site, local, or regional scales can be lost. This debate
over the relevance of anthropogenic inputs to the lead
biogeochemical cycle in todays environment has its
parallel with the scientific debate in the 1990s
regarding the important influence of anthropogenic
contributions to the global mercury cycle (e.g.,
Rasmussen 1994; Fitzgerald et al. 1998). The aim
of this review is not to delve into this controversy per
se, but I think that these recent scientific exchanges
suggest that it is time to review again some of the
results from the application of lead isotope analyses
in environmental research, which in the case here is
rooted largely in data from Sweden with supporting
data from other areas.
Second, any purported revieweven in the case
here where I mostly synthesize data from our
groups research in Swedenmust in the end make
a selective use of studies in order to meet restraints
on space that will undeniably be based on the
authors/authors selection from the available data.
However, by choosing data mainly from a geographically restricted area such as Sweden some of
the variability relating to geological setting and to
the geographic diversity of pollution history is
reduced. Besides our results from Sweden, I make
substantial reference to data particularly from studies
of a similar scope by research groups in Norway,
Scotland, Canada, and Switzerland/Germany referenced above.
A third premise is that stable lead isotopes, as
Patterson and colleagues had shown, are a powerful
tool for distinguishing between the lead naturally
present in the environment and the lead added to the
environment from human activities, which is derived
from ores. Lead-bearing ores usually have a deviating
composition in comparison with the common bedrock
because the ore lead was separated from the uranium

313

and thorium in the initial rock material, and therefore


the isotopic composition of these ores does not
appreciably alter over time, whereas lead isotope
ratios continue to evolve in the original bedrock
(Brown 1962; Faure 1986). However, although we
can specifically characterize the lead isotopic composition of many anthropogenic lead sources (e.g.,
Hopper et al. 1991; Stos-Gale et al. 1995; Farmer
et al. 1999) as well as geogenic lead (Erel et al. 1994;
Harlavan et al. 1998; Harlavan and Erel 2002;
Klaminder et al. 2005), both of these sources are in
fact quite heterogeneous. The mineralogy of soils can
be quite complex and weathering processes and their
potential influence on lead isotopic composition are
generally well understood, but cannot be well quantified in all regards. Nonetheless, the isotopic composition of geogenic and anthropogenic sources can
in most cases be characterized within well-defined
boundaries.
The fourth premise, for which there is no space to
delve into in this paper, is that the biogeochemical
cycling of other metals besides lead are also greatly
impacted by human activities, not least mercury
(Fitzgerald et al. 1998). Lead has the advantage in
that stable isotope analyses have become routine,
many environmental components have been isotopically characterized, and from a biogeochemical
perspective lead mobility is not significantly influenced by processes such as plant uptake (Hagemeyer
and Hubner 1999; Hovmand et al. 2009) or acidification (Norton and Kahl 1991).
The objectives of this paper are to: (1) review the
evidence for a long-term deposition of pollution lead,
based largely on results from analyses of lake
sediment and peat records in Sweden; (2) demonstrate that this anthropogenic lead can be traced in the
environment using stable lead isotope analyses; and
(3) demonstrate that this long-term historical loading
of lead in the environment has important implications
when studying the biogeochemical cycling of lead in
boreal forest soils of Scandinavia. By incorporating
numerous references to similar research elsewhere in
Europe, and to lesser extent elsewhere, a further aim
is to (4) show that the implications of these results are
similar to many other areasalthough, of course,
there will be many differences due to differences in
deposition histories and the precise biogeochemical
conditions, such as vegetation cover, soil type, and
mineralogy, as well as climatic factors.

123

314

Evidence for millennial scale impacts on global


lead cycling from anthropogenic activities
Based on the earlier work by Patterson (1971, 1972),
Settle and Patterson (1980) summarized the global
lead production history from ancient times to the late
twentieth century (Fig. 1), which was later refined
further by Nriagu (1983, 1996). In brief, lead
production has its roots more than 5,000 years ago
in association with the smelting of lead and silverbearing sulfide ores and the subsequent cupeling of
silver. However, lead was emitted as a by-product of
copper smelting on a local scale already some
1,000 years or more prior (Grattan et al. 2007;
Mighall et al. 2009). Lead production rose from c.
2,700 years ago with the introduction of silver
coinage and peaked initially c. 2,000 years ago during
the Roman period. Production was reduced following
the collapse of the Roman Empire, but began to rise
again from about AD 1000 with opening (or reopening) of silver mines particularly in Germany.
Only with the start of the industrial revolution did the
global production of lead exceed that during the
Roman period. The importance of this is that from a
long-term perspective large-scale metal production
and thus also emissionsdid not originate with the
eventual Industrial Revolution.

Fig. 1 Top panel the


estimated global production
of lead over the past
4,000 years (Settle and
Patterson 1980). Middle
panel 206Pb/207Pb ratio and
lead concentration record
from the Greenland summit
ice (Rosman et al. 1997).
Bottom panel 206Pb/207Pb
ratio and lead concentration
records from 11 lakes in
southern and central
Sweden (Brannvall et al.
2001a)

123

Environ Geochem Health (2011) 33:311329

This schematic pattern outlined for historical lead


production is the same general pattern that has
subsequently been found for lead accumulation in
natural archives in much of Europe as well as the
Greenland summit ice (Renberg et al. 2001) (Fig. 1).
These archives include lake sediments in Sweden
(Renberg et al. 1994; Brannvall et al. 1999, 2001a;
Bindler et al. 2001); peat deposits in Sweden (Bindler
et al. 1999; Klaminder et al. 2003), Spain (MartnezCortizas et al. 2002; Kylander et al. 2005), France
(Monna et al. 2004a, b; Baron et al. 2005), Belgium
(De Vleeschouwer et al. 2007), Switzerland (Shotyk
et al. 1998), Germany (Le Roux et al. 2005), the UK
(Le Roux et al. 2004; Cloy et al. 2008), and Iceland
(Marshall et al. 2009); and ice records from Greenland and Devon Island (Hong et al. 1994; Rosman
et al. 1997; Zheng et al. 2007).
In most studies cited above, the data also include
stable lead isotope composition. Lake sediments,
peat, and ice represent fairly distinct environmental
geochemical conditions; yet in all cases, the characteristic increases in lead concentration and accumulation rates that occurred c. 2,000 years ago and c.
AD 1000 are accompanied by a change in the lead
isotopic composition, which is most commonly
represented as declining 206Pb/207Pb isotope ratios.
For ombrotrophic peat records and the Greenland ice

Environ Geochem Health (2011) 33:311329

record (Figs. 1, 2), in both of which cases the lead


content is controlled solely by atmospheric deposition, 206Pb/207Pb ratios prior to c. 3,000 years ago
were typically in the range of 1.191.23 and characteristic of average upper continental crust values and
the pelagic sediments of mixed continental origin in
the North Atlantic (Chow and Patterson 1962;
Hamelin et al. 1990; Kramers and Tolstikhim
1997). In contrast, the periods of increased lead
concentrations and accumulation rates in all three
types of archives (i.e., peat, ice and lake sediments)
coincide with an influx of lead with a 206Pb/207Pb
ratio in the range of 1.161.18, which is a range
characteristic of lead-bearing ores across continental
Europe (see references provided in, e.g., Rosman
et al. 1997; Kylander et al. 2005), but excluding the
Precambrian lead-bearing ores of Scandinavia that
were exploited from the medieval period having a
ratio of 1.02 (Ek and Renberg 2001; Bindler et al.
2009).
Although this historical pattern is broadly repeatable in natural archives across Europea continental
scale pattern of a sort, which is to be expected given
the interlinked technological, economic, and political

315

historiesthe precise details are quite heterogeneous.


Historical mining was not restricted to only a few
specific mining areas, but occurred at a widespread
number of locales and regions across Europe. Based
on economic and political conditions, the scale and
location of mining varied over time (Postan and
Miller 1987), and this is reflected in the diversity of
the lead records across Europe, which display distinct
regional differences (Renberg et al. 2001). For
example, during the Roman period mining was quite
extensive in the Iberian Peninsula, which is reflected
in a more distinct peak in lead in peat records from
this region at that time (Kylander et al. 2005).
Lead accumulation rates increased by nearly
30-fold from natural background values of 0.03 mg
Pb m-2 year-1 prior to 3000 BP to 0.85 mg Pb m-2
year-1 during the period 25001700 BP. In contrast,
during the Middle ages mining was more intense in the
Harz region in northern Germany, and the increases in
lead are most pronounced in this region at that time
but hardly visible at all in the Spanish peat records. In a
peat record from the Harz mountains, lead concentrations increased from natural background values of
0.3 lg Pb g-1 to 1,500 lg g-1 about AD 1200

Fig. 2 Lead concentration


and 206Pb/207Pb ratios in
three peat records from
southern Sweden (Bindler
et al. 1999). Average lead
accumulation rates (lg Pb
m-2 year-1) for
background, medieval, and
the 1970s are marked

123

316

(Kempter and Frenzel 2000). The concentrations in


layers from this time period were never exceeded again
in this region, not even in modern times (Kempter and
Frenzel 2000; Hettwer et al. 2003).
For many peat sites, such as in Spain, England,
France, or Germany, the precise isotopic composition
of the lead entering the records is highly dependent in
large part on the proximity to local or regional mining;
many of these ores have been well characterized in
terms of their isotopic composition (e.g., Grogler et al.
1966; Brill and Wampler 1967; Monna et al. 2000;
Kylander et al. 2005; Baron et al. 2009). However, in
the case of study sites located in Scotland, Sweden,
Iceland, and most obviously Greenland, these regions
were far removed from the earliest centers of mining
and metallurgy, and the additional lead must have
been derived from long-range atmospheric transport.
Not only do the lead isotope analyses indicate an
ore origin for the additional lead entering the natural
archives from the Roman period onwards, but
analyses of the geochemical matrix of the archives
precludes other explanations for the source of the
lead. Although early land use certainly increased soil
dust fluxes c. 3,0005,000 years ago in Europe, this
would have led to only a small 23-fold increase in
the quite low lead accumulation rates (discussed
further below). The lead peak occurring about
2,000 years ago across much of Europe as well as
the renewed increase about AD 1000 were certainly
not driven by increases in mineral matter fluxes nor
by other changes in the inorganic geochemistry in the
peat or ice records (e.g., Rosman et al. 1997; Shotyk
et al. 2001; Kylander et al. 2005).
Historical lead pollution and lead deposition rates
in Sweden
Following deglaciation, which ranged from about
14000 BP in southernmost Sweden to 8000 BP in the
north (and in some areas also the subsequent marine
regression) and up until about 3500 BP, the lead
isotopic composition of the lake sediment records
reflected values typical of Precambrian shield bedrock, which has had time to evolve their characteristically higher 206Pb/207Pb ratios (Chow 1965). In
Sweden, the sediments up to 3500 BP had consistently high 206Pb/207Pb ratios in the range of 1.3 to
2.0 (Brannvall et al. 1999; Bindler et al. 2001, 2009;
Brannvall et al. 2001a).

123

Environ Geochem Health (2011) 33:311329

In Sweden, the earliest changes in lead composition


in lake sediments and peat occurred as both a small
peak in lead concentrations, and a decline in
206
Pb/207Pb ratios that began gradually as early as
3,500 years and reached a well-defined peak
2,000 years ago. Based on the more precise chronology available from a few annually laminated sediment
records, this peak was centered about AD 80 (Brannvall et al. 1999; Bindler et al. 2009). A greater increase in
lead concentrations and a sharp decline in 206Pb/207Pb
ratios in sediments began AD 1000, which at least in
southern Sweden was likely driven more by long-range
transport from mainland Europe and particularly
Germany based on atmospheric modeling of historical
source regions (Brannvall et al. 1999; Brannvall et al.
2001a; Klaminder et al. 2003), which is in accordance
with the distribution of atmospherically transported
pollutants based on current atmospheric modeling.
For the pollution lead signal 2,000 and 1,000 years
ago, there is an overall declining gradient from south to
north (Renberg et al. 2000), which has been demonstrated for modern pollution gradients in surface
sediments (Renberg et al. 1994), soil O-horizons
(Alriksson 2001), and biomonitoring (forest mosses)
surveys (Ruhling and Tyler 2001). However, in central
and possibly northern Sweden, the lead pollution
occurring from about AD 1000 also involved a
significant regional component derived from the
burgeoning mining and metallurgical activities in the
Bergslagen mining region of central Sweden (Ek and
Renberg 2001; Bindler et al. 2009), a regional
influence that was still apparent in the sediment, soil,
and forest moss surveys in 19801990 (Fig. 3).
For the peat records from Sweden (Fig. 2), which
can be used as a close approximation for the changes in
atmospheric lead deposition, lead deposition prior to
3500 BP was dominated by 206Pb/207Pb ratios characteristic of soil dust from mainland European
bedrock and soils, 1.191.24 (Bindler et al. 1999;
Klaminder et al. 2003; Kylander et al. 2010). More
importantly, the accumulation of lead in the peat
records during the mid-Holocene was quite low,
approximately 0.0010.01 mg Pb m-2 year-1, which
is similar to the estimated values in the range of
0.010.3 mg Pb m-2 year-1 from sites in Switzerland
(Shotyk et al. 1998), southern Germany (Le Roux et al.
2005), and northwestern Spain (Kylander et al. 2005).
From about 3000 BP, the heterogeneous lead composition of the Swedish peat records began to change

Environ Geochem Health (2011) 33:311329

317

Fig. 3 Spatial distribution


of lead in Sweden from the
forest mosses biomonitoring
program in 1985 (data from
ivl.se), in surface sediments
sampled in 1986 (Renberg
et al. 1994), and in the
O-horizon of forest soils
(Alriksson 2001) sampled in
19931995. Lead
concentrations (mg kg-1)
are divided into quartiles for
each sample type

toward isotope ratios characteristic of mainland


European ores; and by 2,000 years ago, the
206
Pb/207Pb ratios had declined to values of
1.1751.19, and by AD 1000 declined further to
1.171.175. These changes in isotopic composition
during the Roman period were accompanied by an
increased deposition of lead to about 0.1 mg Pb m-2
year-1, which corresponded to a 10-fold increase in
Sweden and in other regions. The deposition rate
increased a further 10-fold to *1 mg Pb m-2 year-1
by AD 1200 in the Swedish, Swiss, and southern
German sites (Bindler et al. 1999; Klaminder et al.
2003; Le Roux et al. 2005), and in the Harz mining
region the increase in lead concentration in the peat
records from this area corresponded to at least a 1,000fold increase in deposition (Kempter and Frenzel
2000; Hettwer et al. 2003). This rate of lead deposition
to remote sites in south-central Sweden and elsewhere
c. AD 1200, *1 mg Pb m-2 year-1, is comparable to
lead deposition rates experienced at these sites in the
first decade of the twenty-first century (Swedish
deposition data including forest mosses and precipitation chemistry available at ivl.se).
Metallurgy is of course not the only human-related
environmental change to have occurred since the
mid-Holocene that might have had some relevance to
the atmospheric transport of lead and other trace
metals. Lead deposition rates increased about 23-

fold over background values in conjunction with


increased atmospheric dust transport beginning in
Sweden about 30004000 BP with the wider spread
of agriculture and associated deforestation. This is
visible, for example, as a small increase in scandium
and titanium concentrations and fluxes (Klaminder
et al. 2003; Bindler and Klaminder 2006). This 23fold increase in soil dust fluxes, which is also
observed elsewhere in Europe (Shotyk et al. 2001;
Kylander et al. 2005; Martnez Cortizas et al. 2005,
2007), is unable to account for the 10, 100 and 1,000fold increases in lead accumulation recorded during
the Roman, Medieval, and late twentieth century,
respectively.
During the later half of the twentieth century, lead
deposition rates at remote sites in southern Sweden
and Norway and in southern Germany increased a
further 10-fold to 1015 mg Pb m-2 year-1 (Ross
1990; Berg and Steinnes 1997; Le Roux et al. 2005),
i.e., to values 1,000-fold greater than the natural
background deposition rates prior to 3500 BP. From
1970 to the present day, lead deposition rates have
declined by more than 90%. Importantly, this
declining trend is captured both by biomonitoring
programs (Ruhling and Tyler 2001; Steinnes et al.
2005a) and by the peat records (Bindler et al. 1999;
Le Roux et al. 2005) (Fig. 4), as well as sediment and
ice records.

123

318

This overlap between 40 years of monitoring and


the recent 40 years in peat records is critical, because
it provides an opportunity to validate the peat records
as an archive for past atmospheric deposition rates of
lead [for mercury, however, this question is more
problematic (Biester et al. 2007)]. Lead deposition
rates calculated from the forest mosses in southern
Sweden have declined from 810 mg Pb m-2 year-1
in 1975 to 0.5 mg Pb m-2 year-1 in 19952005; lead
deposition rates have been slightly higher in southern
Norway due to the closer proximity to emission
sources in the UK. By including moss concentration
from herbaria samples (Swedish EPA 1987) and
applying the same equation from Ruhling and Tyler
(2001) to calculate lead deposition rates, the mossbased deposition model can be extended back to
1870. These values can then be compared to the lead
accumulation rates in, e.g., replicate cores from Store
mosse (Bindler et al. 1999, 2004a), which show the
same changes in lead deposition given by the
biomonitoring data over the past 40 years, as well
as the extended moss record back to 1870. Although
within-bog variability of lead accumulation is known
to occur (Bindler et al. 2004a; Coggins et al. 2006),
the close agreement between the long-term peat and
recent moss archives convincingly indicates that the
peat record preserves a close approximation of past
atmospheric lead deposition rates. This would also
Fig. 4 Top panel Lead
accumulation modeled from
the moss monitoring
programs for southern
Sweden (data from ivl.se)
and southern Norway
(Steinnes et al. 2005a),
based on the equation from
(Ruhling and Tyler 2001),
which is extended back to
1870 using moss data from
(Naturvardsverket 1987);
and recent lead
accumulation rates in two
peat cores from Store
mosse, southern Sweden
(Bindler et al. 1999, 2004a).
Lower panel 206Pb/207Pb
ratios in the two peat cores
along with the moss data
from Norway

123

Environ Geochem Health (2011) 33:311329

suggest that the flux rates calculated for the peat


records extending back several millennia (Fig. 2) can
also be considered as a reasonable reflection of the
approximate past deposition rates for lead.
Whereas lead pollution sources from antiquity
through the medieval period and into the early
industrial era are largely constrained within a limited
isotopic field (206Pb/207Pb & 1.161.18), the atmospheric lead pollution during the twentieth century has
entailed more dynamic changes in lead composition.
This is due in large part to the introduction of alkyl
lead in gasoline from the 1930s and the globalization
of the metal industry. A major source of the lead used
in gasoline, for example, has been the Broken Hill
mines in Australia (206Pb/207Pb = 1.04), but also lead
ores from Tunisia, Canada, and many other mining
regions have been utilized. However, because of the
strong reliance on Broken Hill ores as a source for
alkyl-lead additives, there was a common shift in
Europe in the lead isotopic composition, with a
minimum 206Pb/207Pb ratio occurring generally during
the 1980s coinciding with the maximum influence of
gasoline lead emissions (cf. Weiss et al. 1999;
Renberg et al. 2001). Since then, 206Pb/207Pb ratios
have increased and shifted again toward values more
characteristic of European ores and coals.
While industrialization has certainly been of great
consequence for the emission of lead to the

Environ Geochem Health (2011) 33:311329

environment, these emissions must be placed into a


longer context. Over the past 3,500 years, the total
cumulative burden of atmospherically deposited
pollution lead is estimated from the peat and lake
sediment records (as well as in soils, but this is
discussed further on) to be about 25 g Pb m-2 in
southern Sweden and about 1 g Pb m-2 in northern
Sweden (Bindler et al. 1999, 2001; Brannvall et al.
2001a, b; Klaminder et al. 2005, 2006). About half of
this lead was deposited from 3500 BP until AD 1800
and the remainder over the past 200 years. Shotyk
et al. (2000) and Le Roux et al. (2004) have made
similar estimates that 5075% of the anthropogenic
lead was pre-industrial in peat records from Switzerland and Germany. Thus, alkyl lead in gasoline
although a significant source of lead in the mid and
late twentieth centurydoes not account for the
majority of the total amount of pollution lead that has
entered the environment over time, which was the
main assumption in the mass-balance calculation by
Reimann et al. (2008b) to discount these cumulative
pollution lead estimates. When put into a long-term
perspective, gasoline lead is an important, but not the
dominant, source of lead to the environment at least
from a European perspective.

The fate of pollution lead in the boreal forest:


evidence from stable lead isotope analyses
The question then remains as to the fate of this
anthropogenic lead that has been deposited in the
environment in Europe over three millennia [and as
many millennia or more in China (Lee et al. 2008),
and a millennia or more in South America (Abbott
and Wolfe 2003; Cooke et al. 2008)].
The major recipient of atmospheric fallout in
terrestrial systems is the soil. The dominant soil type
in the boreal forest zone is a podzol, which is stratified
into an organic horizon underlain by an eluvial
E-horizon, the illuvial Bs-horizon, which then grades
downward into the largely unaltered parent soil
material in the C-horizon. In contrast to soils affected
by agriculture or significant bioturbation, the O-horizon of boreal soils is characterized by a stratified mortype humus (with L-, F- and H-layers) that exists on
top of the mineral soil with little in-mixing of mineral
grains. The limited mixing between the mor and the
mineral soil makes the elemental chemistry of the mor

319

layer distinct from the mineral soil. That is, for lead,
which is essentially excluded by plant roots (Hovmand et al. 2009), the input is mainly derived from
atmospheric sources in similar fashion to peat. That
only a small fraction of the lead found in the mor layer
is derived from plant uptake has been shown through
various approaches including application of lead
radionuclides (Hovmand et al. 2009) and massbalance calculations based on stable lead isotope
geochemistry (Watmough et al. 2004; Klaminder
et al. 2005, 2008a).
Not surprisingly because of the fundamental
properties of a mor-type humus, the isotopic composition of the mor layer overlaps with that of
atmospheric aerosols (Hopper et al. 1991) and peat
(Bindler et al. 1999; Klaminder et al. 2003) and is
independent of the underlying geological matrix. This
would clearly indicate that the mor layer only
receives inputs of lead from atmospheric fallout.
That the 206Pb/207Pb isotope ratios of the mor layer
are low and are identical to the range of values found
in the upper peat layers covering the past 150 years
(Fig. 5), and quite divorced from the lead composition of the mineral soil, is shown in Fig. 6. For
example, the average 206Pb/207Pb ratio for mor layer
samples from three old-growth forest soil sites in
southern Sweden (Bottnaryd, Hasthult and Norra
Kvill) was 1.150 0.007 [based on a strong acid
extraction, and 1.152 0.004 after total digestion
(Bindler et al. 1999)]; by comparison, the average
206
Pb/207Pb in peat samples covering the past c.
150 years in 6 cores from 4 bogs (Store mosse,
Trollsmosse, Dumme mosse, and Limbergsmosse) in
the same general region of southern Sweden is
1.157 0.010 (Bindler et al. 1999, 2004a). Not only
are the general range of values the same, but also the
stratigraphic changes in 206Pb/207Pb in the mor have
the same pattern as the temporal changes in all of the
environmental archives (Fig. 5). That a temporal
record of past lead deposition is preserved in the mor
reflects the physical characteristics of this type of
organic horizon, and it would not necessarily be
expected that other O-horizon types would retain a
chronological record.
Below the O-horizon, the lead isotopic composition changes in the Swedish forest soils, as exemplified by 206Pb/207Pb ratios increasing downward
through the E-horizon and B-horizon and reaching
consistently high values in the parent C-horizon

123

320

Fig. 5 Vertical changes in 206Pb/207Pb ratios in three mor-type


humus O-horizons (Brannvall et al. 2001b) in comparison with
the temporal changes in 206Pb/207Pb ratios in 3 peat records
from southern Sweden (Bindler et al. 1999), 2 varved lake
sediment records from northern Sweden (Brannvall et al.

Environ Geochem Health (2011) 33:311329

1999), herbaria mosses from Scotland (Farmer et al. 2002) and


forest mosses (Steinnes et al. 2005a), and ice (Rosman et al.
2000), peat and herbaria (Weiss et al. 1999) from Switzerland
and the Alps

Fig. 6 Temporal changes


in the 206Pb/207Pb ratios in
Swedish lake sediments
(left) (Brannvall et al.
2001a) and the stratigraphic
changes in the 206Pb/207Pb
ratio in 12 podzol soil
profiles from southern and
northern Sweden (Brannvall
et al. 2001b), along with the
206
Pb/207Pb composition of
alkyl lead and industrial/
historical ore lead in
Europe, soil mor layers (11
sites) and the surface layers
of six ombrotrophic bogs
(see references cited in the
aforementioned papers)

below 50 cm depth. The same isotopic patterns are


observed in forest soils from Norway (Steinnes et al.
2005b) and Canada (Watmough et al. 2004), which
are similarly derived from older Precambrian bedrocks. In the largely unaltered C-horizon, the lead
composition has 206Pb/207Pb ratios from 1.3 to [3.0
and lead concentrations of 510 lg Pb g-1, which are
the value ranges for sediments [3,500 years old in

123

Swedish lakes (Fig. 6). In the upper weathered part of


the mineral soil, the isotopic composition of the bulk
soil in relation to the parent material is altered by
atmospherically derived lead leached from the mor
layer and transport downward along with particulate
and colloidal organic matter (Dorr and Munnich
1991; Wang and Benoit 1997; Watmough et al. 2004;
Klaminder et al. 2006), as well as by the selective

Environ Geochem Health (2011) 33:311329

weathering of soil minerals (Erel et al. 1994;


Harlavan and Erel 2002).
The lead isotopic composition of the parent soil
material is also further complicated by the fact that in
formerly glaciated areas such as Sweden soil mineralogy can be quite complex as a result of glacial
transport of material from a mixture of local and
distant sources. As an example, in analyzing the lead
isotopic composition of different rock types found
within the mineral soil from a forest podzol from
northern Sweden, we had found that the different
parent rocks had 206Pb/207Pb isotope ratios ranging
from 1.29 to 2.31 after digestion with strong acids,
but which were somewhat lower, 1.231.45, after
extraction with weak acid (acetic acid) (Klaminder
et al. 2005). This difference is well-known and
related to the typically higher uranium content in
more resistant minerals such as zircon, which thus
develop higher ratios in contrast to more easily
weathered accessory minerals, such as carbonates and
potassium feldspar (Shirahata et al. 1980; Erel et al.
2004).
The vertical stratigraphy in the lead isotopic
composition in the soils shows many parallels to
the temporal trends in lake sediments, where both
show high 206Pb/207Pb isotope ratios and low lead
concentrations in deeper layers and declining ratios
and increasing concentrations toward the surface
layers. The soil profiles, of course, do not strictly
speaking represent a chronological record; rather, the
lead isotope profiles are produced by the same longterm loading of an additional lead source with a low
206
Pb/207Pb ratio, but where the lead composition is
governed by a downward migration of lead together
with organic matter.
Given that the geology (e.g., bedrock types and
ages, glacial history, age and type of soils), climate,
and even forest types (frequently coniferous dominated) may be quite similar between many areas of
northern North America and Scandinavia, it is
interesting to compare and contrast the results of
the different studies on lead isotopic composition and
biogeochemistry. While the results are mostly similar, Steinnes and Friedland (2005) observed that one
contrasting aspect is the greater depth observed for
the lowered 206Pb/207Pb ratios in the mineral soil of
Scandinavian soils, which could be explained by the
much longer history of atmospheric lead pollution in
Europe in comparison with the much shorter history

321

of pollution in North America. This increased depth


in the mineral soils for lower isotope ratios also
indicates a greater total accumulation of pollutant
lead in the mineral soil at the Scandinavian sites,
where 2575% of the estimated total inventory of
pollution lead has accumulated in the B-horizon.
The influence of plant uptake and recycling
of lead for surface soils
Studies of lead uptake by spruce in soils spiked with
lead have shown that lead is largely excluded at the
roots and that the uptake of lead into the wood and
especially the canopy (i.e., needles) is minimal
(Hagemeyer and Hubner 1999; Klaminder et al.
2008b; Hovmand et al. 2009). In their study using
soils spiked with 210Pb, Hovmand et al. calculated
that\2% of the lead in twigs and needles was derived
from soil uptake and thus [98% was taken up from
atmospheric deposition. From isotopic analyses of the
lead composition of a range of forest plants including
the major tree types (birch, pine, and spruce) and
field-layer plants (e.g., bilberry, lingon, heather,
crowberry, and juniper), we had previously estimated
that from 10 to 30% of the lead in the roots and
stemwood could be derived from uptake of mineral
soil lead while the rest of the root Pb is derived from
uptake in the mor (Bindler et al. 2004b; Klaminder
et al. 2005). Watmough et al. (2004) likewise
concluded that plant uptake from the soil represented
an insignificant component of the lead cycle, which
they based on experimental addition of 207Pb as a
tracer in the forest floor.
However, regardless of whether the source of the
lead in plants is derived from atmospheric or geogenic
sources, the amount of lead in the plants is extremely
low, typically \0.2 lg Pb g-1. Forest vegetation
contributes very little to the total mass balance of
pollution lead in the boreal forest. For example, in a
mature forest site from northern Sweden, we calculated that the total inventory of lead in the vegetation
was only 1 mg Pb m-2 as compared to an estimated
total pollution inventory in the soil of 700 mg Pb m-2
(Klaminder et al. 2005). Based on an isotopic
partitioning model for lead in the forest plants at this
site, the annual uptake of lead from the mineral soil
site was B0.04 mg Pb m-2 year-1 (Klaminder et al.
2005, 2008b), which is similar to the estimated natural
background deposition rates estimated from the peat

123

322

records, 0.0010.03 lg Pb m-2 year-1. Using their


modeling approach based on 210Pb uptake in spruce in
an experimental plot, Hovmand et al. (2009) calculated an uptake of lead that was an order of magnitude
lower, 0.002 mg Pb m-2 year-1; they estimated that
the internal recycling of lead represented only
0.040.13% of the total lead soil flux.

Contrasting patterns for lead in proximity


to a major industrial emission source
The temporal trends in lake sediments and peat and
the vertical stratigraphy of lead in soils discussed thus
far represent a general pattern for a widespread
number of sites in southern and northern Sweden,
which are removed from major point sources. That is,
these sites receive diffuse inputs from a combination
of long-range sources as well as diffuse regional
sources that would include smaller industries and car
emissions, for example. Below is an example of a
local point source that interferes with the general
pattern observed elsewhere Sweden described in the
above sections.
On Swedens northeastern coast along the Gulf of
Bothnia is the large copper smelter, Ronnskar, which
has been Swedens largest point pollution source. The
smelter began operation in 1930 originally to process
copper from the metal-sulfide ores of the Skellefte
district, but from the mid-1940s and from the late
1960s sulfide ores from Laisvall and Malmberg,
respectively, were also processed at Ronnskar. The
206
Pb/207Pb ratios of these ores are typically around
1.00, 1.311.35, and 1.361.46, respectively. Emissions of lead and many other metals expanded rapidly
and peaked around 1970 after which time-improved
technologies were added to reduce emissions from
the facility. In geochemical surveys of mosses, soil
O-horizons, and lake sediments, the influence of
Ronnskar on the distribution of metals is pronounced
(Fig. 3). The detectable range of influence is about
80 km from the smelter, beyond which the emissions
from the smelter merge with the broader background
atmospheric contamination. Based on studies of
similar large-scale smelters, such as in Canada, it
can be assumed that this observable pollution gradient extending up to * 100 km from the smelter is
connected with particulate emissions and deposition
(Sim et al. 1999).

123

Environ Geochem Health (2011) 33:311329

In a peat record from Vorrmyran, a mire located in


a forest setting 12 km from the smelter, we found a
pattern for the lead isotopic composition that contrasted with the general pattern found at other sites in
southern and northern Sweden (Klaminder et al.
2008b). As with peat cores from other parts of Sweden
and Europe, the concentration of lead in deeper layers
of the mire is quite low, \5 lg Pb g-1, and by the
1970s, the concentration in the peat was as its highest,
575 lg Pb g-1. As can be expected based on the
metal-sulfide ores processed at Ronnskar, there are a
wide range of other metals that increase along with
lead, such as copper, iron, zinc, and most notably
arsenic. Unlike sites from other parts of Sweden,
however, the temporal changes in lead isotopic
composition (Fig. 7) show a contrasting pattern with
the lowest 206Pb/207Pb ratios (1.121.14) occurring
during the first half of the twentieth century when
mining in the Skellefte field expanded and the smelter
came on line in 1930. Shortly, thereafter, the isotope
ratio begins to increase gradually until the late 1960s,
after which the ratio increases rapidly to maximum
values of about 1.25 in the late 1980searly 1990s.
These temporal shifts in isotopic composition are in
accordance with the known changes in the ores
processed at the smelter, which included ores from
Laisvall and Malmberg.
In a series of soil profiles collected from 2 to
100 km distant from the Ronnskar smelter, we
measured lead concentrations of 6,00010,000 lg
Pb g-1 in mor samples 2 km from the smelter, which
at a distance of 1217 km declines by an order of
magnitude to 4501,000 lg Pb g-1. By 80100 km,
the mor lead concentration, 40100 lg Pb g-1, is
typical of forest sites elsewhere in central and
northern Sweden. This soil transect away from
Ronnskar is valuable because it is possible to trace
not only concentration changes but also the influence
of a specific site on the soil lead isotopic composition,
because of the unique lead isotopic composition of the
ores involved. For the two nearest sites at 2 and 17 km
away from the smelter (Fig. 7), the lowest 206Pb/207Pb
ratios are 1.071.10, which occur at or just above the
transition between the organic horizon and the
mineral soil. Within the mor layer, the ratio increases
to 1.21, which is only slightly lower than the
maximum ratio of 1.25 in the Vorrmyran peat record
in the late 1980s. Like the peat record, the 206Pb/207Pb
ratio declines again in the top 12 samples for each

Environ Geochem Health (2011) 33:311329

323

Fig. 7 Lead concentrations and 206Pb/207Pb ratios in 3 soil mor layers located 3, 60 and 100 km away from the Ronnskar smelter
(left panels) and lead accumulation and 206Pb/207Pb ratio in the Vorrmyran peat record 12 km from Ronnskar (right panels)

site. This stratigraphic pattern is only slightly discernable 60 and 80 km away, with a smaller increase
to 1.20 at the more distant of the two sites. However,
at 100 km, the isotopic profile within the mor is
similar to other sites in southern and northern Sweden
(Fig. 5). This provides further validation for the use of
lead isotope analyses as a tool to trace anthropogenic
lead. Similar work of this type using lead isotope
analyses to trace the influence of smelters has been
done, for example, in Canada (Sim et al. 1999;
Simonetti et al. 2000, 2004).

Implications for environmental health


The main focus of our research involving lead has
been on the recent and long-term temporal record of
lead deposition and its implications for biogeochemical cycling in the environment today. Only to a
lesser extent have issues specific to environmental
health been studied. In the vicinity of the Ronnskar
smelter in northern Sweden, Berglund et al. (2009)
assessed the changes in lead uptake in pied flycatchers, which is a bird species that has been used to
monitor metal contamination, as well as used lead

isotopes to trace the sources of lead in their diet.


Emissions from the Ronnskar smelter have declined
by as much as 98% since the early 1980sa decline
that is well documented in the Swedish biomonitoring
program of forest mosses discussed earlier. During
the 1980s, studies showed that there was a clear link
with reduced reproductive success (e.g., clutch size
and nestling survival) and higher metal concentrations along this gradient. Increased blood lead
concentrations have been correlated with reduced
hematocrit and Hb levels and reduced q-aminolevulinic acid dehydratase activities in birds (Berglund
2010).
Despite the greatly reduced metal emissions at
Ronnskar, soil lead concentrations have changed little
over this time period because of the slow overturn of
soil organic matter in the colder northern climate, and
the past deposition gradient from the smelter is still
clearly displayed both in terms of lead concentrations
and stable lead isotopes as discussed in the previous
section (Klaminder et al. 2008b). The main question
addressed by Berglund et al. was whether reduced
emissions have led to reductions in contamination
levels for the pied flycatcher, or whether the
unchanged soil levels still affect the bird population.

123

324

Much of the diet of the pied flycatcher is


composed of soil-living biota such as ants. Lead
isotope analyses of these food sources showed that
they have 206Pb/207Pb ratios comparable to the soil
O-horizons in which they live, with the ants and soils
both having ratios in the range of 1.141.18 (Berglund et al. 2009). In contrast, the 206Pb/207Pb ratio of
recent lead deposition in closer proximity to the
smelter as measured in forest mosses is lower, about
1.11. Analyses of liver and feces samples from the
birds showed 206Pb/207Pb ratios in the same range as
the ants and O-horizon rather than values in recent
deposition; furthermore, the liver analyses showed
only a slight improvement in lead levels with
reductions of 915% from the late 1980s to
20002006. Lead analyses of the feces showed
somewhat higher reductions in lead of 1840%,
which were still well below the 98% reduction in
emissions. The poor response in lead levels in pied
flycatchers near Ronnskar can be attributed to the
extremely high soil metal contamination levels,
where lead concentrations in the O-horizon are in
the range of 2,0007,000 lg g-1, as are the concentrations of copper and zinc. In other areas such as
Harjavalta, Finland, where emissions from a copper
smelter have likewise declined sharply but where the
cumulative burden in soils is about an order of
magnitude lower than at Ronnskar, pied flycatcher
populations have experienced 9095% reductions in
lead levels, i.e., comparable to the reductions in metal
emissions (Eeva and Lehikoinen 2000).
While pollution gradients surround smelters reflect
an extreme situation, research elsewhere in Sweden
has focused on the effects of the ambient contamination levels, which result from diffuse long-range
atmospheric transport, on microbial activity in boreal
kerblom
forest soils (e.g., Bringmark et al. 1998; A
et al. 2010). This research in both laboratory and field
settings has indicated that there can be negative
effects on microbial respiration at levels of about
225 lg Pb g-1. However, results from field studies
are complicated by the presence of a suite of other
contaminant metals in soils, such as mercury and
cadmium, which also may contribute to the observed
responses. Isolating the specific effects of lead
contamination alone from the range of other contaminants present in the natural environment is a difficult
task, and it is likely that the synergistic effects of
multiple contaminants are the most important.

123

Environ Geochem Health (2011) 33:311329

A further difficulty in these studies aimed at


assessing the negative effects of metal contamination
on the natural environment is the choice of reference
conditions to be used for comparison, which are
typically chosen based on the lowest concentrations
typically found in undisturbed forest soils, such as
those in remote areas of northern Scandinavia. While
this choice of reference conditions is obvious for
field-based studies, these values are also transferred
to laboratory studies as well. But, as discussed earlier
with regard to peat records of past lead deposition, it
may be the case that true natural background lead
levels in soil organic horizons were one or even two
orders of magnitude lower than the background
contamination levels used in these soils studies,
2545 lg Pb g-1 rather than estimated natural lead
levels of 0.11.0 lg Pb g-1 (Bindler et al. 1999;
Klaminder et al. 2006).

Conclusions
Lead concentrations in soils and vegetation in
northern Scandinavia are generally much lower
than in mainland Europe; and until the 1990s, it
was assumed that these values were an approximation of natural or background conditionsa
belief still deeply rooted among the general public
and some scientists. However, Clair Patterson and
colleagues demonstrated already four decades ago
that the lead cycle was greatly altered on a global
scale by humans, and that theses changes began
already a few thousand years ago, which is well
supported from subsequent studies of lead in lake
sediment, peat, and ice records. Patterson and
colleagues also developed stable lead isotope analyses as a tool to differentiate between natural and
pollution-derived lead. Since then, stable isotope
analyses of sediment, peat, herbaria collections,
soils, and forest plants have given us new insights
into lead biogeochemical cycling in space and time.
Three important conclusions from our studies in
Sweden, which are well supported by extensive
results from other parts of Europe and from North
America are:
(1)

Lead deposition rates at sites removed from


major point sources during the twentieth century
were about 1,000 times higher than a few

Environ Geochem Health (2011) 33:311329

(2)

(3)

(4)

thousand years ago, and today are still almost


100 times greater than natural rates. This
estimated increase in deposition over time is
similar to the estimated changes in body
burdens of lead from ancient times to the
twentieth century (Ericson et al. 1975; Settle
and Patterson 1980). Only a very small fraction
of the increased deposition can be attributed to
increased soil dust fluxes.
Stable lead isotopes (206Pb/207Pb ratios discussed here) are an effective tool to separate
anthropogenic lead from the lead naturally
present in sediments, peat, and soils for both
the majority of sites receiving diffuse inputs
from long range and regional sources and for
sites in close proximity to point sources. Using
lead isotopes, we can trace not only changes in
the sources of lead over time, but also the fate of
this lead in the environment.
Using stable lead isotopes, we have estimated
that in southern Sweden the cumulative anthropogenic burden of atmospherically deposited
lead is *25 g Pb m-2 and *1 g Pb m-2 in the
pristine north. Steinnes and Friedland (2005)
have made similar estimates for Norwegian
soils. Half of this cumulative total was deposited before industrialization.
Although not discussed but of importance for
future assessments, predicted recovery rates for
soils in the cold climate of Scandinavia are slow;
we have estimated that the soil surface (Ohorizon), where most soil biota reside, retains
lead deposited over the past 150500 years.
Surface soils in more temperate climates are
predicted to respond to changes in deposition
over somewhat shorter timescales, c.
1580 years (Miller and Friedland 1994).

Acknowledgments Although I take sole responsibility for


the contents and writing of this paper, I nonetheless benefited
greatly from the direct or indirect help of Jonatan Klaminder,
Johan Rydberg, and Antonio Martnez Cortizas during the
writing process. Most of the original research cited in this
paper also involved Ingemar Renberg, Maja-Lena Brannvall,
and in the laboratory Ove Emteryd. I would also like to thank
the organizers of the 2010 SEGH meeting in Galway, Ireland,
for the invitation to submit a more extensive written version of
a brief presentation. The revised manuscript also benefited
from the helpful suggestions of two anonymous reviewers.

325

References
Abbott, M. B., & Wolfe, A. P. (2003). Intensive pre-Incan
metallurgy recorded by lake sediments from the Bolivian
Andes. Science, 301, 18931895.
kerblom, S., Bringmark, L., & Nilsson, M. (2010). Organic
A
matter control of mercury and lead toxicity in mor layers.
Ecotoxicology and Environmental Safety, 73(5), 924931.
Alriksson, A. (2001). Regional variability of cd, hg, pb and c
concentrations in different horizons of swedish forest
soils. Water, Air and Soil Pollution: Focus, 1, 325341.
Bacon, J. R., Berrow, M. L., & Shand, C. A. (1995). Isotopic
characterization of lead in the Scottish upland environment. International Journal of Environmental Analytical
Chemistry, 59, 253264.
Bacon, J. R., Farmer, J. G., Dunn, S. M., Graham, M. C., &
Vinogradoff, S. I. (2006). Sequential extraction combined
with isotope analysis as a tool for the investigation of lead
mobilisation in soils: Application to organic-rich soils in
an upland catchment in Scotland. Environmental Pollution, 141, 469481.
Bacon, J. R., Jones, K. C., McGrath, S. P., & Johnston, A. E.
(1996). Isotopic character of lead deposited from the
atmosphere at a grassland site in the United Kingdom
since 1860. Environmental Science and Technology, 30,
25112518.
Baron, S., Lavoie, M., Ploquin, A., Carignan, J., Pulido, M., &
De Beaulieu, J.-L. (2005). Record of metal workshops in
peat deposits: History and environmental impact on the
Mont Loze`re Massif, France. Environmental Science and
Technology, 39, 51315140.
Baron, S., Le-Carlier, C., Carignan, J., & Ploquin, A. (2009).
Archaeological reconstruction of medieval lead production: Implications for ancient metal provenance studies
and paleopollution tracing by Pb isotopes. Applied Geochemistry, 24(11), 20932101.
Berg, T., & Steinnes, E. (1997). Use of mosses (Hylocomium
spendens and Pleurozium screberi) as biomonitors of
heavy metal deposition: From relative to absolute deposition values. Environmental Pollution, 98, 6171.
Berglund, A. M. M. (2010). Responses to reduced industrial metal
emissions. PhD dissertation, Umea University, Umea.
Berglund, A. M. M., Klaminder, J., & Nyholm, N. E. I. (2009).
Effects of reduced lead deposition on pied flycatchers
(Ficedula hypoleuca) nestlings: Tracing exposure routes
using stable lead isotopes. Environmental Science and
Technology, 43, 208213.
Biester, H., Bindler, R., Martnez Cortizas, A., & Engstrom, D.
R. (2007). Modeling the past atmospheric deposition of
mercury using natural archives. Environmental Science
and Technology, 41, 48514860.
Bindler, R. (2008). Comment on The biosphere: A homogeniser of Pb-isotope signals By C. Reimann, B. Flem, A.
Arnoldussen, P. Englmaier, T.E. Finne, F. Koller and .
Nordgulen. Applied Geochemistry, 23, 25192526.
Bindler, R., Brannvall, M.-L., Renberg, I., Emteryd, O., &
Grip, H. (1999). Natural lead concentrations in pristine
boreal forest soils and past pollution trends: A reference

123

326
for critical load models. Environmental Science and
Technology, 33, 33623367.
Bindler, R., & Klaminder, J. (2006). Beyond the peat: Synthesizing peat, lake sediments and soils in studies of the
Swedish environment. In I. P. Martini, A. Martnez Cortizas, & W. Chesworth (Eds.), Peatlands: Evolution and
records of environmental and climate changes (pp.
431448): Elsevier, Amsterdam.
Bindler, R., Klarqvist, M., Klaminder, J., & Forster, J. (2004).
Does within-bog spatial variability of mercury and lead
constrain reconstructions of absolute atmospheric deposition rates from single peat records? The example of
Store mosse. Global Biogeochemical Cycles, 18, GB3020.
doi 3010.1029/2004GB002270.
Bindler, R., Renberg, I., Brannvall, M.-L., Emteryd, O., & ElDaoushy, F. (2001). A whole-basin study of sediment
accumulation using stable lead isotopes and flyash particles in an acidified lake, Sweden. Limnology and
Oceanography, 46(1), 178188.
Bindler, R., Renberg, I., Klaminder, J., & Emteryd, O. (2004b).
Tree rings as Pb pollution archives? A comparison of
206
Pb/207Pb isotope ratios in pine and other environmental
media. The Science of The Total Environment, 319,
173183.
Bindler, R., Renberg, I., Rydberg, J., & Andren, T. (2009).
Widespread waterborne pollution in central Swedish lakes
and the Baltic sea from pre-industrial mining and metallurgy. Environmental Pollution, 157, 21322141.
Brannvall, M.-L., Bindler, R., Emteryd, O., & Renberg, I.
(2001a). Four thousand years of atmospheric lead pollution in northern Europe: A summary from Swedish lake
sediments. Journal of Paleolimnology, 25, 421435.
Brannvall, M.-L., Bindler, R., Emteryd, O., & Renberg, I.
(2001b). Vertical distribution of atmospheric pollution
lead in Swedish boreal forest soils. Water, Air, and Soil
Pollution: Focus, 1, 357376.
Brannvall, M.-L., Bindler, R., Renberg, I., Emteryd, O.,
Bartnicki, J., & Billstrom, K. (1999). The medieval metal
industry was the cradle of modern large-scale atmospheric
lead pollution in northern Europe. Environmental Science
and Technology, 33, 43914395.
Brill, R. H., & Wampler, J. M. (1967). Isotope studies of
ancient lead. American Journal of Archaeology, 71,
6377.
Bringmark, L., Bringmark, E., & Samuelsson, B. (1998).
Effects on mor layer respiration by small experimental
additions of mercury and lead. Science of the Total
Environment, 213, 115119.
Brown, J. S. (1962). Ore leads and isotopes. Economic Geology, 57, 673720.
Chow, T. J. (1965). Radiogenic leads of the Canadian and
Baltic shield regions. Symposium Marine Geochemistry,
3, 169184.
Chow, T. J., & Patterson, C. C. (1962). The occurrence and
significance of lead isotopes in pelagic sediments. Geochimica et Cosmochimica Acta, 26, 263308.
Cloy, J. M., Farmer, J. G., Graham, M. C., MacKenzie, A. B.,
& Cook, G. T. (2008). Historical records of atmospheric
Pb deposition in four Scottish ombrotrophic peat bogs: An
isotopic comparison with other records from western
Europe and Greenland. Global Biogeochemical Cycles,

123

Environ Geochem Health (2011) 33:311329


22, Article Number: GB2016. doi:10.1029/2007GB00
3059.
Coggins, A. M., Jennings, S. G., & Ebinghaus, R. (2006).
Accumulation rates of the heavy metals lead, mercury and
cadmium in ombrotrophic peatlands in the west of Ireland.
Atmospheric Environment, 40, 260278.
Cooke, C. A., Abbott, M., & Wolfe, A. P. (2008). LateHolocene atmospheric lead deposition in the Peruvian and
Bolivian Andes. Holocene, 18, 353359.
De Vleeschouwer, F., Ge`rard, L., Goormaghtigh, C., Mattielli,
N., Le Roux, G., & Fagel, N. (2007). Atmospheric lead
and heavy metal pollution records from a Belgian peat
bog spanning the last two millennia: Human impact on a
regional to global scale. Science of the Total Environment,
377, 282295.
Dorr, H., & Munnich, K. O. (1991). Lead and cesium transport
in European forest soils. Water, Air, and Soil pollution,
5758, 809818.
Eeva, T., & Lehikoinen, E. (2000). Pollution: Recovery of
breeding success in wild birds. Nature, 403, 851852.
Ek, A. S., & Renberg, I. (2001). Heavy metal pollution and
lake acidity changes caused by one thousand years of
copper mining at Falun, central Sweden. Journal of Paleolimnology, 26, 89107.
Erel, Y., Blum, J. D., Roueff, E., & Ganor, J. (2004). Lead and
strontium isotopes as monitors of experimental granitoid
mineral dissolution. Geochimica et Cosmochimica Acta,
68, 46494663.
Erel, Y., Harlavan, Y., & Blum, J. D. (1994). Lead isotope
systematics of granitoid weathering. Geochimica et Cosmochimica Acta, 58, 52995306.
Ericson, J. E., Shirahata, H., & Patterson, C. C. (1975). Skeletal
concentrations of lead in ancient peruvians. New England
Journal of Medicine, 300, 949951.
Farmer, J. G., Eades, L. J., Atkins, H., & Chamberlin, D. F.
(2002). Historical trends in the lead isotopic composition
of archival Sphagnum mosses from Scotland
(18382000). Environmental Science and Technology, 36,
152157.
Farmer, J. G., Eades, L. J., & Graham, M. C. (1999). The lead
content and isotopic composition of British coals and their
implications for past and present releases of lead to the
UK environment. Environmental Geochemistry and
Health, 21, 257272.
Farmer, J. G., Eades, L. J., MacKenzie, A. B., Kirika, A., &
Bailey-Watts, T. E. (1996). Stable lead isotope record of
lead pollution in Loch Lomond sediments since 1630 A.D.
Environmental Science and Technology, 30, 30803083.
Faure, G. (1986). Principles of isotope geology (2nd ed.). New
York: Wiley.
Fitzgerald, W. F., Engstrom, D. R., Mason, R. P., & Nater, E.
A. (1998). The case for atmospheric mercury contamination in remote areas. Environmental Science and
Technology, 32, 17.
Graham, M. C., Vinogradoff, S. I., Chipchase, A. J., Dunn, S.
M., Bacon, J. R., & Farmer, J. G. (2006). Using size
fractionation and Pb isotopes to study Pb transport in the
waters of an organic-rich upland catchment. Environmental Science and Technology, 40, 12501256.
Grattan, J. P., Gilbertson, D. D., & Hunt, C. O. (2007). The
local and global dimensions of metalliferous pollution

Environ Geochem Health (2011) 33:311329


derived from a reconstruction of an eight thousand year
record of copper smelting and mining at a desert-mountain frontier in southern Jordan. Journal of Archaeological
Science, 34, 83110.
Grogler, N., Geiss, J., Grunenfelder, M., & Houtermans, F. G.
(1966). Isotopenuntersuchungen zur Bestimmung der
Herkunft romischer Bleirohre und Bleibarren. Naturforschg, 21a, 11671172.
Hagemeyer, J., & Hubner, C. (1999). Radial distributions of Pb
in stems of 6-year-old spruce trees (Picea abies (l.) karst.)
grown for 2 years in Pb-contaminated soil. Water, Air,
and Soil pollution, 111, 215224.
Hamelin, B., Grousset, F., & Sholkovitz, E. R. (1990). Pb
isotopes in surficial pelagic sediments from the North
Atlantic. Geochimica et Cosmochimica Acta, 54, 3747.
Harlavan, Y., & Erel, Y. (2002). The release of Pb and REE
from granitoids by the dissolution of accessory phases.
Geochimica et Cosmochimica Acta, 66, 837848.
Harlavan, Y., Erel, Y., & Blum, J. D. (1998). Systematic
changes in lead isotopic composition with soil age in
glacial granitic terrains. Geochimica et Cosmochimica
Acta, 62, 3346.
Hettwer, K., Deicke, M., & Ruppert, H. (2003). Fens in karst
sinkholesarchives for long lasting immission chronologies. Water, Air, and Soil pollution, 149, 363384.
Hong, S. M., Candelone, J. P., Patterson, C. C., & Boutron, C.
F. (1994). Greenland ice evidence of hemispheric lead
pollution 2 millennia ago by Greek and Roman civilizations. Science, 265, 18411843.
Hopper, J. F., Ross, H. B., Sturges, W. T., & Barrie, L. A.
(1991). Regional source discrimination of atmospheric
aerosols in Europe using the isotopic composition of lead.
Tellus, 43B, 4560.
Hovmand, M. F., Nielsen, S. P., & Johnsen, I. (2009). Root
uptake of lead by Norway spruce grown on 210 Pb spiked
soils. Environmental Pollution, 157, 404409.
Kaste, J. M., Friedland, A. J., & Sturup, S. (2003). Using stable
and radioactive isotopes to trace atmospherically deposited Pb in montane forest soils. Environmental Science
and Technology, 37, 35603567.
Kempter, H., & Frenzel, B. (2000). The impact of early mining
and smelting on the local tropospheric aerosol detected in
ombrotrophic peat bogs in the Harz mountains, Germany.
Water, Air, and Soil pollution, 121, 93108.
Klaminder, J., Bindler, R., Emteryd, O., & Renberg, I. (2005).
Uptake and recycling of lead by boreal forest plants:
Quantitative estimates from a site in northern Sweden.
Geochimica et Cosmochimica Acta, 69, 24852496.
Klaminder, J., Bindler, R., & Renberg, I. (2008a). The biogeochemistry of atmospherically derived Pb in the boreal
forest of Sweden. Applied Geochemistry, 23, 29222931.
Klaminder, J., Bindler, R., Rydberg, J., & Renberg, I. (2008b).
Is there a chronological record of atmospheric mercury
and lead deposition preserved in the mor layer (O-horizon) of boreal forest soils. Geochimica et Cosmochimica
Acta, 72, 703712.
Klaminder, J., Renberg, I., Bindler, R., Appleby, P. G., Emteryd, O., & Grip, H. (2006). Estimating the mean residence time of lead in the mor layer of boreal forest soils
using 210-lead, stable lead and a soil chronosequence.
Biogeochemistry, 78, 3149.

327
Klaminder, J., Renberg, I., Bindler, R., & Emteryd, O. (2003).
Isotopic trends and background fluxes of atmospheric lead
deposition in N Europe: Analyses of three ombrotrophic
bogs from south Sweden. Global Biogeochemical Cycles,
17, art.no.1019.
Kramers, J. D., & Tolstikhim, I. N. (1997). Two terrestrial lead
isotope paradoxes, forward transport modelling, core
formation and the history of the continental crust.
Chemical Geology, 139, 75110.
Kylander, M. E., Klaminder, J., Bindler, R., & Weiss, D. J.
(2010). Natural lead isotope variations in the atmosphere.
Earth and Planetary Science Letters, 290, 4453.
Kylander, M. E., Weiss, D. J., Martinez Cortizas, A., Spiro, B.,
Garcia-Sanchez, R., & Coles, B. J. (2005). Refining the
pre-industrial atmospheric Pb isotope evolution curve in
Europe using an 8000 year old peat core from NW Spain.
Earth and Planetary Science Letters, 240, 467485.
Le Roux, G., Aubert, D., Stille, P., Krachler, M., Kober, B.,
Cheburkin, A., et al. (2005). Recent atmospheric pb
deposition at a rural site in southern Germany assessed
using a peat core and snowpack, and comparison with
other archives. Atmospheric Environment, 39, 67906801.
Le Roux, G., Sonke, J. E., Cloquet, C., Aubert, D., & de
Vleeschouwer, F. (2008). Comment on The biosphere: A
homogeniser of pb-isotope signals By C. Reimann, B.
Flem, A. Arnoldussen, P. Englmaier, T.E. Finne, F. Koller
and . Nordgulen. Applied Geochemistry, 23, 27892792.
Le Roux, G., Weiss, D., Grattan, J. P., Givelet, N., Krachler,
M., Cheburkin, A., et al. (2004). Identifying the sources
and timing of ancient and medieval atmospheric lead
pollution in England using a peat profile from Lindow
Bog, Manchester. Journal of Environmental Monitoring,
6, 502510.
Lee, C. S. L., Qi, S. H., Zhang, G., Luo, C.-L., Zhao, L. Y. L.,
& Li, X.-D. (2008). Seven thousand years of records on
the mining and utilization of metals from lake sediments
in central China. Environmental Science and Technology,
42, 47324738. doi:10.1021/es702990n.
Marshall, W. A., Clough, R., & Gehrels, W. R. (2009). The
isotopic record of atmospheric lead fall-out on an Icelandic salt marsh since ad 50. Science of the Total Environment, 407, 27342748.
Martnez Cortizas, A., Mighall, T., Pontevedra Pombal, X.,
Novoa Munoz, J. C., Peiteado Varela, E., & Pineiro Rebolo, R. (2005). Linking changes in atmospheric dust
deposition, vegetation change and human activities in
northwest Spain during the last 5300 years. Holocene, 15,
698706.
Martnez-Cortizas, A., Biester, H., Mighall, T., & Bindler, R.
(2007). Climate-driven enrichment of pollutants in peatlands. Biogeosciences, 4, 905911.
Martnez-Cortizas, A., Garcia-Rodeja, E., Pontevedra-Pombal,
X., Novoa Munoz, J. C., Weiss, D., & Cheburkin, A.
(2002). Atmospheric Pb deposition in Spain during the
last 4600 years recorded by two ombrotrophic peat bogs
and the implications for the use of peat as archive. Science
of the Total Environment, 292, 3344.
Mighall, T. M., Timberlake, S., Foster, I. D. L., Krupp, E., &
Singh, S. (2009). Ancient copper and lead pollution
records from a raised bog complex in central Wales, UK.
Journal of Archaeological Science, 36, 15041515.

123

328
Miller, E. K., & Friedland, A. J. (1994). Lead migration in
forest soils: response to changing atmospheric inputs.
Environmental Science and Technology, 28, 662669.
Monna, F., Galop, D., Carozza, L., Tual, M., Beyrie, A.,
Marembert, F., et al. (2004a). Environmental impact of
early Basque mining and smelting recorded in a high ash
minerogenic peat deposit. Science of the Total Environment, 327, 197214.
Monna, F., Hamer, K., Leveque, J., & Sauer, M. (2000). Pb
isotopes as a reliable marker of early mining and smelting
in the northern Harz province (Lower Saxony, Germany).
Journal of Geochemical Exploration, 68, 201210.
Monna, F., Petit, C., Guillaumet, J.-P., Jouffroy-Bapicot, I.,
Blanchot, C., Dominik, J., et al. (2004b). History and
environmental impact of mining activity in Celtic Aeduan
territory recorded in a peat bog (Morvan, France). Environmental Science and Technology, 38, 665673.
Murozumi, M., Chow, T. J., & Patterson, C. C. (1969).
Chemical concentrations of pollutant lead aerosols, terrestrial dusts and sea salts in Greenland and Antarctic
snow strata. Geochimica et Cosmochimica Acta, 33,
12471294.
Naturvardsverket (1987). Monitor 1987. Tungmetallerforekomst och omsattning i naturen. (Swedish Environmental
Protection Agency report).
Norton, S. A., & Kahl, J. S. (1991). Progress in understanding
the chemical stratigraphy of metals in lake sediments in
relation to acidic precipitation. Hydrobiologia, 214,
7784.
Nriagu, J. O. (1983). Lead and lead poisoning in antiquity. NY,
USA: Wiley-Interscience.
Nriagu, J. O. (1996). Pollution caused by heavy metals can be
traced back to the Roman Empire. Science, 272, 223.
Patterson, C. (1965). Contaminated and natural environments
of man. Archives of Environmental Health, 11, 344360.
Patterson, C. C. (1971). Native copper, silver, and gold
accessible to early metallurgists. American Antiquity, 36,
286321.
Patterson, C. C. (1972). Silver stocks and losses in ancient and
medieval times. Economic History Review, 25, 205234.
Patterson, C. C., & Hirao, Y. (1974). Lead aerosol pollution in
the high sierras overrides natural mechanisms which
exclude lead from a food chain. Science, 184, 989992.
Patterson, C. C., Tilton, G. R., & Inghram, M. (1955). Age of
the earth. Science, 212, 6975.
Postan, M. M., & Miller, E. (1987). The Cambridge Economic
History of Europe. II. Trade and Industry in the Middle
Ages (2nd ed). Cambridge University Press.
Rasmussen, P. E. (1994). Current methods of estimating
atmospheric mercury fluxes in remote areas. Environmental Science and Technology, 28, 22332241.
Reimann, C., Englmaier, P., Flem, B., Gough, L., Lamothe, P.,
Nordgulen, ., et al. (2009a). Geochemical gradients in
soil O-horizon samples from southern Norway: Natural or
anthropogenic? Applied Geochemistry, 24, 6276.
Reimann, C., Englmaier, P., Flem, B., Gough, L., Lamothe, P.,
Nordgulen, ., et al. (2009b). Reply to the comment on
Geochemical gradients in soil O-horizon samples from
southern Norway: Natural or anthropogenic? By E.
Steinnes. Applied Geochemistry, 24, 20232025.

123

Environ Geochem Health (2011) 33:311329


Reimann, C., Flem, B., Arnoldussen, A., Englmaier, P., Finne,
T. E., Koller, F., et al. (2008a). Reply to the comment on
The biosphere: A homogenizer of Pb-isotope signals
By G. Le Roux, J. Sonke, C. Cloquet, D. Aubert, and F.
De Vleeschouwer. Applied Geochemistry, 23, 27932798.
Reimann, C., Flem, B., Arnoldussen, A., Englmaier, P., Finne,
T. E., Koller, F., et al. (2008b). Reply to the comments on
The biosphere: A homogenizer of Pb-isotope signals by
R. Bindler and W. Shotyk. Applied Geochemistry, 23,
25272535.
Reimann, C., Flem, B., Arnoldusson, A., Englmaier, P., Finne,
T. E., Koller, F., et al. (2008c). The biosphere: A homegeniser of Pb-isotope signals. Applied Geochemistry, 23,
705722.
Renberg, I., Bindler, R., & Brannvall, M.-L. (2001). Using the
historical atmospheric lead deposition record as a chronological marker in sediment deposits in Europe. Holocene, 11, 511516.
Renberg, I., Brannvall, M.-L., Bindler, R., & Emteryd, O.
(2000). Atmospheric lead pollution history during four
millennia (2000 BC to 2000 AD) in Sweden. Ambio, 29,
150156.
Renberg, I., Wik-Persson, M., & Emteryd, O. (1994). Preindustrial atmospheric lead contamination detected in
Swedish lake sediments. Nature, 368, 323326.
Rosman, K. J. R., Chisholm, W., Hong, S. M., Candelone, J. P.,
& Boutron, C. F. (1997). Lead from Carthaginian and
roman Spanish mines isotopically identified in Greenland
ice dated from 600 bc to 300 ad. Environmental Science
and Technology, 31, 34133416.
Rosman, K. J. R., Ly, C., van de Velde, K., & Boutron, C. F.
(2000). A two century record of lead isotopes in high
altitude alpine snow and ice. Earth and Planetary Science
Letters, 176, 413424.
Ross, H. B. (1990). On the use of mosses (Hylocomium
splendens and Pleurozium schreberi) for estimating
atmospheric trace metal deposition. Water, Air, and Soil
pollution, 50, 6376.
., & Tyler, G. (2001). Changes in atmospheric
Ruhling, A
deposition rates of heavy metals in Sweden. A summary
of nationwide Swedish surveys in 1968/701995. Water,
Air and Soil Pollution: Focus, 1, 311323.
Settle, D., & Patterson, C. C. (1980). Lead in albacore: Guide
to lead pollution in Americans. Science, 207, 11671176.
Shirahata, H., Elias, R. W., & Patterson, C. C. (1980). Chronological variations in concentrations and isotopic compositions of anthropogenic atmospheric lead in sediments
of a remote subalpine pond. Geochimica et Cosmochimica
Acta, 44, 149162.
Shotyk, W. (2008). Comment on The biosphere: A homogeniser of pb-isotope signals by C. Reimann, B. Flem, A.
Arnoldussen, P. Englmaier, T.E. Finne, F. Koller and .
Nordgulen. Applied Geochemistry, 23, 25142518.
Shotyk, W., Blaser, P., Grunig, A., & Cheburkin, A. K. (2000).
A new approach for quantifying cumulative, anthropogenic, atmospheric lead deposition using peat cores from
bogs: Pb in eight swiss peat bog profiles. Science of the
Total Environment, 249, 281295.
Shotyk, W., Weiss, D., Appleby, P. G., Cheburkin, A. K., Frei,
R., Gloor, M., et al. (1998). History of atmospheric lead

Environ Geochem Health (2011) 33:311329


deposition since 12,370 14C yr BP from a peat bog, Jura
Mountains, Switzerland. Science, 281, 16351640.
Shotyk, W., Weiss, D., Kramers, J. D., Frei, R., Cheburkin, A.
K., Gloor, M., et al. (2001). Geochemistry of the peat bog
at Etang de la Grue`re, Jura Mountains, Switzerland, and
its record of atmospheric Pb and lithogenic trace metals
(Sc, Ti, Y, Zr, and REE) since 12,370 14C yr BP. Geochimica et Cosmochimica Acta, 65, 23372360.
Sim, B. L., Agterberg, F. P., & Beaudry, C. (1999). Determining the cutoff between background and relative base
metal smelter contamination levels using multifractal
methods. Computational Geosciences, 25, 10231041.
Simonetti, A., Gariepy, C., Banic, C. M., Tanabe, R., & Wong,
H. K. (2004). Pb isotopic investigation of aircraft-sampled
emissions from the Horne smelter (Rouyn, Quebec):
Implications for atmospheric pollution in northeastern
North America. Geochimica et Cosmochimica Acta, 68,
32853294.
Simonetti, A., Gariepy, C., & Carignan, J. (2000). Pb and Sr
isotopic compositions of snowpack from Quebec, Canada:
Inferences on the sources and deposition budgets of
atmospheric heavy metals. Geochimica et Cosmochimica
Acta, 64, 520.
Steinnes, E. (2009). Comment on Geochemical gradients in
soil O-horizon samples from southern norway: Natural or
anthropogenic? by C. Reimann, P. Englmaier, B. Flem,
L. Gough, P. Lamothe, . Nordgulen, and D. Smith.
Applied Geochemistry, 24, 20192022.
berg, G., & Hjelmseth, H. (2005a). Atmospheric
Steinnes, E., A
deposition of lead in Norway: Spatial and temporal

329
variation in isotopic composition. Science of the Total
Environment, 336, 105117.
Steinnes, E., & Friedland, A. J. (2005). Lead migration in
podzolic soils from Scandinavia and the United States of
America. Canadian Journal of Soil Science, 85, 291294.
Steinnes, E., Sjbakk, T. E., Donisa, C., & Brannvall, M. L.
(2005b). Quantification of pollutant lead in forest soils.
Soil Science Society of America Journal, 69, 13991404.
Stos-Gale, Z., Gale, N. H., Houghton, J., & Speakman, R.
(1995). Lead isotope data from the isotrace laboratory,
oxford: Archaeometry data base 1, ores from the western
Mediterranean. Archaeometry, 37, 407415.
Wang, E. X., & Benoit, G. (1997). Fate and transport of contaminant lead in spodosols: A simple box model analysis.
Water, Air, and Soil pollution, 95, 381397.
Watmough, S. A., & Dillon, P. J. (2007). Lead biogeochemistry in
a central Ontario watershed. Biogeochemistry, 84, 143159.
Watmough, S. A., Hutchinson, T. C., & Dillon, P. J. (2004).
Lead dynamics in the forest floor and mineral soil in
south-central Ontario. Biogeochemistry, 71, 4368.
Weiss, D., Shotyk, W., Kramers, J. D., & Gloor, M. (1999).
Sphagnum mosses as archives of recent and past atmospheric lead deposition in Switzerland. Atmospheric
Environment, 33, 37513763.
Zheng, J., Shotyk, W., Krachler, M., & Fisher, D. A. (2007). A
15,800-year record of atmospheric lead deposition on the
Devon Island ice cap, Nunavut, Canada: Natural and
anthropogenic enrichments, isotopic composition and
predominant sources. Global Biogeochemical Cycles, 21,
GB2027. doi:2010.1029/2006GB002897.

123

Reproduced with permission of the copyright owner. Further reproduction prohibited without permission.