atmospheric deposition of lead in norway: spatial and temporal variation in isotopic composition

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Science of the Total Environment 336 (2005) 105–117

Atmospheric deposition of lead in Norway:

spatial and temporal variation in isotopic composition

E. Steinnesa,b,*, G. Abergb, H. Hjelmsethb

aDepartment of Chemistry, Norwegian University of Science and Technology, NO-7491 Trondheim, Norwayb Institute for Energy Technology, NO-2027 Kjeller, Norway

Received 5 February 2004; received in revised form 29 April 2004; accepted 30 April 2004

Abstract

Moss samples collected from 22 sites all over Norway at five different times during 1977–2000 were analysed for stable

lead isotope ratios. These data together with total lead concentrations and relevant literature lead isotope data from UK, western/

central Europe and eastern Europe/Russia were used to elucidate major source regions for lead deposited in different parts of the

country at different times. The southernmost part of the country was most affected from western/central Europe around 1975,

but the deposition declined rapidly and UK became a more significant source region in the 1980s. Recently, the influence is

mostly from Eastern Europe. In the west, UK was the dominant source region during the whole period. In the middle and

northern regions, the deposition was low but also decreasing regularly, and the main source region was probably the North

Atlantic. In the far north–east, influence from Russia and eastern Europe was dominant during the whole period.

D 2004 Published by Elsevier B.V.

Keywords: Atmospheric lead; Stable lead isotopes; Moss; Norway; Transboundary pollution; Temporal trends

1. Introduction been strongly affected (Steinnes et al., 1992, 1994).

Studies over the last 25 years have shown that

terrestrial ecosystems all over Norway have been

contaminated moderately to strongly by lead and other

trace elements from atmospheric deposition (Steinnes,

2001). Long-range transport from other parts of

Europe appears to be the main reason for this exten-

sive lead contamination (Amundsen et al., 1992), and

especially the southernmost part of the country has

0048-9697/$ - see front matter D 2004 Published by Elsevier B.V.

doi:10.1016/j.scitotenv.2004.04.056

* Corresponding author. Department of Chemistry, Norwegian

University of Science and Technology, NO-7491 Trondheim,

Norway. Tel.: +47-73-59-62-37; fax: +47-73-55-08-77.

E-mail address: [email protected] (E. Steinnes).

Since the initial measurements in the 1970s (Hanssen

et al., 1980; Steinnes, 1980), the lead deposition has

decreased regularly all over the country (Berg and

Steinnes, 1997; Steinnes et al., 2001), but the earlier

deposits are retained in surface soils (Steinnes et al.,

1989, 1997) and may still be a source of significant

concern for considerable time in the future.

Thanks to the moss biomonitoring technique, the

temporal and spatial distribution of lead deposition in

Norway has been monitored in great detail since 1977.

This approach is especially well suited for lead since

the Pb concentration measured in naturally growing

terrestrial moss is closely related to the bulk deposi-

tion (Berg et al., 1995). Still the contribution of lead

E. Steinnes et al. / Science of the Total Environment 336 (2005) 105–117106

from different source regions and categories to a given

site cannot be estimated from the moss technique

alone. Since the ratios between the four stable lead

isotopes vary in different lead deposits due to differ-

ences in the geological history, the determination of

the stable isotope composition of lead using high

precision thermal ionisation mass spectrometry

(TIMS) has been shown to be a useful method to

study the contribution from different source categories

to lead pollution in various types of environmental

Fig. 1. Locations of the m

samples (Flegal et al., 1986; Maring et al., 1987;

Smith et al., 1990; Rosman et al., 1993; Graney et

al., 1995; Dunlap et al., 1999). Stable lead isotope

ratios in moss samples were studied for the first time

by Rosman et al. (1998) on a material from seven sites

in different parts of Norway. The samples from each

site had been collected at four different times, in 1977,

1985, 1990, and 1995, and they appeared to exhibit

considerable temporal as well as spatial variation in

lead isotope composition. The present work is an

oss sampling sites.

Table 1

Stable lead isotope ratios in moss samples collected at five different times at 22 different localities in Norway

Location Coordinates (decimal) Year 206/204 206/207 208/207 Pb Ag/g

jN jE

(1) Rømskog 59.68 11.82 2000 18.012 1.1558 2.4294 10.9

1995 17.835 1.1468 2.4167 11.9

1990 17.795 1.1411 2.4153 14.5

1985 17.664 1.1363 2.4083 24

1977 17.796 1.1411 2.4182 49

(2) Trysil 61.42 12.38 2000 17.947 1.1523 2.4254 2.01

1995 17.908 1.1473 2.4215 6.9

1990 17.653 1.1338 2.4078 13.7

1985 17.714 1.1394 2.4087 15

1977 17.724 1.1379 2.4125 35

(3) Brandbu 60.43 10.58 2000 17.873 1.1473 2.4203 5.6

1995 17.613 1.1340 2.4015 10.3

1990 17.766 1.1401 2.4133 12.5

1985 17.656 1.1335 2.4062 24

1977 17.730 1.1398 2.4154 50

(4) Vang/Valdres 61.15 8.40 2000 17.880 1.1477 2.4223 3.6

1995 17.677 1.1389 2.4082 6.7

1990 17.702 1.1375 2.4097 13.5

1985 17.632 1.1329 2.4057 13

1977 17.711 1.1374 2.4130 38

(5) Andebu 59.30 10.12 2000 18.089 1.1604 2.4350 4.6

1995 17.979 1.1550 2.4251 26.1

1990 17.882 1.1454 2.4191 23.5

1985 17.731 1.1390 2.4111 37

1977 m m m 123

(6) Amot/Vinje 59.50 7.97 2000 18.039 1.1554 2.4291 4.9

1995 17.849 1.1479 2.4167 7.4

1990 17.760 1.1411 2.4110 21.6

1985 17.703 1.1373 2.4094 25

1977 17.731 1.1393 2.4130 19

(7) Vegarshei 58.97 8.93 2000 18.067 1.1574 2.4329 13.9

1995 17.941 1.1498 2.4234 29.9

1990 17.806 1.1431 2.4167 27.1

1985 m m m 53

1977 17.777 1.1415 2.4180 112

(8) Evje 58.58 7.87 2000 18.238 1.1678 2.4316 6.2

1995 17.889 1.1486 2.4183 12.5

1990 17.725 1.1367 2.4089 26.8

1985 17.553 1.1297 2.4004 29

1977 17.887 1.1374 2.4251 50

(9) Øyslebø 58.17 7.58 2000 17.937 1.1513 2.4245 18.1

1995 17.872 1.1467 2.4201 24.4

1990 17.648 1.1346 2.4071 52.3

1985 17.553 1.1268 2.4025 86

1977 17.685 1.1391 2.4140 148

(10) Gya 58.60 6.37 2000 17.800 1.1432 2.4156 8.7

1995 17.614 1.1322 2.4042 21.6

1990 17.449 1.1221 2.3950 41.7

1985 m m m 99

1977 17.989 1.1280 2.4141 106

(continued on next page)

E. Steinnes et al. / Science of the Total Environment 336 (2005) 105–117 107

Table 1 (continued)


jN jE

(11) Nedstrand 59.33 5.70 2000 17.857 1.1462 2.4114 5.5

1995 17.527 1.1277 2.3988 13.5

1990 17.482 1.1204 2.3976 21.2

1985 17.329 1.1133 2.3897 30

1977 17.545 1.1264 2.4054 49

(12) Kvitingen 60.45 5.86 2000 17.715 1.1373 2.4118 4.9

1995 17.526 1.1259 2.3993 11.3

1990 17.374 1.1174 2.3916 35.5

1985 17.265 1.1110 2.3846 35

1977 17.528 1.1280 2.4023 30

(13) Haukeland 60.83 5.58 2000 17.800 1.1436 2.4183 6.7

1995 17.523 1.1246 2.3988 21.8

1990 17.392 1.1183 2.3931 29.7

1985 17.321 1.1160 2.3879 35

1977 17.590 1.1305 2.4064 47

(14) Vagsøy 61.98 5.17 2000 17.746 1.1413 2.4160 4.4

1995 17.637 1.1338 2.4079 9.1

1990 17.473 1.1252 2.3983 12.5

1985 17.360 1.1176 2.3925 18

1977 17.579 1.1323 2.4071 19

(15) Karvatn 62.78 8.85 2000 17.848 1.1480 2.4221 0.94

1995 17.704 1.1380 2.4094 1.5

1990 17.612 1.1324 2.4047 2.9

1985 17.450 1.1246 2.3941 4

1977 17.628 1.1361 2.4074 8

(16) Momyr 64.08 10.52 2000 17.880 1.1494 2.4229 1.38

1995 17.712 1.1378 2.4105 4.4

1990 17.561 1.1305 2.4020 6.0

1985 17.488 1.1261 2.3966 9

1977 17.744 1.1409 2.4152 26

(17) Muru 64.47 14.12 2000 18.043 1.1582 2.4305 1.16

1995 17.826 1.1443 2.4138 1.9

1990 17.758 1.1399 2.4118 5.9

1985 17.572 1.132 2.401 8

1977 17.748 1.1414 2.4144 4

(18) Vassvatnet 66.40 13.18 2000 17.907 1.1513 2.4243 4.8

1995 17.815 1.1435 2.4155 9.3

1990 17.597 1.1333 2.4046 11.7

1985 m m m 14

1977 17.678 1.1402 2.4141 37

(19) Moskenes 67.92 13.05 2000 17.899 1.1520 2.4270 2.5

1995 17.833 1.1420 2.4171 9.3

1990 17.601 1.1296 2.4043 13.4

1985 17.641 1.1351 2.4054 28

1977 17.828 1.1452 2.4157 18

(20) Øverbygd 69.00 18.95 2000 18.011 1.1577 2.4335 2.1

1995 17.862 1.1456 2.4191 1.9

1990 17.589 1.1273 2.4046 3.4

1985 17.532 1.1284 2.3974 6

1977 17.730 1.1386 2.4108 5


Table 1 (continued)


jN jE

(21) Karasjok 69.45 25.78 2000 18.038 1.1569 2.4357 0.87

1995 17.891 1.1495 2.4180 1.4

1990 17.783 1.1436 2.4132 2.6

1985 17.629 1.1329 2.4042 6

1977 17.773 1.1452 2.4165 5

(22) Gamvik 71.07 28.23 2000 17.915 1.1520 2.4274 1.45

1995 17.902 1.1495 2.4259 2.7

1990 17.881 1.1491 2.4236 7.2

1985 17.698 1.1373 2.4087 3

1977 17.899 1.1487 2.4235 5

m =missing value.


extension of that work to 22 different sites covering

the entire mainland of Norway and including samples

from year 2000 in addition to the four previous years

of sampling.

2. Materials and methods

Samples of the feather moss Hylocomium splen-

dens from 22 sites in different parts of Norway,

respectively, in 1977, 1985, 1990, 1995, and 2000

were investigated in the present work. The samples

had been collected as part of a national program

monitoring the deposition of pollutants from long-

range atmospheric transport, and the parts of the moss

plant representing the incremental growth during the

last 3 years preceding the year of collection were

taken for analysis. The locations of the 22 sites are

shown on the map in Fig. 1, and their geographical

coordinates are listed in Table 1. All selected sites are

located in relatively remote areas far from towns or

other significant sources of air pollution.

Moss samples of about 0.2 g were decomposed in a

low-temperature plasma asher. The residue was dis-

solved in a few drops of concentrated HNO3. After

evaporating the solution to dryness, the residue was

dissolved in 0.2 ml 3 MHNO3 before chromatographic

separation of Pb according to a modification of the

method described by Horwitz et al. (1992, 1994). The

sample solution was fed on a column packed with a

crown ether resin. After removing most other elements

by washing with 3 M HNO3, Pb was eluted with dilute

ammonium carbonate solution. The analyses were

performed on a Finnigan MAT 261 mass spectrometer

using single rhenium filaments and the total Pb blank

was < 100 pg. Before loading the sample, 2 Al of silicagel (Merck) was evaporated to dryness on the filament

at a current of 1 A. The sample was dissolved in 1 Al of10% H3PO4, loaded onto the silica gel, and evaporated

to dryness at 1 A. The current was then raised to 1.5 A

for 1 min and subsequently to 2.0–2.1 A followed by a

swift raise to red glow. The turret was loaded with 12

samples and 1 NBS 981 Pb standard. Filament current

during analyses varied between 1.6 and 1.8 A. Data

collection was made in 10 blocks of 10 measurements.

The Pb isotopic ratios were corrected for mass frac-

tionation by repeated analyses of the NBS 981 Pb

standard, which showed a reproducibility of 206Pb/204Pb =0.16%, 206Pb/207Pb = 0.06%, and 208Pb/206Pb = 0.16% at the 2s level.

3. Results and discussion

Results from the lead isotope analyses, expressed

by the ratios 206Pb/207Pb, 208Pb/207Pb, and 206Pb/204Pb, are listed in Table 1, along with the cor-

responding Pb concentrations from previous analyses

by electrothermal AAS (1977, 1985) or ICP-MS

(1990–2000). Since much of the Pb isotope data for

environmental samples in the literature are presented

as 206Pb/207Pb, the subsequent discussion will be

based on this ratio in order to make the comparison

with the previous data easier.

The trends apparent from the preliminary report on

Norwegian mosses (Rosman et al., 1998) based on

seven sites are confirmed and fortified by the present

results. In general, the 206Pb/207Pb ratio drops from


1977 to 1985 and then turns gradually to higher values

during the period 1990–2000. The regional differences

in 206Pb/207Pb however are considerable at any time,

with the lowest values observed in the southwest. In

order to facilitate a more detailed discussion, isopleths

of the 206Pb/207Pb ratio were constructed for each of the

sampling years 1977 (Fig. 2), 1985 (Fig. 3), 1990 (Fig.

4), 1995 (Fig. 5), and 2000 (Fig. 6). These dates

represent the year of collection. Since the moss samples

were collected in a way to represent the incremental

growth during the three preceding years, the represen-

tative years for comparison with literature data (with

Fig. 2. Geographical variation of 206Pb/207Pb

the exception of Scottish moss samples) may be 1975,

1983, 1988, 1993, and 1998, respectively.

Previous knowledge on contributions from different

source regions to the lead deposition in Norway at

different sites and times is very limited. Some evidence

is available from the Birkenes station in southernmost

Norway, about 40 km southwest of the present site 7,

where lead and other trace elements were studied in

diurnal aerosol samples collected during 1978–1979

and 1985–1986 (Amundsen et al., 1992) and the

corresponding air trajectories assigned to eight sectors

representing different source regions. The predomi-

ratio in moss samples collected in 1977.

Fig. 3. Geographical variation of 206Pb/207Pb ratio in moss samples collected in 1985.


nant contributions came from the sectors covering the

European mainland and UK. Contributions to the

integrated amount of lead from the sectors covering

Norwegian territory were only 11.7% and 11.8%,

respectively, for the two periods (not including trajec-

tories that could not be assigned to any particular

sector). Corresponding data do not exist for other

relevant sites in Norway, but since all sampling sites

were quite remote from densely populated areas, it

may be assumed that the contribution of lead from

domestic sources did not play a major role at any site.

Since long-range atmospheric transport from

source regions elsewhere in Europe is the main source

of lead deposition in Norway, it seems appropriate to

start the discussion by reviewing literature data for206Pb/207Pb in air in different potential source regions

over the time period concerned. Data for aerosols as

well as from analyses of precipitation and dated ice

and peat cores are useful for this purpose. A survey of

available literature data is presented in Table 2. The

most complete data are from the UK, where relevant

data exist for the entire period covered by the Nor-

wegian moss survey. Considering all data, it appears

that the 206Pb/207Pb ratio dropped by nearly 2% from

the mid 1970s to the early 1980s, stayed low for some

years, and then increased again from the late 1980s



due to the gradually increasing use of unleaded petrol

after 1986 (Farmer et al., 2000). For the years repre-

sented by the Norwegian moss samples, the following

approximate values may be estimated from the UK

data: 1975, 1.120; 1983, 1.105; 1988, 1.125; 1993,

1.135; 1998; 1.145. This estimation does not consider

the peat values from Western Scotland (Weiss et al.,

2002), which are systematically higher than the other

data by about 1% but show the same temporal trend.

For mainland Europe, the data are relatively scarce,

and the corresponding estimates are therefore presum-

ably less reliable. For western/central Europe, the206Pb/207Pb ratio does not show the same variation as

in the UK but seems to have been of the order of 1.13–

1.14 over the entire period 1975–1993. In some of

these countries, the use of unleaded petrol started

earlier than in the UK. In the western part of the Soviet

Union and possibly other states in eastern Europe, a

relatively stable value around 1.155 may be estimated.

Leaded gasoline is still used in this part of Europe.

Before entering a detailed discussion of the infor-

mation carried by the present lead isotope data for



mosses, some additional pieces of information need to

be considered. First, although a strong and consistent

decline of lead deposition all over the country is evident

from the numbers for total Pb in moss in Table 1, there

are distinct geographical differences in these trends, as

illustrated in Fig. 7. In the 1977 survey, the observed

lead deposition was far higher in the south than

elsewhere, particularly in areas near the Skagerrak

coast (sites 5, 7, 8, 9), but the deposition there dropped

by over a factor of 3 until 1990 followed by a regular

but somewhat slower decline through the 1990s. Pre-

cipitation in this region is predominantly supplied by

southerly to easterly winds. Turning to the southern

part of the west coast (sites 11–14), the 1977 lead

figures were only about 30% of those in the far south,

but the level stayed relatively constant until 1990 after

which there was a similar decay as in the south. In this

area, in particular at sites approximately 20–50 km

from the coast (cf. sites 12–13), the annual precipita-

tion is about three times higher than at the southern

coast, but the prevailing wind direction during precip-

itation events is south–southwest. From site 14 and



northward, the 1977 values were only 10–20% of those

in the far south, and a regular decline was observed

over the whole period. In most of this area, precipita-

tion is supplied mainly by westerly/north–westerly

winds from the North Atlantic.

Considering all the above information and relating

it to the moss 206Pb/207Pb data, the following inter-

pretations may be offered with respect to the most

important source regions of lead deposition in Norway

at different times:

Southern–southeastern region (sites 1–9): This

region probably received most of its lead in the past

from mainland Europe. The rapid decline during the

1970s–1980s is probably to a great extent associated

with early introduction of unleaded gasoline in some

of the source countries. An influence from UK is also

evident in this region, however, with declining206Pb/207Pb between 1977 and 1985 and gradually

decreasing ratios toward the west at all times. Recent-

ly ratios of 1.15–1.16 are observed in this region,

indicating that a greater fraction of the recent lead

from long-range transport has its origin in Eastern

Europe, including Russia.

West coast (sites 10–14): Ratios here are consis-

tently lower than elsewhere, and follow quite closely

the UK trend for airborne lead. In this region, the

Table 2206Pb/207Pb in aerosol and other relevant media in different parts of Europe

Country, Site Sampling medium Year 206Pb/207Pb (number) Reference

UK

Perth Aerosols 1994 1.101 Rosman et al., 1998

Scotland Moss 1970–1979 1.127(30) Farmer et al., 2002

1980–1989 1.120(10)

1990–1999 1.137(16)

2000 1.151(7)

Rainwater 1989–1991 1.120(31) Farmer et al., 2000

1997–1998 1.144(145)

Scotland, rural Aerosols 1985 1.118(10) Farmer et al., 2000

Lancashire Aerosols 1985 1.108(5) Farmer et al., 2000

Harpenden Herbage 1971–1975 1.116(2) Bacon et al., 1996

1976–1980 1.108(2)

1981–1985 1.098(2)

1986–1990 1.128(2)

Scotland, western Peat 1975F 2 1.133 Weiss et al., 2002

1981F 2 1.129

1986F 2 1.117

1988F 2 1.115

1991 1.133

Oxford Aerosols 1998 1.122(6) Bollhofer and Rosman, 2002

Western Europe

Mont Blanc Snow/ice 1975–1977 1.132(6) Rosman et al., 2000

1981–1984 1.138(7)

1986 1.144(3)

1990–1991 1.156(3)

France Aerosols 1994 1.137(4) Rosman et al., 1998

Germany Aerosols 1994 1.139(3)

Netherlands Aerosols 1994 1.137(2)

W. Europea Aerosols 1988 1.138(5) Hopper et al., 1991

Avignon Aerosols 1998 1.130(6) Bollhofer and Rosman, 2002

Grenoble Aerosols 1996–1998 1.112(10)

Constance Aerosols 1998 1.145(6)

Poln Aerosols 1998 1.156(6)

Eastern Europe

Moscow Aerosols 1994 1.152(2) Mukai et al., 2001

Moscow Aerosols 1999 1.160(6) Bollhofer and Rosman, 2002

E. Europea Aerosols 1988 1.169(4) Hopper et al., 1991

W. USSR Aerosols 1988 1.153(5)

a Aerosols in southern Sweden representing air transport from the respective sectors.


dominant contribution is most probably from the UK,

in particular during the 1980s.

Central and northern part (sites 15–20): In this

region, the temporal variation is less pronounced than

farther south. Ratios around 1.14 are typical, and the

main source region is probably the North Atlantic,

where even sources in North America, which have

relatively high 206Pb/207Pb values, may have contrib-

uted in addition to the European ones (Rosman et al.,

1998). The UK-associated decline in 1985 however is

also seen in most of this region, but less distinctly than

farther south. Recent development towards values of

1.15 and above may indicate some Russian/Eastern

European influence as well.

Far north-eastern sites (21–22): Here the level

stays quite stable at 1.14–1.15 during the entire

period, with the exception of a drop in 1985. In this

area, the relative importance of Russia/Eastern Europe

Fig. 7. Time trends in atmospheric deposition of lead in three

different parts of Norway as reflected by moss samples (Ag Pb/g

moss). Years shown are the years of sampling.


is obviously greater than in areas farther south, at least

until 1995.

Since local soil dust is invariably a problem in the

interpretation of data from moss surveys (Steinnes,

1995), contribution to the present data from local

mineral soil particles should also be considered. The

knowledge on lead isotope ratios in Norwegian bed-

rock is limited in general. In a recent study of stable

lead isotopes in podzolic soil profiles from different

parts of Norway, however, 206Pb/207Pb ratios within

the range 1.20–1.73 were observed in the C-horizon

(Steinnes et al., unpublished). Thus, it seems that none

of the moss data discussed in this work were appre-

ciably influenced from the geochemical background at

the sampling site.

Acknowledgements

This work was supported by a grant from the

Research Council of Norway.

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