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URBAN METAL FLOWS – A CASE STUDY OF STOCKHOLM

Review and Conclusions

B. BERGBÄCK1∗ , K. JOHANSSON2,3 and U. MOHLANDER4


1 Department of Biology and Environmental Science, Kalmar University, Kalmar, Sweden; 2
Swedish Environmental Protection Agency, Stockholm, Sweden; 3 Swedish University of
Agricultural Sciences, Department of Environmental Assessment, Uppsala, Sweden; 4 Stockholm
Environment and Health Protection Administration, Stockholm, Sweden
(∗ author for correspondence, e-mail: bo.bergback@hik.se; fax: +46 480 446262; tel: +46 480
446245)

(Received 20 September 2000; accepted 15 December 2000)

Abstract. Metals have rapidly accumulated in the anthroposphere, especially in urban areas, indic-
ating possible environmental and resource problems. Here, Stockholm City was chosen for a case
study of urban metal flows, i.e. metal inflow to, metals in the stock of, and metal outflow from
the anthroposphere to the biosphere. The metal stock of Stockholm is large and still growing. The
large amounts of metals in the solid waste fraction totally dominate the outflow from the city. For
major parts of the stock, the emissions from goods in use are negligible. There are, however, goods
applications corresponding to significant emissions: e.g. the traffic sector (Cu, Zn, Cr, Ni, Pb), the
tapwater system (Cu), roofs/fronts or other metal surfaces (Cu, Zn). Today’s known metal flows from
the anthroposphere of Stockholm to the biosphere and sewage sludge are quantitatively dominated
by Zn (34 ton y−1 ) and Cu (14 ton y−1 ). Historical and present emissions have resulted in high
metal concentrations in sediments (especially Cd, Hg and Pb, but also Cu and Zn), groundwater (Cu,
Hg) and in soils (Hg, Cu, Pb). At present the annual median concentrations are below the Swedish
limits for metals in sewage sludge, even if the safety margins are small for Cd, Hg and to some extent
Cu. The flows of Cu and Zn to Stockholm soils are high with a significant accumulation indicating
an environmental impact in a longer time perspective. High levels of metals in surface sediments in
the water environments reflects an ongoing input where these metals are transported from known
(Cu, Zn) and or partly unknown (Cd, Hg, Pb) sources. In future urban areas, monitoring of metal
flows must be performed both in the anthroposphere and the biosphere in order to have a pro active
approach to urban environmental problems and to get prompt answers to measures taken.

Keywords: corrosion, emissions, goods, metals, sediment, sewage sludge, soils, urban, waters

1. Introduction

The use of metals is well documented in man’s history e.g. in the bronze and iron
ages and in the Roman Empire. Since the beginning of the 20th century, marked
increases in the global population and in the GNP of developed countries have been
accompanied by a significant raise in metal production. Thus, metals have rap-
idly accumulated in man’s sphere of life – the anthroposphere, indicating possible
environmental and resource problems.

Water, Air, and Soil Pollution: Focus 1: 3–24, 2001.


© 2001 Kluwer Academic Publishers. Printed in the Netherlands.
4 B. BERGBÄCK, K. JOHANSSON AND U. MOHLANDER

Environmental impact by heavy metals was earlier mostly connected to indus-


trial emissions. In Sweden and other Western countries, metal production emissions
have decreased markedly since the 1970s, due to legislation, improved cleaning
technology and altered industrial activities. Today, and in the future, dissipative
losses from consumption of various goods are therefor of most concern. The accu-
mulated amount of metals in use, the stock, is to a large extent protected to corro-
sion or to other degrading processes. However, applications where large surfaces
are exposed to more corrosive environments may release significant metal amounts.
Other applications correspond to a limited stock but to relatively high metal re-
lease, e.g. sacrificial anodes (Zinc) or brakes (Copper). To assess the risk for man
and environment connected to this type of metal flows and their contribution to
metal exposure, there is a need for analysis of metal flow and accumulation in the
anthroposphere as well as in the biosphere, especially in urban areas corresponding
to the major part of the metal stock.
The large amounts in urban metal flow and accumulation are also connected to
resource problems. For a sustainable use of metals, secondary metal production is
preferable as far as possible in order to minimise use of substances and energy. For
example, to produce a ton of pure copper, it is necessary to process 110 tons of cop-
per ore, leaving millions of tons of gangue and overburden behind (Ayres, 1997).
However, the recycling rate for many metals is still too limited to prevent significant
metal fractions in the waste flow. Finally, metals that contaminate sewage sludge
may prohibit a recycling of valuable nutrients.
Urban metal flows have earlier been studied through analysis of waste wa-
ter, storm water and/or solid waste in e.g. Washington (Davidsson et al., 1978),
Gothenburg (Malmqvist, 1983) and Lelystad (van Dam et al., 1986). Metal emis-
sion sources, industrial and diffuse, have been evaluated in densely populated areas,
e.g. the Hudson-Raritan basin (Tarr and Ayres, 1990) and the Rhine river basin
(Anderberg and Stigliani, 1994). Material flow analysis has frequently been per-
formed in urban areas, but only a few have involved metals, e.g. Pb in Vienna
(Obernosterer and Brunner, 2001). Thus, there are a number of studies concerning
specific urban metal flows, but there is a need for studies that synthesises different
parts. Furthermore, metal load in the biosphere has mostly been studied for non
urban areas.
In order to assess the environmental impact of urban metal flows, a five year
research programme ‘Metals in the Urban and Forest Environment’ (SEPA, 1994)
was started in Sweden in 1994. Here, studies of metal flows and accumulation in the
anthroposphere and the biosphere of Stockholm were to be analysed. The results of
the research programme are presented in this volume of WASP in separate papers
and the aim of this review article is to summarise the urban parts of the programme.
URBAN METAL FLOWS – A CASE STUDY OF STOCKHOLM 5

2. System Boundaries of the Study

The administrative boarder of Stockholm City was chosen as the spatial system,
representing one of Sweden’s most densly populated areas with approximately 700
000 inhabitants in an area of 190 km2 . The work focused on the metals cadmium
(Cd), chromium (Cr), copper (Cu), lead (Pb), mercury (Hg), nickel (Ni) and zinc
(Zn). These metals were chosen due to their toxicity and/or frequent use in urban
areas.
The study covers a complete substance flow analysis, i.e. metal inflow to, metals
in the stock of, and metal outflow from the anthroposphere of Stockholm in 1995.
The recycling rates per metal varies from high (Cu) to low (Zn). National recycling
levels of Cu have been calculated to 40–90% (Landner and Lindeström, 1998a)
and for Zn approximately 30% (Landner and Lindeström, 1998b). However, the
recycling rates have not been calculated on the Stockholm level due to lack of
data. Thus, outflows from the city have here been represented by metals in sewage
sludge, solid waste and emissions from various sources. Environmental impacts on
areas outside Stockholm City which are related to activities from within the system
boundaries (the ‘Hinterland’) were excluded as well as studies of biological effects.

3. Metal Stock of Stockholm

Stockholm, the capital of Sweden, has a history of approximately 700 yr. At the
beginning of the 20th century the industry sector was diversified with e.g. tanneries,
foundries, battery and rubber factories, impregnation and galvanisation plants, gas,
dye and printing works. Today the trade, service and financial sectors are domin-
ant. To the west of the city lies Lake Mälaren, Sweden’s third largest lake, which
discharges into the Baltic Sea east of Stockholm (Figure 1).
The present metal stock of Stockholm has developed mainly during the 20t h
century: electrification (Cu, Pb) started at the turn of the century and culminated
1920–1960; the tapwater system changed in the 1950s from Fe and Zn to Cu; the
use of amalgam (Hg) peaked 1950–1980 and so did the use of Cd in stabilisers,
pigment and plating; applications of stainless steel (Cr, Ni) and galvanised steel
(Zn) became common after the Second World War (Lohm et al., 1997). In Table I
the calculated metal stock in the anthroposphere of Stockholm in 1995 is presented.
A more detailed presentation of various goods per metal is given in Sörme et al.,
(2001a).
The ranges for the metal stock have been estimated by using a method of uncer-
tainty intervals (Hedbrant and Sörme, 2001). Metals in waste per year have been
calculated from metal content in solid waste from households and industry. An
uncertainty range for metal amounts in waste has not been calculated due to lack
of data, but the uncertainty in total amounts is probably high. Analysis of slag and
ashes from Högdalen incineration plant (Stockholm) give lower waste metal flows
6 B. BERGBÄCK, K. JOHANSSON AND U. MOHLANDER

TABLE I
Metals in inflow y−1 , stock and solid waste y−1 in the anthropo-
sphere of Stockholm, Sweden 1995

Metal Inflow Stock Stock Solid Waste


(ton y−1 ) (ton) uncertainty (ton y−1 )
range (ton)

Cd 8.8 120 90–440 4


Cr 360 5600 3000–11000 100
Cu 2300 123000 52000–370000 300
Hg 0.46 7 4–11 1
Ni 190 2500 1300–4800 30
Pb 1600 52000 35000–84000 300
Zn 1900 28000 9900–92000 700

Figure 1. Hg (µg g−1 ds) in surface sediment (0–2 cm), n = 185. Extreme values have been excluded.

per year (Björklund, 1998) but as these calculations are based on few data and
related only to mineralised metal, the uncertainty level will still be high.

4. Metal Load in the Biosphere of Stockholm

Historical and present emissions have resulted in elevated concentrations in urban


sediments, soils and waters. The impact of urban metal load in surface sediments
is obvious in the transect Lake Mälaren to the Stockholm Archipelago (Figure 1).
Here, precipitation mechanisms may be possible as outflowing fresh water of
Lake Mälaren interfaces the brackish water entering from the Baltic sea. However,
according to Lindström et al. (2001) no such effects could be found. For Cd, Hg
and Pb the concentrations are extremely high in surface sediments, corresponding
URBAN METAL FLOWS – A CASE STUDY OF STOCKHOLM 7

to an enrichment factor of 10, 42 and 11 calculated from medians compared to the


distribution of scandium (Blomqvist and Larsson, 1996), while Cu and Zn have
enrichment factors of 3–4. Hence, Stockholm is a strong source of Cd, Cu, Hg,
Pb and Zn. Chromium concentrations are, however, only moderately perturbed and
the Ni concentrations are close to preindustrial levels. The accumulation rates of
especially Cd do, however, show a declining trend during the last 20 yr according
to Sternbeck and Östlund (2001). Also Hg, Pb and Zn show this trend though not
quite as strongly as Cd.
Results from urban soil analyses showed a wide range in heavy metal concentra-
tions, as well as in other soil properties (Linde et al., 2001). Sampling were made
in- and outside the city centre. Sites in the city centre were dominated by public
parks on areas with lawns or other types of vegetation. Sampling sites outside the
central zone were grouped based on present land use, i.e. undisturbed soils, public
parks, waste lands and roadside soils. The city centre and the wasteland soils gener-
ally showed enhanced heavy metal concentrations to at least 30 cm depth compared
to park soils outside the city centre and arable soils in the region. The amounts of
the various metals per m2 down to 30 cm depth in soil in the city centre were
calculated as well as for corresponding values for park soils and for arable soils in
the region. Since the city centre soils were all sampled in parks, the soil properties
and management practices can be assumed to be similar in these soils as in the
outside park soils, which enables a direct comparison between the two soil groups.
The differences between the metal contents in the park soils and the city centre soils
were calculated to provide a rough estimate of the amounts of metals accumulated
in the city centre environment due to local emissions. The relative enhancement
(0–30 cm depth) in the city centre soils was highest for Hg, 0.29 g m−2 compared
to 0.05 g m−2 in the park soils outside the city centre, i.e. an enhancement of more
than 6 times. The pools of Pb, Zn and Cu were 38, 58 and 21 g m−2 respectively,
which for Pb was 3–4 times higher and for Zn and Cu 1.5–2 times higher than in
the outside park soils. The soil Cd, Cr and Ni pools in the city centre were at the
same level as those in the outside park soils. Bringmark et al. (2001) reported high
Cu and Pb concentrations in the mor layers of soils surrounding a busy motorway
at Kista, Stockholm. The mean Cu and Pb content 10–60 m from the road was
elevated 3 and 8 times respectively, compared to reference samples. Contrary to
what is usually reported from roadsides, the mean Cu and Pb levels were still high
further away from the road at 200 and 700 m.
Concentrations of heavy metals in the groundwater of Stockholm are in general
very high in comparison with groundwater in forested areas (Aastrup et al., 2001).
Cu and Hg have median concentrations exceeding ‘background’ median 10 re-
spectively 8 times. For Cr, Ni and Pb the median values were 3–4 times higher,
while Cd and Zn have the least elevated median concentrations (2 times). The
annual contribution of metals by groundwater to the main surface water bodies was
estimated to be most limited, mainly explained by the small groundwater recharge
in the urban area due to land sealing.
8 B. BERGBÄCK, K. JOHANSSON AND U. MOHLANDER

TABLE II
Stock of heavy metals in goods (ton) for Cd, Cr, Cu, Pb, Hg,
Ni, Zn in use in different exposure conditions, Stockholm,
1995 (rounded numbers)

Metal Total Protected Exposed to


Soil Water Air

Cd 120 75 12 0 12
Cr 5600 3000 540 640 1350
Cu 123000 78000 17000 19000 9000
Pb 52000 32000 11000 8500 700
Hg 7 71 0 0 0
Ni 2500 1800 0 240 500
Zn 28000 8800 0 8600 11000

1 C.f. Table VII.

To what extent these elevated concentrations can be explained with known


emission sources will later be discussed.

5. Goods as Metal Emission Sources

In order to assess the metal load to the biosphere of Stockholm, both present and
historical emission sources must be considered. Industrial point source emissions
were earlier significant but are today most limited. Diffuse emissions from the
metal stock of the anthroposphere of Stockholm have historically been important
for some metals. For Hg, approximately 200 tons were used in various goods,
mainly medicine, between 1795 and 1995. A major part of this amount may even-
tually have reached the biosphere of Stockholm (Svidén et al., 2001). After the
Second World War leaded petrol became frequently used and up till 1995 approx-
imately 4200 tons of Pb have been emitted in Stockholm (Lohm et al., 1997).
These, and other historical emissions, may today be important secondary emission
sources from soils and sediments. However, the knowledge of metal pools in e.g.
polluted soils is limited, but there are indications that they correspond to significant
amounts (Bergbäck, 1998).
Today, the stock (or goods in use) represent the major source of emission for
all metals studied, i.e. the focus should be on the parts of metals in infrastructure,
buildings, vehicles etc. that are exposed to corrosive conditions or other degrading
processes. The part of the metal stock of Stockholm exposed to soil, water and air
(Table II) have been calculated by Sörme et al. (2001b).
A partly new research field has developed within this programme in analysing
corrosion rates related to metal run off from different surfaces. Extensive research
URBAN METAL FLOWS – A CASE STUDY OF STOCKHOLM 9

has earlier been carried out regarding corrosion rates of Cu and Zn in various
environments, but knowledge of actual runoff rates has been limited. Through a
field exposure program in Stockholm the corrosion and runoff rates for Cu and
Zn of different age were determined. New Cu exposed for 48 weeks in the urban
atmosphere shows a runoff rate of 1.3 g m−2 y−1 while naturally aged Cu exhibits
a higher runoff rate of 2 g m−2 y−1 . For Zn the runoff rate is approximately 3.1 g
m−2 y−1 regardless of age (He et al., 2001).
Investigations of run-off from materials used on buildings and other construc-
tions have been performed both by short-term exposures of smaller model surfaces
and by long-term exposures of larger materials surfaces on buildings and other
constructions (Persson and Kucera, 2001). Elevated concentrations compared to a
inert surface were observed in run-off for Zn, from galvanised steel and surfaces
painted with zinc containing paints; for Cu from surfaces on copper roofs and wood
impregnated with copper compounds; for Cr from concrete and stainless steel and
for Ni from surfaces of asphalt, asphalt roofing felt, concrete surfaces and stainless
steel.
These and other data (mainly Sörme et al., 2001b and Bergbäck and Svensson,
1998), were used to calculate emissions from goods in use, here called goods
emissions (Tables III-IX). For some applications there is a lack of ‘release’ data
or corrosion rate. In the tables they have been marked as unquantified emission
sources. Thus, calculated emissions per year correspond to minimum levels.

5.1. C ADMIUM

For Cd, car washes represent the major known emissions source (Table III). How-
ever, some double counting may take place when including car washes as metals
from tyres, brakes etc. may influence the waste water metal concentration. Ob-
viously, this is also true for the other metals. In the last decades, electrolytic Zn
with an average Cd content of 10 ppm has dominated. Earlier, the Cd content
was at least ten times higher and some applications may still be in use. The part
of the Cd stock exposed to air, soil or water is approximately 25 tons dominated
by Cd in stabilisers (15 tons) and surface plating (6 tons). Thus, the release from
these unquantified sources could be significant and in the same magnitude as the
calculated total emissions.

5.2. C HROMIUM

Wear of tyres and road pavements are the two major Cr emission sources identi-
fied (Table IV). Roofs/fronts and pipes in waste water treatment plants represent
approximately 15% of the exposed stock of stainless steel. The major part of the
stock is, however, found in households in e.g. sinks and cutlery. If the same release
rates are assumed for the total stainless steel stock, the annual emission will be
120–290 kg. The stock of Cr in concrete (230 tons), impregnated wood (520 tons),
paints and pigments (70 tonnes) and in modern car exhaust systems (50 tons) is
10 B. BERGBÄCK, K. JOHANSSON AND U. MOHLANDER

TABLE III
Major goods emission sources in Stockholm, 1995 – Cadmium. For further details, see Sörme et
al., 2001b

Goods Calculated emissions (kg y−1 )

Vehicles Tyres 0.2–3


Brakes <1
Petrol 5
Car wash 11
Buildings Roofs/fronts <1 Impurities in Zn (Cd content 10 ppm)
Tap water <1 Impurities in Zn (Cd content 10 ppm)
Infrastructure Galvanised goods <1 Impurities in Zn (Cd content 10 ppm)
Road pavements 2
Households Artists paint 1–3
Fertilis ers 1–2
Detergents <1
Total Cd emissions 20–26+?a

a Unquantified emission sources: stabilisers, pigments, surface plating and alloys.

TABLE IV
Major goods emission sources in Stockholm, 1995 – Chromium For further details, see
Sörme et al., 2001b

Goods Calculated emissions (kg y−1 )

Vehicles Tyres 200


Brakes 6
Petrol <1
Car wash 60
Buildings Roofs/fronts <1 Stainless steel
Pipes WW treatment plants 3–4 Stainless steel
Infrastructure Road pavements 500
Total Cr emissions 770 + ?a
a Unquantified emission sources: concrete, impregnated woods, paints and pigments,
exhaust systems.

to a varying degree exposed to corrosive environments. Thus, the release from


these unquantified sources could be significant and in the same magnitude as the
calculated total emissions.
URBAN METAL FLOWS – A CASE STUDY OF STOCKHOLM 11
TABLE V
Major goods emission sources in Stockholm, 1995 – Copper. For further details, see Sörme et
al., 2001b

Goods Calculated emissions (kg y−1 )

Vehicles Tyres 200


Brakes 3900
Petrol 2
Protection painting, boats 700 To water recipient
Car wash ? No data available
Buildings Roofs/frontsb 1000
Electrical grounding 40–900
Tap water 4300
Infrastructure Aerial lines 1200
Road pavements 400
Total Cu emissions (except painting, boats) 11500-12400 +?a
a Unquantified emission sources: Brass, wood preservative, cars.
b For more details – see Ekstrand and Östlund (2001)

5.3. C OPPER

Copper lined brakes together with Cu and brass goods in the tapwater system are
major Cu emission sources (Table V). Brass has otherwise a most diverse use but
the degree of exposure to corrosive environments is more limited. The exposed
part of the Cu stock in wood preservative (570 tons) and in car radiators and
brake-pipes (1200 tons) are also unquantified emission sources, but these contri-
butions are probably significantly lower than the calculated total Cu emissions in
Table V. Thus, the major annual emissions are identified even though the calcu-
lated emissions from electrical grounding is most uncertain due to varying soil
conditions.

5.4. L EAD

The Pb stock in Stockholm is dominated by cables, where the major part is not
exposed to corrosive conditions. Thus, the corresponding emissions are probably
limited. The major emission sources, ammunition and sinkers, have been treated
separately as they mostly have an impact on restricted areas (Table VI). The un-
certainty level is high for calculated emissions from pigments used as wood pre-
servatives (Falu-Red). For other pigments, e.g. red lead on miniated steel bridges
and in different paints, the data is to scarce for quantification, but probably these
applications represent significant annual emissions in the magnitude of one tonne.
12 B. BERGBÄCK, K. JOHANSSON AND U. MOHLANDER

TABLE VI
Major goods emission sources in Stockholm, 1995 – Lead. For further details, see Sörme et
al., 2001b

Goods Calculated emissions (kg y−1 )

Vehicles Tyres 300


Brakes 560
Petrol 100
Car wash 300
Buildings Chimney collars 6–70
Wood preservative, 200–1200
‘Falu-Red’
Infrastructure Road pavements 100
Specials Ammunition 5500 Mostly shooting grounds
Sinkers, sport fishing 5000 Mostly Norrström
(Stockholm City)
Total Pb emissions (except ammunition 1700–2700+?a
and sinkers)

a Unquantified emission sources: Balance weights, miniated steel bridges, paints/pigments.

5.5. M ERCURY

The Hg stock in Stockholm (7 tons) is totally dominated by the use of amalgam (5


tons). In Table II, this part has been classified to be in a protected environment.
However, Hg is continuously released from dental fillings but the rate is most
uncertain (Table VII). Amalgam is also a Hg emission source through cremation,
corresponding to 20 kg y−1 in Stockholm, 1995, but most of this Hg will probably
be long-range transported and deposited outside Stockholm. As discussed earlier,
historical emissions accumulated in soil, sediments or the wastewater system may
today be important secondary emission sources. Thus, the total Hg emissions are
significantly higher than presented in Table VII.

5.6. N ICKEL

For Ni, the traffic sector dominates the calculated emissions (Table VIII). There
are indications of Ni release from especially older concrete surfaces (Persson and
Kucera, 2001) that may add to the total Ni emissions, but probably are the major
sources identified.
URBAN METAL FLOWS – A CASE STUDY OF STOCKHOLM 13
TABLE VII
Major goods emission sources in Stockholm, 1995 – Mercury. For further
details, see Sörme et al., 2001b

Goods Calculated emissions (kg y−1 )

Vehicles Tyres 0.4


Brakes < 0.1
Car wash ? No data available
Petrol <2
Infrastructure Road pavements 1
Special Amalgam 11–16
Total Hg emissions 12–17 +?a
a Unquantified emission sources: Secondary emission sources – waste water
system.

TABLE VIII
Major goods emission sources in Stockholm, 1995 – Nickel. For further details, see Sörme
et al., 2001b

Goods Calculated emissions (kg y−1 )

Vehicles Tyres 200


Brakes 8
Petrol <3
Car wash 55
Buildings Roofs/fronts 0.5 Stainless steel
Pipes in WW treatment plants 2 Stainless steel
Infrastructure Road pavements 300
Total Nie missions 566+?a

a Unquantified emission sources: Concrete.

5.7. Z INC

The major Zn emission sources quantified are tyres and galvanised goods (Table
IX). Various applications of Zn chemicals (in pigments and dermal care products)
and galvanised goods in cars are emission sources, here unquantified do to lack of
data. However, these contributions will probably not significantly change the total
calculated Zn emissions.

6. Metal Flows – Anthroposphere to Biosphere

The use of metals in goods may have an environmental impact that either is re-
lated to metal flows in the solid waste fraction, or to emissions from goods to the
14 B. BERGBÄCK, K. JOHANSSON AND U. MOHLANDER

TABLE IX
Major goods emission sources in Stockholm, 1995 – Zinc. For further details, see Sörme
et al., 2001b

Goods Calculated emissions (kg y−1 )

Vehicles Tyres 10000


Brakes 900
Petrol 60
Sacrificial anodes(boats) 1500 To water recipient
Car wash 3000
Buildings Roofs/fronts 2100
Tap water 700
Infrastructure Galvanised goods 5000
Road pavements 1000

Total Zn emissions (except sacrificial anodes) 24300 +?a

a Unquantified emission sources: Chemicals, cars.

biosphere. In Figures 2–8, some major metals flows in the anthroposphere and bio-
sphere of Stockholm, 1995, are elucidated. The total metal flows to the biosphere
of Stockholm were calculated from emissions from goods (Tables III-IX), atmo-
spheric deposition, industrial emissions and metals via food. For the magnitude of
wet and dry deposition in Stockholm, a study mainly from 1995/96 has been used
(Johansson and Burman, 1998, Burman and Johansson, 2000). Obviously, part of
the deposition may be influenced by goods and industrial emissions from within
Stockholm, i.e. some double counting may occur. Metal flows via food inclusive
drinking water have been calculated roughly from (SEPA, 1993).
Soil and sediment were chosen as sinks in the biosphere, which together with
sewage sludge and solid waste represent the four end stations considered. Obvi-
ously, these end stations are to some extent temporary as a part of the metal flow
may continue to other destinations, e.g. soil metals may leach to the groundwater.
However, for all metals studied, the flow via groundwater to water recipients is
in general most limited (Aastrup et al., 2001), but the metal flows from specific
polluted areas can be significant. Correspondingly, a most limited fraction of metals
in waste (Table I) will reach the biosphere through incineration or leachate from
deposits (Bergbäck, 1998).
As a significant part of urban soil surfaces is impermeable, metals via atmo-
spheric deposition will be transported with stormwater to wastewater treatment
plants (WTP) in combined sewage pipes or directly to water recipients. Also metals
in food, industrial emissions are transported to the WTPs and so are partly ‘goods
emissions’, e.g. from the tapwater system (Cu, Zn), artists paint (Cd), car washes
(Cd, Pb, Zn), amalgam (Hg), dermal products and pigments (Zn). Other goods
URBAN METAL FLOWS – A CASE STUDY OF STOCKHOLM 15

applications may result in emissions to soils and/or stormwater, e.g. roofs and
fronts (Cu, Zn, Cr, Ni) or via the traffic sector (Cd, Cr, Cu, Ni, Pb and Zn).
The total metal emissions per year have been assumed to load either soils, storm
water or sewage water. Annual metal amounts to the WTPs of Stockholm, via waste
water or storm water, are relatively well known and so are the metal amounts to
water recipients (Stockholm Vatten, 1996). The magnitude of emissions per year to
soils can roughly be estimated as the difference between total calculated emissions
and metal flows in storm and sewage water. Metal flows to water recipients have
been calculated for groundwater by Aastrup (2001) and the flows from the WTPs
or directly via storm water to the water recipients were calculated via data from
Stockholm Vatten (compiled in Bergbäck, 1998). As a comparison, the metal flow
through Stockholm corresponding to the watershed of the lake Mälaren has been
calculated and so has the anthropogenic contribution to the metal deposition rate
(Dep. rate, Figures 2–8) to sediments (Lindström et al., 2001).

6.1. C ADMIUM

For Cd, most of the stock is unexposed to corrosion and constitute more a waste
problem with approximately 4000 kg Cd per year in the solid waste from Stock-
holm. The total emissions are estimated to be 50–80 kg y−1 including unquantified
goods emission sources (c.f. Table III). However, only identified emissions are rep-
resented in Figure 2. Artist’s paint and car washes are important emission sources
that have a major impact on the sewage sludge where most of the anthropogenic
Cd ends up. Cadmium concentrations are extremely high in sediments, probably
due to secondary emission sources, e.g. historically polluted areas, as the present
deposition rate to sediment significantly exceeds the total calculated emissions to
the water recipients.

6.2. C HROMIUM

The stock of Cr is totally dominated by stainless steel. No significant environmental


impact can be predicted as the emissions from these applications are most limited.
The traffic sector dominates the present Cr emissions, especially wear from road
pavements and tyres. The total emissions are probably higher than the calculated
0.8 ton y−1 (Figure 3) due to unquantified goods emission sources (c.f. Table
IV) with an estimated upper limit of 2 ton y−1 . The major part of the identified
emissions end up in sewage sludge. Calculated metal deposition rate to sediments
corresponds reasonable with emissions to the water recipient.

6.3. C OPPER

The major part of the Cu stock is unexposed to degrading processes. However,


there are applications with high emissions, e.g. the tapwater system being the major
source for the sewage sludge Cu content. The runoff from Cu roofs/fronts is still
16 B. BERGBÄCK, K. JOHANSSON AND U. MOHLANDER

Figure 2. Cadmium flows to soil, sediments, sewage sludge and solid waste (kg y−1 ) from different
metal emission sources in Stockholm, 1995. WTP Waste water Treatment Plant. For further details –
see text.

high even if corrosion rates have decreased with sulphur emissions. Brake linings
has been a most important Cu emission source to soil and storm water since the
introduction in the 1980s. Cu from brakes may, however, not only impact traffic
areas as emission of finer particles can be more long-ranged transported. Approx-
imately 50% of the total emissions ends up in the sludge and 25% reach the soils of
Stockholm (Figure 4). Calculated metal deposition rate to sediments corresponds
reasonable with emissions to the water recipient.

6.4. M ERCURY

Today, amalgam is totally the dominating part of the Hg stock. Even if calculated
emissions are uncertain, amalgam fillings will continuously be a major source of
sewage sludge Hg (Figure 5).
However, historical use and emissions are of major importance, e.g. Hg accumu-
lated in soils or in deposits in the waste water system (c.f. Table VII). An indication
for this is that the present deposition rate to sediment significantly exceeds the total
calculated emissions to the water recipients.
URBAN METAL FLOWS – A CASE STUDY OF STOCKHOLM 17

Figure 3. Chromium flows to soil, sediments, sewage sludge and solid waste (ton y−1 ) from different
metal emission sources in Stockholm, 1995. WTP Waste water Treatment Plant. For further details –
see text.

6.5. N ICKEL

As for Cr, stainless steel is the absolutely dominating part of the Ni stock, i.e.
the environmental impact is most limited. In contrast, the Ni emissions from the
traffic sector are relatively high (Figure 6). A special Ni source is the chemicals
used in waste water treatment plants. According to Lindström et al. (2001), the
anthropogenic Ni deposition rate to sediments is negligible.

6.6. L EAD

As discussed previously, the total Pb goods emissions are probably higher than
calculated (Figure 7) due to unquantified Pb release from paint/pigment applica-
tions. Thus, the total emission could be in the magnitude of 2–3 ton yr−1 . The use
of metallic Pb in ammunition and sinkers result in large amounts to the environ-
ment (10 ton y−1 ). Even if the uses mainly are restricted to specific areas and the
oxidation to Pb ions is slow, these activities may be considered as major emission
sources. Other emission sources are connected to the traffic sector, i.e. brakes, tyres
and car washes. The identified goods emissions, ammunition and sinkers excluded,
18 B. BERGBÄCK, K. JOHANSSON AND U. MOHLANDER

Figure 4. Copper flows to soil, sediments, sewage sludge and solid waste (ton y−1 ) from different
metal emission sources in Stockholm, 1995. WTP Waste water Treatment Plant. For further details –
see text.

load mainly soils and sewage sludge with approximately 1 ton y−1 respectively.
The present Pb deposition rate to sediment significantly exceeds the total calculated
emissions to the water recipients. In this comparison, sinkers should be excluded
as the are lost in a most restricted area. Thus, traces from historical activities are at
present important secondary emission sources.

6.7. Z INC

Zinc emissions from the traffic sector (tyres, brakes, car washes, road pavements)
correspond to approximately half the total goods emissions per year (Figure 8).
Other major sources are roofs/fronts and galvanised goods. A significant part of
the emissions loads the soils of Stockholm. Calculated metal deposition rate to
sediments corresponds reasonable with emissions to the water recipient.
URBAN METAL FLOWS – A CASE STUDY OF STOCKHOLM 19

Figure 5. Mercury flows to soil, sediments, sewage sludge and solid waste (kg y−1 ) from different
metal emission sources in Stockholm, 1995. WTP Waste water Treatment Plant. For further details –
see text.

7. Conclusions

The metal stock of Stockholm is large and still growing for Cr, Cu, Ni, Pb, and Zn.
The large amounts of metals in the waste fraction totally dominate the outflow from
the city, and indicate a potential for an improved recycling. For major parts of the
stock, the emissions from goods in use are negligible. There are, however, goods
applications corresponding to significant emissions: e.g. the traffic sector (Cu, Zn,
Cr, Ni, Pb), the tapwater system (Cu), roofs/fronts or other metal surfaces (Cu,
Zn). In contrast, the present emissions from solid waste management (incineration,
deposits) are most limited. Thus, even if the total metal stock of Stockholm is large
and still growing, only a minor fraction may cause environmental problems under
existing conditions.
Today’s known metal flows from the anthroposphere of Stockholm to the bio-
sphere and sewage sludge are quantitatively dominated by Zn (34 ton y−1 ) and Cu
(14 ton y−1 ) followed by Pb (3 ton y−1 ), Cr and Ni (1 ton y−1 each). For Cd and Hg
the corresponding flows are approximately 50 and 20 kg y−1 respectively. However,
these are minimum levels as some potential sources have not been quantified due
20 B. BERGBÄCK, K. JOHANSSON AND U. MOHLANDER

Figure 6. Nickel flows to soil, sediments, sewage sludge and solid waste (ton y−1 ) from different
metal emission sources in Stockholm, 1995. WTP Waste water Treatment Plant. For further details –
see text.

to lack of data, e.g. paints (especially Zn) or secondary emission sources of Hg


in polluted soils or in deposits in the waste water system. For all seven metals,
diffusive emissions from goods in use are major sources.
The magnitude of the known metal flows to sediments via ground-, storm- and
waste water are in agreement with the estimated anthropogenic deposition rates
for Cu, Cr, Ni and Zn, indicating that major emission sources probably have been
identified. However, for Cd, Hg and Pb historical emission sources still are import-
ant giving a higher deposition rate to sediments via unidentified pathways. Thus,
to assess present and future metal load, a historical time perspective is needed.
Historical and present emissions have resulted in high metal concentrations in
sediments (especially Cd, Hg and Pb, but also Cu and Zn), groundwater (Cu, Hg)
and in soils (Hg, Cu, Pb). To assess the environmental risk, the bioavailability has
to be considered.
According to known or calculated metal flows and concentrations, some areas
with a possible resource and/or environmental impact must be considered: sewage
sludge, soils and sediments/ water recipients.
URBAN METAL FLOWS – A CASE STUDY OF STOCKHOLM 21

Figure 7. Lead flows to soil, sediments, sewage sludge and solid waste (ton y−1 ) from different metal
emission sources in Stockholm, 1995. WTP Waste water Treatment Plant. For further details – see
text.

A significant part of the anthropogenic emissions end up in sewage sludge. At


present the annual median concentrations are below the Swedish limits for metals
in sludge, even if the safety margins are small for Cd, Hg and to some extent Cu.
Thus, present and future recycling of valuable nutrients may be limited, especially
when considering possible future demands of lower limit values. Major inputs for
Cu to the sewage sludge are from the tap water system and for Cd car washes,
faeces and artists paint are the dominating sources. The contributions to sludge Hg
from dental use and previously mentioned deposits in the waste water system are
hard to estimate, but both are probably significant sources.
The flow of Cu and Zn to Stockholm soils is high with a significant accumula-
tion indicating a possible environmental impact in a longer time perspective. Today,
the environmental impact is mainly limited to soils close to roads with elevated
concentrations of especially Pb and Cu. Here, indications of decreased microbial
activities have been found (c.f. Bringmark, 2001). However, the concentrations of
Cu, Hg, Pb and Zn in the central parts of Stockholm are enhanced 2 (Cu, Zn), 4
(Pb) and 6 times (Hg) to at least 30 cm depth compared to park soils outside the
city centre. For Hg, the enhancement probably reflects various historical uses for
more than 200 yr, while most of the Cu, Pb and Zn enhancement may be connected
to the traffic sector. The previous use of leaded gasoline and the present use of ZnO
22 B. BERGBÄCK, K. JOHANSSON AND U. MOHLANDER

Figure 8. Zinc flows to soil, sediments, sewage sludge and solid waste (ton y−1 ) from different metal
emission sources in Stockholm, 1995. WTP Waste water Treatment Plant. For further details – see
text.

in rubber are major sources of Pb and Zn. The Cu emissions mostly derive from
brake linings were Cu or brass is a major component, resulting in approximately
4 tons of Cu annually emitted in Stockholm. Thus, reduced Cu and Zn emissions
from the traffic sector are needed to prevent future accumulation in urban soils.
High levels of metals in surface sediments reflects an ongoing input where these
metals are transported from known (Cu, Zn) and/or partly unknown (Cd, Hg, Pb)
sources. The yearly deposition rates to sediments culminated in the 1970s, but
present rates are still high compared to the 1920s. Effects on biota are probably
limited as long as the metals are immobilised in the sediments. However, the high
concentrations of especially Cd, Hg and Pb indicate that altered redox conditions
due to e.g. dredging or a decreased euthrophication may drastically increase the
bioavailability of the metals. The ongoing reduction of the discharge of phosphor-
ous and nitrogen to the waters surrounding Stockholm will most certainly result in
an increased concentration of Hg in fish in this area. Obviously, metals transported
to and from sediments may elevate the concentrations in the water body.
From the results of this research programme a scenario can be made in order to
achieve a sustainable use of metals: In future urban areas, Cd and Hg are phased
URBAN METAL FLOWS – A CASE STUDY OF STOCKHOLM 23

out; the Pb use is restricted to a few applications, e.g. radiation protection; Cr, Cu,
Ni and Zn are still used but in applications that do not cause harmful effects not
even in a long time perspective and with a high recycling potential. Finally, mon-
itoring of metal flows are performed both in the anthroposphere and the biosphere
in order to have a pro active approach to urban environmental problems and to get
prompt answers to measures taken.

Acknowledgements

Financial support was provided by the Swedish Environmental Protection Agency,


the Stockholm County Council and the City of Stockholm.

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