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DOCTORA L T H E S I S

Pit Lakes from Sulphide Ore Mining, Geochemical and


Limnological Characterization before Treatment, after
Liming and Sewage Sludge Treatments

MING LU
Lule University of Technology
Department of Chemical Engineering and Geosciences
Division of Applied Geology
:|: -|: - -- --

Pit Lakes from Sulphide Ore Mining, Geochemical and


Limnological Characterization before Treatment, after
Liming and Sewage Sludge Treatments
cases studies at Rvlidmyran and Udden, Sweden

MING LU

Department of Chemical Engineering and Geosciences


Division of Applied Geology
Lule University of Technology
SE-971 87 Lule, Sweden

Never put off till tomorrow


what you can do today
Lord Chesterfield, 1749

ABSTRACT
Due to the increasing number of acidic mining-pit lakes and a growing awareness of the
environmental risks associated with them, pit lakes have attracted more and more attention. This
study started with a full-year-round investigation of two abandoned sulphide mine pit lakes, the
Rvlidmyran and Udden pit lakes in northern Sweden, followed by studies of two full-scale
remediation treatments, liming and sewage sludge treatment, respectively, in the Rvlidmyran pit
lake. The aim of this study is to understand the geochemistry of pit lakes and the factors
influencing pit lake water quality. Based on this knowledge, effects of different remediation
methods are investigated and possible improvement of these methods is explored. Furthermore, the
possibility of manipulating the pit lakes to obtain efficient metal attenuation is also explored in this
study. The results showed that these two pit lakes have some common characteristics; they have
low pH, they are oligotrophic and have high metal and sulphate contents. However, they have
developed distinctly different limnology and geochemistry. Rvlidmyran is a meromictic lake,
which has a rather stable stratification due to more saline groundwater inflow at depth. Three
layers have been developed: the mixolimnion at the top, in which the water is well mixed and
saturated with oxygen; the monimolimnion in the deeper lake, which is poor in oxygen and which
does not mix with upper water; and the chemocline, which separates the upper and deeper water.
The distribution of elements such as Ca, Mg, Na, K, S, Mn, Fe and Zn is seen to be strongly
controlled by the stratification with lower concentrations in the upper layer and higher
concentrations in the deeper water. The Udden pit lake is a dimictic lake without permanent
stratification; only seasonal thermal strata develop. The water is well mixed, which results in rather
uniform distribution of parameters such as pH, dissolved oxygen, conductivity and elemental
concentrations. It is concluded that a careful characterization of the limnological situation of a pit
lake is very important, both for designing reasonable remediation treatment methods or being able
to use pit lakes for disposal of contaminants such as mine waste. Rvlidmyran was chosen for fullscale studies of remediation. Liming treatment proved to be an effective method with respect to
increased pH. The effects of the liming on the dissolved elemental concentrations in the lake water
were distinct, especially in the upper oxic water layer. Elements such as Fe, Mn, Zn and Mg were
largely removed in the upper oxic water, probably due to formation of oxyhydroxides. Some
elements such as Na, K and S were barely influenced. Al and Cu were almost completely removed
from the water throughout the profiles, due to pH increase and precipitation of minerals such as
gibbsite [Al(OH)3]. Sorption of Cu was probably removed from the water by to gibbsite and Feoxyhydroxides, since pH was rather high. However, liming is not a long-term solution as long as
the acidic sources flow continuously into the lake. Therefore, the liming effect will not last long
and it will be rather costly to continue liming. The sewage sludge treatment did not show distinct
effects on the water quality during the monitoring period. However, particulate elemental
concentrations were influenced, especially during the early stages of the treatment. Concentrations
of total organic carbon increased in the water column after sewage sludge treatment. However,
most of the organics and nutrients settled rapidly and accumulated at the lake bottom.
Key words: pit lake, aqueous geochemistry, acid mine drainage (AMD), sulphide minerals,
liming, bio-remediation, sewage sludge, sulphate-reducing bacteria (SRB)

LIST OF PAPERS
This thesis comprises the following five papers
I.

Lu M., Carlsson E. and hlander B., 2002, Aqueous geochemistry of pit lakesa case
study at Rvlidmyran, Sweden. Accepted by Applied Geochemistry.

II.

Lu M., Carlsson E. and hlander B., 2002, Aqueous geochemistry of pit lakesa case
study at Udden, Sweden. Submitted to Mine Water and the Environment.

III.

Lu M. and hlander B., 2004, Effects of liming a sulphide mining pit lake. Manuscript.

IV.

Lu M. and hlander B., 2004, Remediation of a sulphide mining pit lake by sewage
sludge a full scale experiment at Rvlidmyran, Sweden. Manuscript.

V.

Lu M., Widerlund, A and hlander B, 2004, Liming of acid mine water, field scale
studies of a tailings impoundment and a pit lake. Manuscript.

During my postgraduate studies the following paper has also been written. However, it is not
included in my doctoral thesis
Lu M., Carlsson E. and hlander B., 2003, Limnological and geochemical comparisons of two
sulphide mine pit lakes. In: Tailings and Mine Waste03. Proceedings of the Tenth International
Conference on Tailings and Mine Waste, Vail, Colorado, USA, 12-15 October 2003, pp.201-212.

TABLE OF CONTENTS
1 BACKGROUND.............................................................................................................................1
2 INTRODUCTION...........................................................................................................................2
2.1 Acid Mine Drainage .................................................................................................................2
2.2 Open pit mining and pit lake formation ...................................................................................3
2.3 Pit lake characterization ...........................................................................................................4
2.4 Remediation of pit lakes...........................................................................................................6
2.5 Possibility of using pit lakes.....................................................................................................7
3 SCOPE OF THE THESIS ...............................................................................................................8
4 SITE DESCRIPTIONS ...................................................................................................................8
5 METHODOLOGY........................................................................................................................10
5.1 Sampling and treatment methods ...........................................................................................10
5.2 Analysis methods ...................................................................................................................12
5.3 Geochemical modelling..........................................................................................................13
6 AQUEOUS GEOCHEMISTRY STUDY OF PIT LAKES ..........................................................13
6.1 Rvlidmyran Pit Lake.............................................................................................................13
6.2 Udden Pit Lake.......................................................................................................................15
7 REMEDIATION OF PIT LAKE ..................................................................................................17
7.1 Liming treatment ....................................................................................................................17
7.2 Sewage sludge treatment........................................................................................................20
8 CONCLUSIONS AND PERSPECTIVES ....................................................................................21
9 ACKNOWLEDGEMENTS ..........................................................................................................24
10 REFERENCES:...........................................................................................................................25

1 BACKGROUND
Sweden is a major metal mining country in Europe, and mining operation in Sweden has a long
tradition of more than 1000 years. Swedish has for many years been one of the major suppliers of
steel, copper, and silver to the Europe (Gustaffsson et al., 1999). Today, Sweden is still the leading
metal producer within the European Union (EU). For example, in 2002, Sweden produced about
92% of the total European Union iron production, 62% of the production of silver, and 44% of the
production of copper, 43% of the lead, 33% of the gold, and 23% of the Zn (SveMin, 2003).
Most of the ore deposits are situated in sparsely populated areas with a sensitive nature of high
ecological and recreational value. Currently, significant exploration takes place in Sweden, which
opens new possibilities for mining operations (MiMi, 2001). About 35 million US $ are invested in
prospecting in Sweden annually (Weihed, 1999). Opening of new mines is likely to be the results
of some of these activities. However, mining activities are always associated with conflicts
between development and environment issues including competition of land uses, fugitive dust,
large amounts of mine wastes etc.. The potential environmental impacts from mining and mining
waste generally do not end when the mining activities end. To meet stricter environmental
requirement, the costs for mining industries to control the environmental impact from the
operations and waste deposits in both short and long terms become higher. This increases the cost
of mining. Therefore, finding appropriate methods which supply metals securely and with efficient
waste remediation is a prioritised area.
Deposition of mining waste is especially important due to the enormous quantities generated and
the long-term security considerations needed. For example, approximately 250 million tons of
waste rock and 400 million tons of tailings from mining of sulphidic ores have been generated in
Sweden. Additionally 13 million tons waste rock and 22 million tons of tailings are added each
year (Naturvrdsverket, 1998). Moreover, sulphidic mine waste may result in the formation of acid
mine drainage (AMD). The demand of safe disposal of mine waste over long periods initiated the
MiMi (Mitigation of the Environmental Impact from Mining Waste) program
(http://www.mimi.kiruna.se). This is a program funded by the Swedish Foundation for Strategic
Environmental Research (MISTRA) and it is coordinated together with the Swedish mining
companies Boliden and LKAB. The program stated in 1998 and closed in 31st of December 2003.
The goal of the MiMi program is to devise safe methods for the disposal of mining waste and for
the reliable prediction of their function over long periods of time (MiMi, 2001). The project
consists of several sub-projects which cover different areas including soil-covered tailings, watercovered tailings, biogeochemical barriers, co-disposal technique, wetlands as metal traps, and
natural attenuation in surface water systems. The study of this thesis is a sub-project within the
projects Near Field Methods and tools for optimized water cover and Far Field Development
of biogeochemical barriers for passive leachate treatment.

2 INTRODUCTION
2.1 Acid Mine Drainage
Possible impacts of mining activities to the environment have gained more and more interest the
last decades. The effects can be revealed in many aspects. Visually, mining operations change the
topography of the land surface. Different mining operation methods may result in either surface
disturbances or underground influences that may affect surface topography (Allgaier, 1997). Far
more important, the effect of mining activities on hydrological regimes has attracted more interest
and has been well studied at many locations. One of the major threats is mine drainage water,
especially acid mine drainage water. Acid mine drainage (AMD) is typically produced by the
exposure of iron sulphide minerals to air and water, resulting in the oxidation of sulphur and the
production of acidity and elevated concentrations of sulphate and metals (Allgaier, 1997; Banks et
al., 1997). Iron sulphides, such as pyrite (FeS2) and pyrrhotite (FeS), are generally contained in
coal, overburden, sulphide ores, and associated waste rock and processing wastes. Dissolved Fe2+,
SO42- and H+ are released when these Fe-sulphides are oxidised. Under most conditions, pyrrhotite
is found to be more easily oxidised (Nicholson and Scharer, 1994). Acid mine drainage may come
from open pits, runoff and leachates from waste rock dumps, mill tailings and ore piles etc. It has
been well understood that oxidation of pyrite and pyrrhotite is a complex process involving several
steps. Taken pyrite oxidation as an example to illustrate the reactions of acid generation, pyrite is
firstly oxidised by oxygen and water to produce ferrous iron, sulphate and acid (Langmuir, 1997):

7
2
FeS 2 ( Pyrite) + O2 + H 2 O Fe 2+ + 2 H + + 2 SO4
2

(1)

In a sufficiently oxidizing environment, ferrous iron may be oxidised to ferric iron and then ferric
iron will precipitate as iron oxyhydroxide (FeOOH) and/or iron hydroxide (Fe(OH)3) (Stumm and
Morgan, 1996):

1
1
Fe 2+ (aq ) + O2 (aq ) + H + (aq) Fe 3+ (aq ) + H 2 O
4
2

(2)

Fe 3+ (aq ) + 2 H 2 O FeOOH ( s ) + 3H + (aq )

(3)

These reactions further lower the pH. However, reaction 2 is a slow process and Fe may remain in
the reduced Fe(II) state for quite some time under the acidic condition of pH 4 (Nordstrom and
Munoz, 1994). Therefore the rate of pyrite oxidation, is in fact, limited by the availability of Fe3+,
which itself depends on the Fe2+ oxidation rate. Thus, reaction 2 is considered the rate-determining
step in the formation of AMD (Kleinmann et al., 1981; Langmuir, 1997). However, studies
(Nordstrom et al., 1978) show that with the presence of the acidophilic iron-oxidizing bacterium
such as T. ferrooxidans and other related species which biotically catalyze the reaction, the rate of
Fe2+ oxidation is accelerated many times and it is fastest at pH of around 2-3 (Banks et al., 1997;
Knapp, 1987).

Moreover, without oxygen involvement, trivalent ferric iron in solution will itself oxidize pyrite:
2

FeS 2 + 14 Fe 3+ + 8H 2 O 15Fe 2+ + 2 SO4 + 16 H +

(4)

Oxidation of other sulphides, such as chalcopyrite (CuFeS2), sphalerite (ZnS) and galena (PbS),
may also either directly oxidized in the presence of air and water catalyzed by bacteria or
indirectly by ferric iron as either Fe3+ or ferric sulphate(Hutchison and Ellison, 1992). Take
chalcopyrite (CuFeS2) as an example (Boon, 2000):
CuFeS 2 + 4O2 Cu 2+ + Fe 2+ + 2 SO4

(5)
2

CuFeS 2 + 16 Fe 3+ + 8H 2 O Cu 2+ + 17 Fe 2+ + 2SO4 + 16 H +

(6)

In contrast to pyrite oxidation, no acid is formed in the oxidation process by reaction 5. Due to
formation of AMD, it is nowadays realised that sulphide-bearing waste should be remediated in a
way that decreases the inflow of oxygen (Hglund et al., 2004). From this consideration, mining
waste either is capped by material with low permeability often various soils, so called dry cover, or
is flooded by raising groundwater or surface water to establish a permanent water cover (Ritcey,
1989).

2.2 Open pit mining and pit lake formation


In this study, acid mine water open pits were studied, so called pit lakes. Pit lakes are unique water
bodies, formed by water infilling of open pits after cessation of mining. Once pit lakes form, they
become complicated systems which interact with surrounding environments and show internal
reactions within the system. The formation of an open-pit is due to open casting mining, which is
an economical way of near surface ore deposits recovery (Lowrie, 1997; Pillard et al., 1996). The
mine-out pit is usually an inverted cone shaped opening with numerous equally spaced narrow
benches. The pit can be very large since in order to reach deeper, it has to be expanded. An
example of famous pit lake is Berkeley Pit in Montana, U.S.A., which is 542 m deep and has a
surface area of 2.5 km2 (Davis and Ashenberg, 1989).
During active mining, water is controlled by perimeter pumping and/or in-pit pumping (Tyler and
Beale, 1991), thus it is possible to excavate material below the original water table. When open
pits are completed, they may be backfilled with mining materials which eliminate the formation of
an open pit lake. However, in some cases, back-filling an open pit may be unpractical and costly
(Allan, 1995). Therefore, the pits may be left open and allow inflow of groundwater and surface
water to fill up the pit. A steady water surface will be established when the lake surface recovers to
the local groundwater table. Eventually, an artificial lake is formed. The time to establish a steady
state in the pit lake depends on the water balance. Studies have shown that it is important to be
able to predicte the filling rate to a pit in support of the geochemical modelling of the steady-state
water quality of pit lakes (Lewis, 1999; Marinelli and Niccoli, 2000; Shevenell, 2000a). However,
since pit lakes relatively recently have gained interest, the work that has been conducted to address
this issue is limited.

2.3 Pit lake characterization


During open pit mining, since the rocks in the pit walls are exposed to the atmosphere they
weather. AMD is also possible to generate from an open pit (Figure 1). A potential problem arises
when the pit is back filled with water. Pit lakes may contaminate adjacent areas by drainage waters
if the lake water is contaminatd. Pit lakes may have very large water volumes. Therefore, along
with the inevitably increased number of pit lakes, they have attracted more attention during recent
years.
Quite several works have been performed to investigate the limnological and geochemical
characters of a pit lake (Campbell and Lind., 1969; Castendyk and Jewell, 2002; Castro, 1998;
Davis and Ashenberg, 1989; Doyle and Runnells, 1997; Klapper and Geller, 2001; Levy et al.,
1996; Lu, 2002; Lyons, 1994; Miller et al., 1996; Shevenell, 2000b; Stevens and Lawrence, 1998;
Tass, 2003). Based on the knowledge obtained by case studies, attempts have been performed to
construct models in order to predict pit lake water quality (Davis and Eary, 1997; Eary, 1999;
Hamblin et al., 1999; Kempton et al., 2000; Lewis, 1999; Marinelli and Niccoli, 2000; Morin and
Hutt, 2001; Pillard et al., 1996; Shevenell, 2000a; Tempel et al., 2000).

Rainfall infiltration
Surface water
runoff
Post-mining
groundwater table

AMD runoff

AMD seepage

Ground
water flow

Pre-mining
groundwater
table

Surface and ground water flow


through sulphide rock debris
Water that collects in the bottom of the
pit is lost by a combination of seepage,
evaporation and surface discharge

Residual
sulphides

Figure 1 Conceptual illustration of showing typical conditions under which AMD can form in
an open pit mine. Sulphide rock inherent in open pits is exposed to air and infiltration after
lowering the groundwater table may generate AMD. Redrawed according to Hutchison and
Ellison (1992)

To summarise these studies, pit lakes have some common characteristics, and compared to natural
lakes, pit lakes are rather unique water bodies:

They normally have higher relative depth (the percentage ratio between maximum
depth of the lake and the mean diameter), in the range of 10-40%, while natural lake
generally have less than 2 % (Doyle and Runnells, 1997; Hamblin et al., 1999; Levy et al.,
1996; Lyons, 1994).

Due to that the history of these lakes is rather short, the sediment layers are thin. In
some cases, the sediments are just a loose, unconsolidated sludge (Lu et al., 2003; Stevens
and Lawrence, 1998).

During the formation, the lakes may undergo substantial and rapid changes in water
level considering the formation history (Boehrer et al., 2003; Ramstedt, 1999; Shevenell et
al., 1999).

Solutes are released into the lake water by weathering of the wall rocks and of other
exposed rocks in the surrounding drainage waters. Therefore, pit lake waters are likely to
contain significantly elevated concentrations of metals. If the lake originated from coal or
sulphide ore mining, the lake can be acidic and the water also contains higher
concentrations of sulphate and toxic metals (Bachmann et al., 2001; Davis and Ashenberg,
1989; Geller et al., 1998; Levy et al., 1997; Miller et al., 1996).

The final pit slopes are usually quite steep (e.g. 45-50 degrees) (Lowrie, 1997).
Therefore, pit lakes normally have high surrounding walls and a steep littoral zone which
may generate microclimate different to that outside the pit (Stevens and Lawrence, 1998)

Most pit lakes lack shorelines or shallow water areas, so submerged rooted
biological communities do not likely develop (Lyons, 1994). Primary productivity is
generally low in pit lakes as well as biological activity (Doyle and Runnells, 1997; Friese
et al., 2002; Lyons, 1994)

A pit lake is a complicated system and many factors may influence the final water quality and
as time goes, the lake also undergoes aging process (Campbell and Lind., 1969; King et al.,
1974). The geochemical situation in a pit lake may evolve with time. Factors which may
influence pit lake water quality can be summarised by the following four major aspects:
Mineralogical factors
The mineralogy of pit walls is relatively important for controlling the evolution of pit
lake chemistry. For example, rocks containing iron sulphides generally produce acid
lakes with high level of sulphate and dissolved metals due to oxidation when minerals
previously exposed to oxidizing conditions during dewatering release sulphuric acid and
metals when they later are flushed with the rising water. If the water is in contact with
calcite (CaCO3) and dolomite [CaMg(CO3)2] in the wall rock, the acidic water may be
naturally neutralised, and water in that case is likely to present better quality.

Hydrological factors
Hydrological factors also strongly influence potential lake water quality and chemistry.
Pit lakes derive water from several pathways including groundwater infiltration, surface
runoff from drainage precipitation, and direct precipitation to lake surface. In most cases,
contributions from the later two are small compared to the inflow of groundwater (Lewis,
1999). Evaporation, groundwater outflow and surface water outflow are the possible
pathways that pit lakes lose water. It is supposed that the composition of a pit lake
should be a function of the flux and chemistry of these flows in combination with
processes taking place within the lake. For example, in an arid area, effects of net
evaporation could become an important process affecting long-term water quality (Eary,
1998). Moreover, if groundwater flows through highly permeable rock zone, the water
chemistry would be different compared to if water filling the pit flows evenly through
the wall and bench rocks (Pillard et al., 1996). Good quality of inflowing groundwater
tends to improve the pit lake water quality.
Limnological factors
Limnological factors, such as wind fetch, latitude, light penetration, relations to the
groundwater table, methods of flooding and morphology of the pit are also important in
affecting the water quality at a pit lake and its evolution. For example, the fetch and the
morphology of the pit may determine if turnover may occur in the lake (Wetzel, 1983).
Overturning in a pit lake is an important issue since it may change the oxygen saturation
situation in a lake water column. Elements such as Fe, Mn, which are sensitive to redox
changes will be influenced. This may subsequently change the concentration of other
elements. Therefore, the equilibrium conditions in the lake are modified. As a result, the
lake water quality changes.

2.4 Remediation of pit lakes


Although water in an acid pit lake is also a kind of acid mine drainage, in situ treatment is more
complicated in a pit lake than to drainage waters from waste deposits. Simple neutralization by
addition of bases, such as lime, caustic soda and other alkaline materials, is proven to be a
successful method in some cases (Fischer and Guderitz, 1996; Lewis et al., 2003). However, it is
rather costly and if there is high availability of acidic sources, base neutralization will not be a
long-term solution.
Since these lakes often have high relative depth, poor circulation, and a steady anoxic layer at
depth, the recovery could be stimulated by adding organics to create bacterially mediated
neutralization. Such ideas have been adopted in treating acid mine drainage water (AMD), either
by building up anaerobic bioreactors in a passive treatment to AMD (Logan et al., 2003; Seyler et
al., 2003), or diverting AMD through a natural or man-made wetland (Wildeman et al., 1993;
Wildeman and Pavlik, 2000). Also, in field experiments, it has been successfully demonstrated on
a small stream in Ohio (Tuttle et al., 1969). Moreover, numerous laboratory studies have also
revealed that application of sulphate-reducing bacteria (SRB) could be a solution (Castro et al.,
1999; Elliott et al., 1998; Fauville et al., 2004; Ueki et al., 1991).

No matter which way, the mechanism behind the treatments is basically the same. That is to use
sulphate-reducing bacteria, which is a term describing a rather heterogeneous assemblage of
microorganisms having in common merely dissimilatory sulfate metabolism and obligate
anaerobiosis, to biodegrade sulphate and precipitate metals. The best-known and most widespread
sulphate-reducing genera are Desulfovibrio, Desulfotomaculum, and Desulfomonas (Postgate,
1984). SRB gain energy for growth by coupling oxidation of organic compounds of hydrogen with
the reduction of sulphate to sulphide (Zehnder, 1988):

SO4

bacteria
+ 2CH 2 O + 2 H + anaerobic

2CO2 + H 2 S + 2 H 2 O

(7)

Reduced sulphur precipitates metals as sulphide minerals. For iron, as an example, microbial
reduction of ferric iron will occur and the ferrous iron may be precipitated as a sulphide mineral.
The net effect of these processes is that acidity in the water is partially neutralized and metal
concentrations decrease:

CH 2 O + 4 FeOOH + 8 H + CO2 + 4 Fe 2+ + 7 H 2 O

(8)

Fe 2+ + H 2 S FeS + 2 H +

(9)

The key to the process is the accretion of enough organic debris at the bottom of the lake to allow
bacterial activity to generate suitably reduced conditions for SRB (Campbell and Lind., 1969). The
formed sulphide minerals are rather stable if the biological activity in the lake will be selfmotivated and sustained. Stimulation of sulphate-reducing bacteria by addition of organic nutrients
could potentially be a cost-effective means of dealing with these contaminated waters. It may be a
long-term solution. In fact, it has been observed that the recovery of an acid mine lake could be a
natural succession process resulting from a gradual decrease in acid production by spoils and
leachates from unmined portions of the watershed (King et al., 1974). It has also shown that
compared to lakes that have access to leaves and grass, the ones that have little input of terrestrial
organic material show little recovery (Campbell and Lind., 1969; King et al., 1974). Therefore,
good water quality could be achieved if one or more of the following condition occurs: low pyrite
availability, high carbonate availability, and/or large input of organic matter and inorganic
nutrients.

2.5 Possibility of using pit lakes


In remediation of mining waste, a common thought is to control oxygen diffusion. Since the
diffusion of oxygen in water is about four orders of magnitude slower than in air, a water cover
will reduce the amount of oxygen that the mining waste may be exposed to. However, the major
problem with water cover is the physical stability of the dam in flooded ponding and fluctuating
water level. In shallow water covers, wind driven turbulence may increase the supply of oxygen,
and resuspension of sulphides in water covered tailing ponds may lead to increased sulphide
oxidation. Therefore, the alternative to submerge mine tailing in natural lakes has been suggested
since there are no problems with dam stability in this case. This method has been proven to be
feasible by a study in Anderson Lake, Manitoba, Canada (Pedersen et al., 1993), which is a small,

shallow and eutrophic lake which received high-sulphide tailings from a mill nearby. Currently,
there is no indication that the tailings on the lake floor are releasing metals to the overlying lake
water. It is expected that in the future, the metal-rich deposits will be progressively blanketed by
an organic-rich veneer, which has been seen occurring at some sites of the lake. The addition of
natural organic-rich cover should ensure that the tailing may be stored in a stable anoxic state for
the foreseeable future.
However, there has also been an increasing interest to explore the feasibility of using pit lakes as
effective containment for contaminants (Allan, 1997; Brassard et al., 1996; Klapper and Geller,
2001). Suggestions that pit lakes could become assets instead of a horror (Castro and Anonymous,
2000) arises. Due to the unique limnological and geochemical situation in pit lakes, thoughts to use
pit lakes as a containment of mine waste such as mine tailing, have been discussed. The main
argument is that, due to the unique morphological characters, pit lakes could develop into
meromictic lakes. As a result, a rather steady anoxic layer develops in the deeper parts of a lake. If
the there is saline groundwater inflow at depth, this may strengthen the stratification. Subaqueous
disposal of mine tailings into pit lakes may prevent tailings oxidation. There have been several
cases such as the Crown Pillar pit at the former Mattabi Mine, Ontario, and Island Copper pit lake,
which have been used for tailings conservation and they seem to be successful up to now (Brassard
and Mudroch, 1994; Poling et al., 2003).

3 SCOPE OF THE THESIS


At present, there exist more than twenty pit lakes in Sweden and most of them are concentrated in
northern Sweden. These lakes mostly originated from sulphidic base metal mining. Up to now, few
studies have been performed to study these special water bodies in Sweden. The evolution of water
quality, the geochemical process in the lakes, their long-term impacts on down-gradient
groundwater quality, their ecological risk and some other environmental issues are all not well
understood. For these reasons this study was initiated.
The first objective of this thesis was to understand the potential problems from the pit lakes
themselves. For this reason, investigations of geochemistry and limnology of pit lakes were
performed. The results are presented in Papers I and II. Remediation methods of pit lakes
including active chemical treatment (liming) and passive treatment (bio-remediation by sulphatereducing bacteria) were tested, which are presented in Papers III and IV. Furthermore, Paper V
also compares the liming effect on a pit lake and water covered tailing impoundment. In the thesis,
the possibilities of using pit lakes as water cover for mine waste are also investigated.

4 SITE DESCRIPTIONS
Rvlidmyran Pit Lake is located in about 180 km southwest of Lule. The ore belongs to the 1.9
Ga old Skellefte ore district of Northern Sweden (Figure 2). The Kristineberg mine is situated 5 to
the east, and Rvliden mine lies 3 km to the south. Rvlidmyran ore is of replacement type
occurring in a limestone environment, and it is pyrite-rich with 4.12% Zn, 0.98% Cu, 0.67% Pb,
and 23.4% S. It also contained about 0.6 g/t Au and 48 g/t Ag (Boliden, 1975). Mining activities in
8

the Rvlidmyran area were first started in 1953, and the ore was mined by both open pit and
underground mining. In 1974, mining at the Sture pit ceased and the open pit was filled up with
water (Boliden, 1975). Nowadays, the pit has formed a lake with a surface area of 49 191 m2, and
a volume of 526 904 m3. The maximum depth of the lake is 28.9 m and the average depth is 10.7m.
The relative depth of the lake is 12%.

Figure 2 Rvlidmyran mine location map. The mining area comprises three parts. A-Industrial
area and some backfilled smaller open pits; B-Sture ore, which formed the present
Rvlidmyran Pit Lake; C-waste rock dump-site covered by till and planted with grass
(Boliden, 1975).

Udden Pit Lake is situated approximately 30 km west of Boliden in northern Sweden (Figure 3).
The Udden ore deposit was part of the Skellefte district 1.9 Ga old volcanic series. The principle
sulphide minerals at Udden were pyrite (FeS2), pyrrhotite (Fe1-xS), sphalerite (ZnS), chalcopyrite
(CuFeS2), galena (PbS), and arsenopyrite (FeAsS). The average grade of the ore was 0.8 g Au/ton,
s0.41% Cu, 4.72% Zn, 0.35% Pb, 0.1% As and 25.6% S. The mining in Udden started in 1971
with an open pit. After three years the surface deposit was depleted and the mining operations
continued under ground. In 1991, mining ceased and the pit was filled up rather rapidly with
groundwater. Nowadays, the open pit forms an approximately 390 m long and 150 m wide,

maximum 50 m deep lake. The lake contains about 5.6105 m3 water and the surface area is about
3.4104 m2. The relative depth of the lake is calculated to be 24%.
There is no surface water inlet to none of the two lakes. The most possible water sources to the
lakes are precipitation, surface runoff, snowmelt and groundwater. The lakes may lose water
through evaporation, groundwater outflow and fluvial outflow, which is only seen on Udden Pit
Lake.

Figure 3 Udden mine location map. The mining area composes three parts: Industrial area
A; Open pitB which formed the present Udden Pit Lake and there is an outlet at the east
bank of lake; and Waste rock deposit areaC, which is covered by till and planted by grass
and trees (Boliden, 1990).

5 METHODOLOGY
5.1 Sampling and treatment methods
In the stage of pit lake geochemistry and limnology investigation, sampling was performed six
times to cover typical seasonal variations. First sampling started at the end of April, 2001 when the

10

lakes were still ice-covered; then the sampling continued in May, after ice melt; in June and
August for summer; the end of October for autumn and middle of March, 2002. For Rvlidmyran
Pit Lake, eight or nine samples were collected during each sampling, including the depths 0.5 m, 2
m, 5 m, 8 m, 10 m, 15 m, 20 m, 23 m and around half meter above the bottom. For Udden Pit Lake,
nine to ten samples were collected on each sampling occasion, including the depths 0.5 m, 2m, 5m,
10m, 15m, 20m, 30m, 40m, 45m and around half meter above the bottom.
Rvlidmyran Pit Lake was chosen to perform liming and sewage sludge treatments. From the mine
closure in 1974 until spring 2003, the lake was left without any treatment until May 2003, when
the lake was limed with 200 tonnes of lime [Ca(OH)2] within a three-week period. The lime
powder was pumped from a truck tank and injected into the lake through a pipe. One and half
month later, 300 tons of sewage sludge, which was transported from Stockholm Vatten, was
pumped into the lake.
Two additional samplings were performed in May 2003 during the liming period, and in June 2003,
one month after the whole liming treatment was finished. After sewage sludge treatment, a whole
year cycle sampling was performed. First sampling started one week after sludge pumping into the
lake. During the beginning of the experiment, sampling was performed twice a month. In winter,
since biological activity may be limited, the sampling frequency was reduced to only sampling in
December 2003, when the lake was ice-covered. The last sampling was performed in August 2004.
During the sewage sludge experiment, besides routine samplings at the regular location, samples
were also taken from two additional random sites on the lake to investigate the horizontal
distribution in the lake. It was found that the lake has very uniform horizontal distribution. All
three locations show very good agreement of physiochemical parameters and elemental
concentration profiles with each other, which indicates that horizontally, the lake is well mixed.
Therefore, measurements from the regular sampling location in this paper are used to represent the
situation of the whole lake. Results from other locations will not be shown here.
In both Rvlidmyran and Udden pit lakes, each time the samples were taken along the deepest
profile of the lakes. Before sampling, measurements including temperature, pH, conductivity,
dissolved oxygen (DO) and redox potential were performed in situ with a Hydrolab Surveyor II
water quality probe at each half-meter and/or one meter. Immediately after measurement, samples
were collected. A metal-free Ruttner sampler (1.7 l, Heraco AB) was used for collecting lake water.
Samples were immediately filtered through a Nitrocellulose filter (0.22 m, 25 mm , Millipore)
with a disposable plastic syringe (50 ml, Sartorius AG, Germany). About 60 ml filtered water was
saved in an acid-leached Azlon HDPE bottle (AnalyticaAB, Sweden) for dissolved phase
analysis. Throughout this paper, the term dissolved refers to material that passes a 0.22 m filter,
including truly dissolved species, as well as colloids (Kimball et al., 1995; Langmuir, 1997;
Stumm and Morgan, 1996). Another 120 ml, without acid-wash, was prepared following the same
procedure to be used for anion analysis. Filters were saved in petri dishes for particulate metal
determination. The water volume that filtered through was recorded in order to calculate
particulate element concentration. Both syringes and polycarbonate filter holders (25 mm ,
Sartorius AG, Germany) were pre-rinsed with acid (5% HNO3). Filters were also rinsed with 5%
Acetic Acid for 24 hours before the sampling.

11

Surface sediment from the pit lake floor was collected in May and June 2001 in both Rvlidmyran
and Udden pit lakes. Sediment samples were also collected during liming treatment and sewage
sludge treatment from Rvlidmyran Pit Lake. The samples were kept in bottles (Analytical AB,
Sweden) without headspace during transportation. Samples for organic carbon and nitrogen
analysis were stored in glass bottles. All the samples were kept in an icebox and were not exposed
to light during transportation.

5.2 Analysis methods


Water and filter samples were analysed by Analytica AB (Sweden). Dissolved metals including Fe,
Al, As, Ba, Cd, Co, Cr, Cu, Mn, Mo, Ni, P, Pb and Zn were measured using ICP-SMS (highresolution ICP-MS), and Ca, K, Mg, Na, S, Si and Sr were analysed by ICP-AES (Atomic
Emission Spectroscopy). Data were reported after three to four runs on each instrument. The
quality of the analyses was checked using synthetic standards. The precision determined in such
conditions as + one standard deviation was generally better than 5%. Four instrumental blanks
were also prepared and analysed as the samples.
Filters for particulate elements including Cu, Cd, Hg, Pb, Zn and S were dissolved with suprapur
HNO3 in closed Teflon bombs in a microwave oven, and then analysed by ICP-AES and ICP-SMS.
Filters for other elements including Al, Ba, Ca, Co, Cr, Fe, K, Mg, Mn, Na, P, Si, Sr and Zn were
wet-ashed in concentrated suprapur HNO3 in platinum crucibles at 75C, and then dry-ashed at
550C. The ashes were fused with lithium metaborate in graphite crucibles at 1000C. The formed
beads were dissolved in 10% suprapur HNO3 (Burman et al., 1978). The elements were then
determined by ICP-AES. For each method, four blank groups each containing four blank filters
were prepared. They were digested and analysed following the same procedure. Blank contribution
was calculated for each sample, and if it was less than 10%, the results were considered reliable. If
larger than 30%, the blank contribution was presumed to be too large and the result was unreliable
and therefore not considered. The results from the laboratory were reported as g total weight. If
divided by the filtered water volume recorded during sampling, the particulate element
concentrations can be reported as g/l.
Sediment samples were also digested following the same procedure as filter samples, except the
samples from 2001 in Rvlidmyran and Udden pit lakes, which was only digested by the leaching
process. Thus elements such as Si and Al are lost in this case. However, elements such as Cu, Zn,
Cd, Pb and S are comparable with the measurements of the 2003 and 2004 sediment samples in
Rvlidmyran Pit Lake. Part of the sediment samples were filtrated and dried in air. After drying,
the material was prepared for mineralogical analysis by X-ray diffraction (XRD) analysis. Samples
were measured over the range of 5 to 65 on a Philips XRD instrument using CuK radiation. Xray diffraction (XRD) analysis was performed on the samples from 2001 in both Rvlidmyran and
Udden pit lakes, June 2003 and September 2003 samples in Rvlidmyran Pit Lake.

12

5.3 Geochemical modelling


To identify the elemental speciation and potential precipitation reactions that may act to control
elemental concentrations in the lake, elemental species distribution and the saturation index (SI)
for solids were calculated by PHREEQC (Parkhurst and Appelo, 1999). Database phreeqc was
used for modelling. The species distribution is expressed as percentage ratio which is calculated by
dividing a certain species molarity with the total molarity of the corresponding element. The SI is
calculated by the following equation:
SI=log(IAP/Ksp)

(10)

where IAP is the ion activity product observed in solution, and Ksp is the theoretical solubility
constant at the field temperature (Parkhurst and Appelo, 1999). A positive SI indicates that the
solution is oversaturated with respect to a given solid phase, and the precipitation of this mineral
phase is theoretically thermodynamically possible. A negative SI indicates undersaturation. At
SI=0, the solution and the solid phases being considered are apparently in equilibrium. During
modelling, situ measured Eh value from the platinum electrode was input as the general redox
condition. However, there is no measurement to specific redox couples such as Fe2+/Fe3+. Since the
lake system may have not reached a redox equilibrium condition, it has to be stressed out that the
speciation and saturation index result given by modelling would be just used as assistant
consultable results (Lindberg and Runnells, 1984).

6 AQUEOUS GEOCHEMISTRY STUDY OF PIT LAKES


6.1 Rvlidmyran Pit Lake
The measurements in Rvlidmyran Pit Lake indicate that it has striking similarities with other
mining lakes in terms of low pH and high metals and sulphate contents. Rvlidmyran Pit Lake is
oligotrophic and meromictic. The water is poorly mixed and a permanent stratification has
developed in the lake. Three layers are identified in the lake; the mixolimnion, the chemocline and
the monimolimnion (Figure 4). The density difference between the mixolimnion and the
monimolimnion is a key factor that prevents water cycling in the lake. Relative depth is also an
important limnological factor.
Groundwater filling and stratification strongly control the elemental distributions in the lake. Most
elements such as Ca, Mg, Na, K, S, Mn, Fe and Zn have lowest and constant concentration in the
mixolimnion (Figure 5). Concentrations increase in the chemocline and keep rising in the
monimolimnion. These elements show quite similar behaviour in the water with strong
correlations. Groundwater is supposed to be the major source. Fe is rather low in the mixolimnion
but higher in the chemocline and the monimolimnion. This is probably due to oxidation reactions,
resulting in the Fe is removed from the mixolimnion. In the chemocline and the monimolimnion,
the environment becomes reduced, and Fe mostly occurs in dissolved phase as Fe2+. Cu and Al are
correlated. The highest concentrations are observed in the chemocline and in the monimolimnion
then decline. The adsorption of Cu on gibbsite [Al(OH)3] may occur (Lee et al., 2002) and this
13

process is important since it controls the Cu and Al concentrations in the lake. Other trace metals
such as Zn, Pb and As show rather high concentrations in the whole water column. Fe and Al
appear to be enriched in the surface sediment. However, Fe and Al oxyhydroxides could not be
observed by the XRD analysis. This could be due to these minerals are mostly in amorphous
phases. Quartz (SiO2) and albite (NaAlSi3O8) have very conspicuous existence in the sediment.

Fe mg/l

Conductivity (ms/cm)
0

mixolimnion

200

300

chemocline

chemocline
10

10

monimolimnion

Depth (m)

Depth (m)

100

mixolimnion

15

20

25

15

20

June
August
October
March

monimolimnion

June
August
October
March

25

30

30

Figure 4 Density stratification in Rvlidmyran


Pit Lake.

Figure 5 Concentration profiles of filtered


Fe in Rvlidmyran Pit Lake.

Scavenging process by particles is not supposed to be a significant factor controlling trace metal
distributions due to the low suspended particle concentration. The content of organic matter in the
water is low, and the small variation between seasons reflects the limited biological activity in the
lake. In deeper parts of the lake, even though the oxygen concentration becomes very low, the
redox potential is still higher than necessary for sulphate reduction. This is possibly caused by the
lack of organics, degradation of which may enhance the reducing environment. Thus, sulphate
reduction is not occurring. As a result, this also limits the formation of sulphides, thus precluding
an important precipitation of trace metals as metal sulphides.

14

6.2 Udden Pit Lake


The study of Udden Pit Lake also shows that it is similar to other mining lakes. The water is acidic
and the metal concentrations are relatively high. Udden Pit Lake is a dimictic lake. The lake
appears to be stratified in winter and summer. In spring and autumn, overturning occurs and the
whole lake circulates which leads to homogeneous distribution of most of the parameters. In
summer and winter the lake is thermally stratified. Three layers; the epilimnion, the metalimnion
and the hypolimnion, could be identified (Figure 6). The strata are not stable and the boundaries
and thicknesses varied with seasons. When stratified, the redox potential is lower in the upper
water and higher in the hypolimnion which is not usually seen in natural lakes. Drainage water rich
in Fe2+ results in the lower redox potential in upper water. Close to the bottom, water suddenly
becomes oxygen poor, conductivity increases and redox drops dramatically.

Fe mg/l

Temperature ( C)
4

10

epilimnion

10

metalimnion

12

14

10

10

Temp.-August
Temp.-October
Eh-August
Eh-October

20
25
30

15

Depth (m)

16

hypolimnion

35

15

Depth (m)

20
25
30
35

40

40

June
August
October
March

45
45

50
300

400

500

Eh (mV)

600

700

50

Figure 6 Thermal and redox profiles of Udden Pit Figure 7 Concentration profiles of filtered
Lake in August and October, 2001.
Fe in June, August, October and March,
2001-2002 of Udden Pit Lake.

Most of the elements have rather homogeneous distribution in the lake (Table 1). This is especially
true during the period when overturn happens. When the lake is stratified, variations mainly occur
in the top water and bottom water. Elements such as Ca, Mg, Na, K, S, Mn, Cu Al and Zn have
15

lower concentration in the epilimnion. Concentrations increase in the metalimnion and kept
constant in the hypolimnion. Fe shows a different distribution with higher concentration in the
surface water and lower in deeper water (Figure 7). This is especially true when the lake is
stratified. The distribution of Fe reflects redox potential strata much better than thermal strata. The
surface water has the highest dissolved Fe concentrations probably due to inflow of drainage water
from the waste rocks dump. This dissolved Fe is precipitated in deeper water where the redox
potential is higher. Moreover, dissolved S has stronger relationship with Mn than Fe, which
supports the precipitation of Fe. Fe is accumulating in the surface sediment. Dissolved Al shows
strong relationship with Cu, Zn and Cd. The adsorption of Cu on gibbsite and coprecipitation is
supposed to occur. Thus gibbsite is an important mineral since it may control both Al and Cu
concentrations in the lake. The decrease of elements such as Cu, Zn and Cd in the bottom waters is
probably an effect of the increased pH. Significant amount of Fe and Al are seen to accumulate in
the surface sediment. But still, their oxyhydroxides are not seen by XRD-analysis probably due to
the same reasons as in the Rvlidmyran Pit Lake. Quartz (SiO2) and albite (NaAlSi3O8) are also
here important minerals in the sediment.
The organic carbon contents in the water are in the normal range of natural lakes indicating that
some biological activities occur. Small variations between seasons indicate that the biological
activity is limited in the lake, which contains certain amount of nutrients but it is not rich in them.
The water always contains significant amount of dissolved oxygen even in the summer
stratification. This prohibits reduction reactions in the lake. The reduction of sulphate should not
happen and the metals seems mainly removed from the water through Fe oxidation and adsorption
on gibbsite, but not by sulphide mineral precipitation.
Table 1 Average elemental concentration in Udden Pit Lake and the standard deviation.
Ca mg/l
Mg mg/l
Na mg/l
K mg/l
S mg/l
Cl mg/l
Si mg/l
Fe mg/l
Mn mg/l
Zn mg/l
Al mg/l
Cu g/l
Pb g/l
Cd g/l
F mg/l

Number of
Samples
66
66
66
66
66
47
47
66
66
66
66
66
66
66
47

Average
Conc.
185.18
41.11
6.57
8.54
278.92
19.20
6.44
1.92
7.22
63.85
21.37
248.60
1.56
81.45
1.84

St.
26.30
4.78
0.58
1.18
27.10
4.21
0.87
2.02
0.79
10.31
7.19
72.12
0.58
18.92
0.75

16

7 REMEDIATION OF PIT LAKE


7.1 Liming treatment
Liming treatment shows that it is an effective method in treating acid pit lakes with respect to
increasing pH. However, the liming did not destroy the stratification of the Rvlidmyran Pit Lake,
since the density differences between upper and deeper water is still strong enough to maintain it.
Thus, water below 10 m remains anoxic (Figure 8).
pH
4

DO Saturation %
8

10

12

10

10

Depth (m)

Depth (m)

15

50

100

150

15

20

20

25

25

30

30

May2001
June2001
October2001
May2003
June2003

Figure 8 Results of in situ measurements of pH and dissolved oxygen saturation for the
Rvlidmyran Pit Lake before and after liming treatment.
One main effect by the liming is increase of Ca concentration due to dissolution of liming material.
However, the liming treatment did not influence the concentrations of elements such Na, K and S
in water since the species distribution of these elements are less controlled by pH (Figure 9). The
strongest effect from the liming with respect to removing metals from water is observed in the oxic
layer. Elements such as Fe, Mn, Zn, Mg are only strongly removed in the uppermost 10 m of the
water column, where oxygen appears (Figure 9). Oxic environment combined with high pH cause
precipitation of mineral such as goethite (FeOOH) and Fe(OH)3 are likely to occur, which removes
Fe from the oxic water (Borggaard and Elberling, 2003). Mn and Zn may be removed by
precipitation of minerals like manganite (MnOOH) and Zn(OH)2 respectively, as well as by
adsorption to Fe-oxyhyroxide particles and coprecipitation. In the anoxic water, redox sensitive
elements such as Fe and Mn still were much higher in deeper water. Precipitation and scavenging
becomes less effective, and Fe-oxhydroxides dissolve. Al and Cu are the metals most strongly
influenced by the liming. Through the whole water profile, dissolved Al and Cu decreased
dramatically, and they are almost completely removed from the water. Increased pH is the main
reason for removal of dissolved Al from the water, probably due to precipitation of gibbsite. Cu is

17

removed from the water not only by adsorption to gibbsite but also to Fe-oxyhydroxides and other
minerals since pH is rather high (Lee et al., 2002).
After liming treatment, about 5 metres thick dark green unconsolidated sludge precipitated at the
lake bottom. Mineral phases determined by XRD were calcite (CaCO3), chlorite
[Mg5Al2Si3O10(OH)8] and small amounts of amphibole. Fe(II)-Fe(III)-hydroxy salt, which is
probable the major composition gives green colour in the sediment sludge as found at the bottom
(Schwertmann and Cornell, 2000). Near to the bottom, modelling results indicates that sulphate
reduction in the sediment sludge may occur. This is may be true since the ratio of concentration
difference between bottom water and sediment water for Fe and S is similar as ratio for pyrite.

18

600

900
800

500

S mg/l

Ca mg/l

700
400

600
500

300
400
200

300
0,5m

5m

8m

10m

15m

20m

23m Bottom

400

5m

8m

10m

15m

0,5m

5m

8m

10m

15m

20m

23m Bottom

20

Mn mg/l

300

Fe mg/l

0,5m

25

200

100

15

10

0
0,5m

5m

8m

10m

15m

20m

23m Bottom

20m

23m Bottom

16000

Al g/l

12000

8000

4000

2003May
2003June
Average of pre-liming
95%confidence interval

0
0,5m

5m

8m

10m

15m

20m

23m Bottom

Figure 9 Concentration profiles of filtered Ca, S, Fe, Mn and Al in May and June 2003
compared with the average concentration before liming treatment, with 95% confidence
interval.

19

7.2 Sewage sludge treatment


Compared with liming, the sewage sludge treatment did not show strong effects on the
geochemical properties of the lake water. Pumping of sewage sludge into the lake and the
subsequent settling of sewage sludge had disturbed the upper water. However, the density
difference between upper and deeper water was still strong enough to resist thermal mixing of the
whole water column (Figure 10). Comparing with the liming period, pH was lower and distributed
rather uniformly. It has to be stressed that the neutral pH in the lake most likely still is a liming
effect. Eventhough the depth of oxygen depletion varied with time, anoxic layer at depth remains
after sewage sludge treatment. Strong decrease of redox is often observed at the depths where
oxygen decreases to zero. At the beginning of sewage sludge experiment, the redox potential
remained similar level as after the liming treatment. However, the redox level in deeper water
increased gradually with time (Figure 10).

Temp (C)
8
12

16

1.2
0

20

3.2

0
5

10

10

10

15

Depth (m)

15
20

20

25

25

25

30

pH
0

10

12

-400
0
5

10

10

15

Depth (m)

Dissolved Oxygen Saturation %


20
40
60
80
100

15

20

30

Depth (m)

Conductivity (ms/cm)
1.6
2
2.4
2.8

Depth (m)

Depth (m)

30
Redox (mV)
0
400

800

15

20

20

25

25

30

30

2001June12
2003June18
2003July05
2003December01
2004August26

Figure 10 Results of in situ measurements of temperature, conductivity, pH, redox, dissolved


oxygen saturation for the Rvlidmyran Pit Lake before treatments (2001 June 12), after liming
treatment (2003 June 18) and different stages after sewage sludge treatment (2003 July 05 to
2004 August 26).

20

Sediment analysis show that sewage sludge particles sank to the lake bottom rapidly, mostly
within the first month after treatment. Therefore, the organics in the sewage sludge may not have
been able to stay in the water long enough to sorb ions, thereby affecting dissolved concentrations
of metals. Sediment analysis also show the erosion occurred at bank sides is strong, which results
in mineral such as quartz (SiO2) and albite (NaAlSi3O8) being the major phase in the sediment, and
increased concentrations of Si, Al, Na and K in the lake sediment.
The sewage sludge treatment had the strongest influence on the particulate elemental
concentrations, especially at the beginning of treatment. Dissolved elemental concentrations are
not distinctly changed by the sewage sludge treatment (Figure 11). S and Fe were supposed to be
removed from the water by sulphate-reducing reactions, but such reactions did not occur during
the monitoring period. The sewage sludge increased the total organic carbon concentration in the
water column. However, nutrients such as phosphorous accumulated in the sediment already one
week after that the sewage pumping was completed.

Dissolved Mn
5

Particulate Mn
20

25

10

10

15

Depth (m)

Depth (m)

Mn mg/l
10
15

10

Mn g/l
20

30

40

15

20

20

25

25

30

30

2002March18
2003June18
2003July05
2003December01
2004August26

Figure 11 Concentration profiles of dissolved and particulate Mn concentrations in


Rvlidmyran Pit Lake before treatments (2002 March 18), after liming treatment (2003 June
18) and different stages after sewage sludge treatment (2003 July 05 to 2004 August 26).

8 CONCLUSIONS AND PERSPECTIVES


The results showed that these two pit lakes have some common characteristics; they have low pH,
they are oligotrophic and have high metal and sulphate contents. However, they have developed
distinctly different limnology and geochemistry. Rvlidmyran Pit Lake is oligotrophic and
meromictic. The lake is permanently stratified and three layers, the mixolimnion at the top, the
21

chemocline below and the monimolimnion further below, are identifiable. Groundwater filling and
stratification strongly control the elemental distributions in the lake. Most elements such as Ca, Mg,
Na, K, S, Mn, Fe and Zn have lowest and constant concentration in the mixolimnion.
Concentrations increase in the chemocline and keep rising in the monimolimnion. These elements
show quite similar behaviour in the water with strong correlations. Groundwater is supposed to be
the major source. Fe is removed from the mixolimnion due to oxidation and precipitation, but it is
redissolved in the monimolimnion.
Udden Pit Lake is a dimictic lake. Distinct overturning in spring and autumn occurs in the lake,
during which the whole lake circulates and most of the parameters and chemical components
become homogeneously distributed. The lake is thermally stratified in summer and winter. Three
layers, the epilimnion at the top, the metalimnion below and the hypolimnion at depth could be
identified. The thermal strata do not control the elemental distribution. During stratification, the
concentrations of dissolved elements appear to be constant at most depths. Variations mainly occur
in the top and bottom waters. Most elements such as Ca, Mg, Na, K, S, Mn, Cu, Al and Zn have
lowest concentration in the epilimnion. Concentrations increase in the metalimnion and kept
constant in the hypolimnion. Fe concentration distribution reflects the changes of redox potential.
High amounts of Fe2+ reaching the surface water by drainage waters from closely situated waste
rock dumps cause higher dissolved Fe concentration and lower redox potential in the top water.
Precipitation of dissolved Fe into suspended Fe occurs in deeper water where the redox potential is
higher.
Rvlidmyran was chosen for full-scale studies of remediation. Liming treatment proved to be an
effective method with respect to increased pH. The effects of the liming on the dissolved elemental
concentrations in the lake water were distinct, especially in the upper oxic water layer. Elements
such as Fe, Mn, Zn and Mg were largely removed in the upper oxic water, probably due to
formation of oxyhydroxides. Some elements such as Na, K and S were barely influenced. Al and
Cu were almost completely removed from the water throughout the profiles, due to pH increase
and precipitation of minerals such as gibbsite [Al(OH)3]. Sorption of Cu was probably removed
from the water by to gibbsite and Fe-oxyhydroxides, since pH was rather high. However, liming is
not a long-term solution as long as the acidic sources flow continuously into the lake. Therefore,
the liming effect will not last long and it will be rather costly to continue liming.
The sewage sludge treatment did not show distinct effects on the water quality during the
monitoring period. However, particulate elemental concentrations were influenced, especially
during the early stages of the treatment. Concentrations of total organic carbon increased in the
water column after sewage sludge treatment. However, most of the organics and nutrients settled
rapidly and accumulated at the lake bottom.
In this study, although lake water has not shown to be distinctly improved quality by sewage
sludge treatment in the field scale, which is mainly due to SRB probably has not been activated yet,
lessons have been learned and knowledge of about pit lakes accumulates. In future work, following
questions are suggested to be considered:
-

Hydrological balance situation of the studied pit lake is the necessary information
especially the quality and flow rate of inflowing groundwater. Since it may still bring the

22

oxidized sulphide minerals into the lake thus continuously acts as the acidic and
contaminant source. This will definitely retard the recovery of a pit lake.
-

Although pit lake has high relative depth, it does not necessarily mean the lake will be
stratified. Overturning may still occur in some cases. Therefore, it is always necessary to
performed limnologcial investigation to the lake, no matter before bio-remediation or
considering using a pit lake as a contaminant sank. Minimum one year round investigation
is suggested. To well understand if lake is stratified and the dynamic reasons of
stratification is very important, since a stable anoxic layer is demanded in this case.

Knowledge to well understand SRB and its interaction with acid mine water need to be
improved. Pilot study in a lab scale before field scale will be helpful. The lab experiment
should be able to answer the questions such as: How organic should be added into the lake?
It should sink from surface down to bottom or pipeline to bottom of the lake? How much
organic materials are needed in the different circumstance, considering the organic carbon
and nutrients composition in the organic material being used and the size of the lake? What
is the optimism situation to stimulate SRB activity and is it necessarily to perform pretreatment such as adjusting pH by adding basic material?

23

9 ACKNOWLEDGEMENTS
First of all, I would like to sincerely thank my supervisor Professor Bjrn hlander, who is
thanked not only for giving me the opportunity to be involved in this project, but more important,
for giving me great support, motivation and encouragement all the time in the past four years. This
thesis is the result of innumerable discussions. Without his knowledge, guidance, support, help and
patience, this thesis would have been impossible to finish.
I am also grateful to Lars-Olof Hglund at Kemakta Konsult AB, who is the program director of
MiMi, and to Roger Herbert at Uppsala University for your help and many valuable suggestions
and discussions.
My colleagues Anders Widerlund and Professor Johan Ingri are also especially thanked for always
being kind and available for discussions with me. Actually, I would like thank all my colleagues in
the Division of Applied Geology. Maj-Len Knutsson, thanks for your kindness, careness and
warmth. I really appreciated your patience of listening to my poor Svenska. Elena Shcherbakova,
Katja Viventsova and Larisa Pekka, we have become close friends rather than colleagues. Thank
you for your supports, the joyful time you spent with me and interesting discussions about almost
everything. Thanks to Milan Vnuk for helping me prepare nice-looking figures, tables and thesis
formats. More than that, Milan, I want to thank you for your patience to me, each time I knock on
the door to your office, which means Could you help me, Milan? Thanks to Johan GeltingNystrm, and Jerry Forsberg and ex-colleague Erick Carlsson for helping me with the fieldwork.
Towards the end of my study in Lule, I just realised that everybody in the division has helped me.
This help is too detailed for me to be able to list all my thanks here. I do appreciate it and it means
a lot to me. Because of you, it has become a wonderful experience to study at the Division of
Applied Geology, Lule University of Technology.
It is not often that I have the opportunity to thank my parents but I must admit they deserve it
every single day. So this is for you, for all you taught me, for teaching me becoming the one who I
am. My husband Han Qingshan has been always supportive. Many times I have been anxious and
worried, and he calmed me down so I was able to move on. His sacrificing and understanding have
been important motivations. I have made great friends including both Chinese and foreign friends
in Lule. I would like to thank you all for the nice time we had and for always cheering me up.
This study was financed and supported by the MISTRA research programme Mitigation of the
environmental impact from mining waste (MiMi) and Lule University of Technology. Liming
and sewage sludge treatment, as well as sampling in August 2004 were financed by Boliden AB.
We would like to thank Boliden AB for co-operation and for providing us with background
information. Special thanks to Michael Sandberg from Boliden AB for great help in field work of
sewage sludge pumping. Mark Wilcox is acknowledged for the language correction.

24

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