CONSTRUCTED WETLANDS AND THEIR

PERFORMANCE FOR TREATMENT OF WATER

CONTAMINATED WITH ARSENIC AND HEAVY
METALS

Ulrich Stottmeister1, Sasidhorn Buddhawong2, Peter Kuschk1, Arndt

Wiessner1 and Jrgen Mattusch1
1

UFZ Centre for Environmental Research Leipzig-Halle, Permoserstr. 15, 04318 Leipzig,
Germany, 2 King Monguts University of Technology Thonburi, 91 Pracha U- thit Rd., Tung
Kru, Bangkok 10140, Thailand

Abstract:

This study investigated the removal mechanisms of arsenic and heavy metals
in constructed wetland systems. The biotic and abiotic processes in the
wetlands and the influences of plants, soil and micro-organisms on arsenic and
heavy metal removal were examined. Various small-scale constructed
wetlands were set up in order to study and compare the removal efficiency of
laboratory-scale wetland models and small-scale field test systems. In the field
test systems, acid mine drainage (AMD) was used as an example of acidic
wastewater contaminated with heavy metals.

Key words:

heavy metals, arsenic, biotic abiotic processes, constructed wetlands,

rhizosphere

1.

INTRODUCTION

Acid mine drainage (AMD) poses worldwide environmental problems of

large dimensions wherever mining occurs. Moreover, arsenic wastes are also
released by many other industries, such as the chemical and electronic
417
I. Twardowska et al. (eds.),
Soil and Water Pollution Monitoring, Protection and Remediation, 323.
2006 Springer.

418

Ulrich Stottmeister et al.

industry, which use arsenic as a material in their processes; this implies

increasing environmental problems worldwide correlated to human health
( Le, 2001; Williams et al., 1996).
In general, contaminated mine water is generated when rock containing
sulphidic minerals is exposed to water and oxygen. This results in the
production of acidity and elevated concentrations of metals and sulphate in
the water (Braun et al., 2001). The generation of contaminated mine water is
a combined chemical and microbiological process (Stumm and Morgan,
1996). Factors influencing the acidity and metal content are the sulphide
grain size and surface area, porosity and permeability of the deposit, nature
of the gangue materials, nature of the sulphide ore, nature of acid-consuming
minerals, and various environmental factors influencing the activity of
micro-organisms (Ritcey, 1989). The generation of the water is highly sitespecific: it can vary greatly even within a single mine site and the chemical
composition may be very different including elements such as Al, As, Cd,
Cu, Fe, Pb, Mn, Ni and Zn with higher or lower concentrations of sulphate
and pH-values ranging from 2.6 to 7.5 (Ritcey, 1989; Wildeman and
Laudon, 1989; Dodds-Smith et al., 1995).
The primary aims of the treatment of contaminated mine water are to
neutralize acidity and to remove metals (Braun et al., 2001). In principle,
two broad categories of available types of treatment can be used: (1) active
systems, mainly for continuous operation and maintenance and (2) passive
systems, which are intended to be self-sustaining after an initial start-up
period (Braun et al., 2001). Active systems involve technologies such as pH
modification, ion exchange, biology-based treatments, adsorption,
electrochemical treatment and physical process technologies. Passive
treatment includes chemical passive treatment by the addition of chemicals
such as limestone, polymers or others (Braun et al., 2001; Brodie et al.,
1993; Ziemkiewicz et al., 1997) and biological passive treatment represented
by primary constructed wetlands and secondary algal systems or special
bioreactors (Braun et al., 2001; Foster, 1982; Phillips et al., 1994; Bender et
al., 1994; Davison, 1993; Duc et al., 1998). The passive treatment systems,
and in particular constructed wetlands, are advantageous mainly because
they cause comparably low costs, are truly self-sustaining and are suitable
for the treatment of mine water from abandoned mines (Braun et al., 2001).
The aqueous chemistry of arsenic is very complex because arsenic can
exist in solution in the -3, +3 and +5 oxidation states. The predominant
aquatic forms are the trivalent arsenite and the pentavalent arsenate.
Arsenates are less soluble and therefore less toxic. Arsenate is predominant
in oxic surface waters, whereas arsenite is present in anoxic waters such as
groundwaters. The oxidation from the arsenite to the arsenate state by

Constructed Wetlands and their Performance for Treatment

419

oxygen proceeds at room temperature only with the aid of catalysts. In an

extended literature review by Riveros and Dutrizac (2000), the chemistry of
arsenic is described in detail with the aim of deriving recommendations for
achieving long-term stability of arsenic wastes.
Nishimura et al. (1996) studied the oxidation of arsenite by oxygen in
presence of sulphite and Fe(II). The authors conclude that the oxidation
reactions of S(IV), As(III) and Fe(II) induce each other and result in a fast
As oxidation and precipitation by Fe(III). The structure of the Fe(III)-As(V)
precipitate according to the formation equation
Fe3+ + AsO4 3- + x H2O FeAsO4 . xH2O

(1)

is controversial. Robins et al. (1991) and Robins and Jayaweera (1992)

demonstrated that the precipitate is similar to a poorly crystalline ferric
oxyhydroxide phase (2-line or 6-line ferrihydrite) with adsorbed arsenate
ions. As(V) is adsorbed on ferrihydrite by complexation, resulting in a stable
inner-sphere complex. Such inner-sphere complexes are extremely stable
against desorption.
In waterlogged soils, bacterial activity may include in this reaction chain
sulphur(VI)-reduction and formation of iron(II) in anaerobic zones. In soil
with a high content of organic matter, the complex link between biotic and
abiotic reactions will be made nearly unforeseeable by the interaction of
humins as alternative electron acceptors. In the case of wetlands, the
presence of plants will further increase the complexity of this multicomponent system up to a level at which the system can only be regarded as
a black box. The scheme in Figure 1 is an attempt to summarise some of
the reactions, according to the scheme of Bhumbla and Keefer (1994).
Constructed wetlands have been used for mine water treatment for about
20 years. However, the potential longevity of constructed wetlands for mine
water treatment is currently not known and the design concepts and sizing
criteria are still under discussion (Braun et al., 2001).
The removal mechanisms in wetlands may include metal
incorporation/accumulation into below- and above-ground plant tissues,
adsorption on soil components, filtration/sedimentation of suspended
particles and microbial actions causing precipitation and co-precipitation
and/or volatilisation in the cases of certain metalloids etc. (Matagi et al.,
1998; Jackob and Otte, 2003; Dushenko et al., 1995).

Ulrich Stottmeister et al.

420

Arsenate

Methyl
arsonic acid

Arsenite
Reduction

HAsO42H2AsO4-

pH8-9
pH6-7

AsO2-

Bacteria

Oxidation

CH3
HO-As-OH

Dimethyl
arsinic acid
Bacteria

+S2 -

Cacodylic acid
Bacteria

+Fe
Adsorption
Precipitation

Fungi

AsS2-

Fungi

Reduction

FeAsO4

CH3
HO-As-CH3

Oxidation

CH3
H-As-CH3
As2S3

Dimethyl arsine

Oxidation

CH3
CH3-As-CH3

Trimethyl arsine

AsH3 ,
CH3AsH2

Figure 1. Chemical forms of As and their transformations (modified from Bhumbla and
Keefer, 1994).

Wetland plants are able to accumulate arsenic and heavy metals, whereby
the content in the roots is considerably higher in comparison to the aboveground plant matter (Stoltz and Greger, 2002). Nevertheless this metal
uptake and accumulation by plants plays only a minor role in wetlands for
water treatment (Mays and Edward, 2001). As and Zn can also be bound to
iron oxides as a consequence of oxidation and the formation of so-called iron
plaque on the roots of wetland plants (Doyle and Otte, 1997, Mendelssohn
et al., 1995). The presence of anoxic and oxic zones with gradients of redox
potential in the wetland system seems to be one of the main pre-conditions
for the functioning of all the above-mentioned biotic-abiotic reactions. This
redox potential will be influenced in general by the concentration of the
ionic redox elements, the pH-value and the oxygen concentration. Some
places of gradient formation are listed in Table 1.
The goal of the study was to characterize the fate of arsenic, zinc and iron
in various wetland systems with different conditions for water flow and
gradient formation. The removal of the toxic elements should be optimised
in laboratory systems and in small-scale field systems with acid drainage
waters.

Constructed Wetlands and their Performance for Treatment

421

Table 1. Main gradients in a subsurface-flow constructed wetland.

Gradients of
Sphere
Eh:
soil organic matter
pore water
rhizosphere
biofilms on the root surface
biofilms on the soil (gravel) particles
O2 :
shoots (aerenchyma)
roots (aerenchyma)
biofilms on the root surface
biofilms on the soil (gravel) surface
pH:
pore water
water
biofilms

2.

MATERIAL AND METHODS

2.1

Laboratory-Scale System of Wetlands and Ponds

A more detailed description of the experimental system can be found in

Buddhawong et al. (2005). The model wetlands were set up in plastic
containers (0.5 m long, 0.3 m wide and 0.3 m high) each with a total volume
of about 45 litres and a surface area of 0.15 m2.
In the Subsurface Water Wetland (SWW) system, plants of Juncus
effusus were planted in a gravel bed (grain size of 0.2 0.6 cm). The height
of the gravel bed was 25 cm, and the water level was kept 5 cm below the
gravel bed surface whereby the pore water volume was about 14 litres.
In the Free Surface Water Wetland (FSW) system Juncus effusus was
planted in the same container type and same gravel material as for the SWW.
However, the height of the gravel layer was only 15 cm and the water level
was kept 10 cm above the gravel layer, resulting in a total (free and pore)
water volume of about 25.5 litres.
The Algae Pond (AP) was in the same container type as for SWW and
FSW but without gravel. The water level was at about 22 cm height (33
litres). With time, algae growth started without additional inoculation.
A glass column of 0.3 m diameter with 0.07 m2 surface area was used as
a Hydroponic System (HP). The water level was at 0.6 m height; the water
volume was 41.5 litres. The floating Juncus effusus plants covered the whole
surface area.

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Ulrich Stottmeister et al.

The Juncus effusus plants used were propagated in hydroponic culture in

a greenhouse. The plants were transferred into the model systems three
month before starting the experiments.
The experimental systems were operated in a greenhouse; the
temperature was adjusted to 25 C. At the beginning of the experiments the
total plant biomass (roots and shoots; in kg wet weight) was 4.2 for SSW,
1.7 for FSW and 1.3 for HP. Within the experimental period of 90 days (16
July 15 October 2001) the biomass increased by 10.8%, 76.0% and 30.3%
respectively.
The model water was prepared by using tap water containing the
following main components (in mg/L): Ca 90.7, Mg 12.6, K 4.6, Na 23.0,
SO42- 157, Cl- 45.5) to which the chemicals were added according to Kuschk
(1991). Furthermore ZnSO4 and As2O5 were added, resulting in a final
concentration of 5 mg/L for Zn and 0.5 mg/L for As. Finally, the artificial
wastewater was adjusted to pH 4 by adding H2SO4.
Because of evapotranspiration, each container was topped-up with
distilled water twice a week in order to maintain the water level in all
containers at the start-up level.
Sulphate was measured by means of ion chromatograph using a Dionex
100 (AS4A-SC column/AG4A-SC column) with conductivity detection
(Rethmeier et al., 1997)
Water samples were taken from 3 different levels of the model systems:
near the bottom (about 3 to 5 cm above the bottom), in the middle (e.g. in the
middle between bottom and the surface of the respective gravel beds or in
the middle of the water column for HP) and near the surface (about 10 cm
below the surface of the gravel bed for SWW and about 5 cm below the
water surface of the other experimental systems).

2.2

Small-Scale Field Test Systems for AMD Treatment

A more detailed description of the experimental system can be found in

Buddhawong et al. (2005). The model experiments were conducted at the
UFZ experimental area in Grosskayna-Beuna, near Merseburg (Germany).
These field test systems consisted of 6 small containers, which were
continuously fed with acid mine drainage (AMD) from the Merseburg-Ost
gravel pit. This AMD had a concentration of 2-3 g/L sulphate and its pH was
about 3. The further main chemical elements of this AMD were (in mg/L):
Na ~450, Ca 390, Fe 150, Mg 120, Al 90, Mn 9, K 3, Zn 1.8, Ni 1.3, Br 0.9,
Li 0.7, Co 0.6 and Ce 0.5; further elements were also detectable at lower
concentrations.

Constructed Wetlands and their Performance for Treatment

423

The 6 different model constructed wetlands were each placed

in containers with a size of 0.47 0.60 0.91 m3 and a surface area of
0.55 m2. Further parameters are summarized in Table 2. Juncus effusus was
used in all the planted wetland systems. Container B1 and B2 represented the
hydroponic systems (HP). FSW and SSW (B3, B4, B5 and B6) contained a
mixture of sand materials, which included sand and fine gravel (0.6-2 mm
size). The water was kept flowing 10 cm below the sand surface of SSW,
and 10 cm over the sand surface of FSW. The inflow rate in different
systems differed from 0.1 -0.4 l/h, the hydraulic retention time 8 and 40
days. For details see Buddhawong (2004).

2.3

Analytical Methods

The redox potential was measured with a SenTix ORP electrode

connected to a Multiline P4 (WTW, Germany). To prevent air contact the
electrode was put into a small flow-through cuvette. The inlet of the cuvette
was connected with a long robust injection needle which was pushed into the
required depth of the model wetland/pond systems. The outlet of the cuvette
was connected with a syringe to suck water samples through the cuvette
containing the electrode. All data were recalculated to the standard hydrogen
electrode in accordance with the temperature.
As, Zn and Fe were analysed by ICP-AES (Spectro Cieros) (APHA,
AWWA, and WEF, 1995). The detection limits were 0.06 mg/L for As, 0.04
mg/L for Zn and 0.05 mg/L for Fe, whereby the analysis of triplicates was
found to be in all cases within a standard deviation of 5 %.

3.

RESULTS AND DISCUSSION

3.1

Removal Performance of Arsenic and Zinc in the

Laboratory-Scale Wetlands

3.1.1

Arsenic

The arsenic concentration gradients along the sampling levels (bottom,

middle, surface) of the 4 experimental systems are shown in Figure 2. In
SSW and FSW, in all cases the concentration decreased after 24 days to
below 0.1 mg/L. However, a no significant decrease of arsenic occurred in
AP and HP.

Ulrich Stottmeister et al.

424
400

250
200

SSW

150
y=39.97+2677.2x
R2=0.8014

100

Middle

Bottom

-1.615

(b)

FSW

200
y = 2025.3x-0.9929
R2 = 0.9646

100

50
0

20

40

60

80

20

40

Days

60

80

Days

600

600

HP

500
400
300
200
100

Bottom

Middle

AP

500

As (g/l)

As (g/l)

Surface

300

As (g/l)

As (g/l)

(a)

Surface

Middle

Bottom

400
300
200
100

Surface

Bottom

Middle

40

60

Surface

20

40

Days

60

80

100

20

Days

80

100

Figure 2. Arsenic concentration in the water of the laboratory model wetlands, dependent on
the time and sampling depth.

In unplanted gravel vessels, a very low adsorption capacity (about 4

g/kg gravel) was measured. Therefore we conclude that there was no
significant direct sorption to the matrix. With the same systems, the
adsorption or incorporation of arsenic into the plants was determined.
However, this amount of arsenic was also found to be negligible
(Buddhawong et al., 2005). As a consequence, the explanation for the
phenomenon of greatest arsenic removal in the planted gravel system could
only be that gravel in combination with plants provides especially favourable
conditions for arsenic binding.
It was of further interest to determine the concentration of iron, the
behaviour of pH and the redox value with respect to the factors influencing
the complex system.
The pH value decreased to about 4 in HP; however, in SSW and FSW the
pH remained relatively constant between 6 and 7 (data not shown). The
redox potential of the SSW and the FSW in dependence on the sampling
level is shown in Figure 3. The redox value was lowest at the bottom of both
systems. However, in the other systems (AP and HP) no differences in the
redox values were observed (data not shown).
It can be assumed that due to the activity of the roots, organic compounds
(rhizodeposition products as the sum of root exudates and dead root matter)
are released into the rhizosphere. Some of these compounds can function as
iron chelating compounds (Hoffland et al., 1992). Furthermore, these organic

Constructed Wetlands and their Performance for Treatment

425

600

SSW

mV

400

200

Bottom

Surface

Middle

20

40

600

60

80

days

FSW

mV

400

200

days

0
0

20

40

60

80

Figure 3. Redox potential in the water of the laboratory model wetlands, dependent on
the time and sampling depth.

compounds can also be used as a carbon source for micro-organisms in the

soil, resulting a decrease of the redox potential. Both the relatively low redox
(see Figure 3) and the chelating rhizodeposition products stimulate the
redissolution of crystalline iron(III), which has a low binding capacity for
As. Nevertheless, because of the capability of some helophytes to transfer
oxygen into their rhizosphere (Jackson and Armstrong, 1999; Colmer, 2003)
the oxic conditions in the rhizosphere and especially on the rhizoplane can
cause the precipitation of the dissolved iron and co-precipitation of other
trace elements such arsenic, especially on the roots forming iron plaques
(Wang and Peverly, 1996).

Ulrich Stottmeister et al.

426

The time course of the formation of dissolved iron and the subsequent
decrease of iron concentration in the pore water especially at the bottom of
SWW (see Figure 4) supports the assumption that, in general, a dissolution
of crystalline iron and subsequently precipitation by the direct and indirect
action of plants and micro-organisms in combination can cause the observed
As removal from the water phase in waterlogged soils having an apparently
low As binding capacity.

-1

Iron [mg l ]

(a)

6
4
2
0
0

20

40

60

80

100

Time [d]
3,5
-1

Iron [mg l ]

(b)

2,5
2
1,5
1
0,5
0
0

20

40

60

80

100

Time [d]
surface

middle

bottom

Figure 4. Iron concentration in the water of the laboratory model wetland (SWW),
dependent on the time and sampling depth (a: SSW, b: FSW).

3.1.2

Zinc

The aqueous chemistry of zinc is simpler than that of iron and arsenic.
Only the formation of insoluble sulphide or carbonate at neutral or higher pH
could be responsible for Zn elimination from solution. In our experiments,
the zinc concentration only decreased in SWW, FSW and HP. In AP, the Zn
concentration did not change significantly during the period of 90 days.
Almost complete elimination was observed for both the planted gravel bed
systems, whereby in SWW the rate was faster than in FSW (see Figure 5).

Constructed Wetlands and their Performance for Treatment

427

In HP, the Zn concentration decreased only slowly by about 27 % during

90 days (data not shown). Similar to the total As concentration, no
concentration gradient dependence on the sampling depth could be observed.
Because of the extremely fast decrease of Zn concentration in both gravel
bed systems (SWW and FSW) within few days, the increase of iron
concentration with time (see Figure 5) and the observation that the redox
potential did not decrease significantly below 100 mV (see Figure 3), the
action of sulphate-reducing bacteria and resulting sulphide precipitation can
be excluded.
0,8

Zinc [mg l -1]

(a)
0,6
0,4
0,2
0
0

20

40

60

80

100

-1

Zinc [mg l ]

Tim e [d]

3,5
3
2,5
2
1,5
1
0,5
0

(b)

20

40

60

80

100

Time [d]
surface

middle

bottom

Figure 5. Zinc concentration in the water of the laboratory model wetlands, dependence on
the time and sampling depth (a SWW, b FSW) (from Buddhawong et al., 2005).

Ulrich Stottmeister et al.

428

Whether Zn is sequestered as its carbonate within the gravel systems

because of higher pH values in comparison to HP and AP is still an open
question.

3.2

Treatment of Acid Mine Drainage (AMD)

in Small-Scale Constructed Wetlands in a Field
Experiment (Preliminary Results)

Operating in an open area, six field test systems were fed continuously with
an AMD of pH 3 in long-term experiments from spring to wintertime. The
results are summarized in Figure 6. As in the previous experiments
6

(a)

pH

(b)

pH

Inflow

Outflow planted

10-Dec-02

21-Oct-02

01-Sep-02

13-Jul-02

24-May-02

04-Apr-02

Outflow unplanted

Figure 6. Changes of pH over time of the AMD in the various small-scale constructed
wetlands in the field test.

Constructed Wetlands and their Performance for Treatment

429

under batch conditions, the SSW and FSW with gravel beds show a clear pH
increase at the outflow in comparison to the inflow AMD. However, when
passing through the HP the pH of the AMD remained almost unchanged.
The behaviour of iron and zinc in this continuous flow system is being
studied as part of our current work.

4.

CONCLUSIONS

The removal capacities for As and Zn are larger in soil- (gravel-) based
wetlands than in hydroponic systems or in algae ponds.
Probably due to diffusion limitations, depth-gradients were found in the
soil-based systems according to various parameters of the pore water such as
redox potential and concentrations of contaminants. These gradients appear
to be a prerequisite for the complex iron dissolution and re-precipitation
processes within the soil-based systems.
Although gravel and plants each separately have low binding capacities
for As, it was found that the combination of both within a single system
obviously effects a dissolution of soil crystalline iron to act as a coprecipitation agent for As, particularly in the oxic zones of the rhizoplane.
The small-scale experiments simulating the treatment of acid mine
drainage by various types of constructed wetlands operated on a field site
showed, in general, similar results. Wetland systems with a combination of
gravel/soil matrix and plants have a better treatment performance than
systems with only soil or only plants without soil.
In the field experiments, the seasonal change, rainfall and temperature
affected the removal efficiency of the constructed wetlands.
In general, these results encourage the implementation of constructed
wetlands for remediation of wastewater from mines and industries which
emit acidity, As, Zn and other heavy metals.

ACKNOWLEDGMENT
Sasidhorn Buddhawong gratefully acknowledges the German Academic
Exchange Service (DAAD) for funding her scholarship. Furthermore the
authors would like to thank Kerstin Puschendorf, Gisela Pltze, Ines Hilbert,
and Reinhard Schumann for technical assistance.

430

Ulrich Stottmeister et al.

We are very grateful to the colleagues from the district office of

Merseburg-Querfurt, especially to Hartmut Handschak for supporting the
field experiments and for the technical assistance of Gerd Beckelmann and
Klaus-Dieter Schwind.

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