Science of the Total Environment 755 (2021) 143725

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Science of the Total Environment

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Long-term redox conditions in a landfill-leachate-contaminated groundwater

Daniel Abiriga ⁎, Live S. Vestgarden, Harald Klempe
Department of Natural Sciences and Environmental Health, Faculty of Technology, Natural Sciences and Maritime Sciences, University of South-Eastern Norway, Bø, Norway

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• Municipal landfill leachate contamina-

tion of a confined aquifer in Southeast
Norway
• Contaminants impaired water quality,
hindering exploitation of the ground-
water.
• Redox conditions that developed are
similar to those reported from phreatic
aquifers.
• Apparent breakdown in long-term
redox conditions as landfill attained
phase IV.
• Redox conditions control spread of pol-
lutant and minimise degradation of
ecosystems.

a r t i c l e i n f o a b s t r a c t

Article history: Indicators of redox conditions; oxygen, sulphate, nitrate, ammonium, iron and manganese, and in addition, bicar-
Received 5 June 2020 bonate and total organic carbon were studied in groundwater samples contaminated by leachate emanating from
Received in revised form 28 October 2020 Revdalen Landfill (Norway). Based on these variables, the study aimed to deduce the redox conditions in the
Accepted 11 November 2020
aquifer. Literature on landfill leachate contamination of confined aquifers is scarce and to the best of our knowl-
Available online 14 November 2020
edge, this study, which describes long-term analysis of redox chemistry, is the first of its kind in such an environ-
Editor: Jurgen Mahlknecht ment. Groundwater samples were monitored for a period of 24 years, enabling us to describe redox conditions on
both short-term and long-term bases. Levels of measured parameters in the contaminated aquifer varied spatially
Keywords: and with time, but were generally elevated except oxygen; pH (4.9–8.8), oxygen (0–11.3 mg/L), sulphate
Confined aquifer (0–28 mg/L), nitrate (0–16 mg N/L), ammonium (0.02–40 mg/L), iron (0–99 mg/L), manganese
Leachate plumes (0.06–16 mg/L), bicarbonate (22–616 mg/L) and total organic carbon (1.3–47 mg/L). From the result, levels of
Pollution iron, manganese, nitrate and ammonium violated the Norwegian drinking water norms. However, iron, ammo-
Attenuation nium, total organic carbon and bicarbonate showed strong attenuation along the groundwater flow path. By con-
Redox condition
trast, oxygen, nitrate and sulphate increased farther out in the plume. The redox conditions that developed in the
Oxidation
aquifer were similar to those previously reported for phreatic aquifers, structuring by proximity to the landfill as
sulphate-reducing, iron-reducing, manganese-reducing, nitrate-reducing, and finally aerobic condition. Eventu-
ally, there was an apparent breakdown of this system due to ecosystem shift in the landfill when leachable re-
duced ions were depleted and the landfill became aerobic. Overall, the redox framework provided remarkable
attenuation to contaminants, and thus prevented potential degradation of ecological health due to the landfill
leachate.
© 2020 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY license (http://
creativecommons.org/licenses/by/4.0/).

⁎ Corresponding author at: Department of Natural Sciences and Environmental Health, University of South-Eastern Norway, Gullbringvegen 36, NO-3800 Bø, Norway.
E-mail addresses: daniel.abiriga@usn.no (D. Abiriga), live.s.vestgarden@usn.no (L.S. Vestgarden), harald.klempe@usn.no (H. Klempe).

https://doi.org/10.1016/j.scitotenv.2020.143725
0048-9697/© 2020 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
D. Abiriga, L.S. Vestgarden and H. Klempe
1. Introduction
Groundwater has been source of drinking water for centuries to
more than half of the world's population (Zaporozec and Miller,
2000). In the Nordic countries, it still supplies about half of the popula-
tion (Kløve et al., 2017). Despite its importance, groundwater faces seri-
ous pollution challenges globally (Chapman, 1996; Pous et al., 2018;
Zaporozec and Miller, 2000). In Norway, contaminations are both an-
thropogenically due to agricultural activities (Haarstad and Ludvigsen,
2007; Kværner et al., 2014), landfills (Basberg et al., 1998; Haarstad
and Mæhlum, 2008), forestry, quarry, industries (Kløve et al., 2017),
and naturally due to the geology (Banks et al., 1998a; Banks et al.,
1998b; Frengstad et al., 2010). In Norway, before the late nineties
solid waste management was primarily through landfilling as was else-
where worldwide, although this has undergone remarkable advance-
ment now. However, the old landfills are still a threat to the
environment, as they are characterised by lack of liners or leachate col-
lection system (Mouser et al., 2005). The leachate can migrate vertically
and horizontally through advection, dispersion and dilution (Xie et al.,
2009; Xie et al., 2016; Zhan et al., 2014), thereby contaminating soil
and groundwater (Indelicato et al., 2017; Rana et al., 2018). The severity
of pollution depends on the underlying geological strata (Lee et al.,
2019; Negi et al., 2020), although generally, the horizontal extend of
pollution decrease along groundwater flow path (Abiriga et al., 2020;
Christensen et al., 2001; Han et al., 2016; Sharma et al., 2020;
Vodyanitskii, 2016).
Landfills present serious pollution problems as they leach a complex
mixture of pollutants, particularly so from old municipal landfills that
were operated before waste segregation was adopted. This poses a seri-
ous challenge to remediation of contaminants in the leachate (Ye et al.,
2019), which may compose of both legacy and emerging pollutants
(Eggen et al., 2010). Nonetheless, new innovative remediation technol-
ogies are being developed, but are still at infancy as most of these are
still lab-based (Ye et al., 2019). Presently, remediation is largely through
monitored natural attenuation. Redox zones are believed to constitute
important chemical frameworks for natural attenuation of contami-
nants in groundwater leachate plumes (Appelo and Postma, 2005;
Bjerg et al., 1995; Jurgens et al., 2009; Saito et al., 2020) and are respon-
sible for minimising the extend of spreading of contaminants from land-
fills (Han et al., 2016). This explains why many of the groundwater
remediation technologies closely mimic redox processes (Tandon and
Singh, 2016). Knowledge on prevailing redox conditions is therefore
fundamental in understanding and evaluating the effectiveness of natu-
ral attenuation processes (Christensen et al., 2000).
Redox zones are principally governed by chemical reactions where
participating elements change their valence states through gain or loss
of electrons (Fetter, 1993). The preference for redox species in oxidation
reactions is, in the decreasing order, dissolved oxygen > nitrate > man-
ganese > iron > sulphate (Bjerg et al., 2003; McMahon and Chapelle,
2008; McMahon et al., 2011; Chung et al., 2019; Stumm and Morgan,
1996), a series referred to as the ecological succession of terminal
electron-accepting processes (McMahon and Chapelle, 2008). Redox se-
quences are observed where leachate from an organic-rich landfill en-
ters into an oxic aquifer (Christensen et al., 2000). Chemical analyses
of methane, sulphate, iron, manganese, ammonium, nitrate and dis-
solved oxygen in groundwater samples are used to deduce redox status
of aquifers (Bjerg et al., 1995; Lyngkilde and Christensen, 1992). For
landfill leachate, the typical redox structure of plumes follows the se-
quence, from the outer edge: aerobic, denitrifying, manganese-
reducing, iron-reducing, sulphate-reducing, and methanogenic condi-
tion developing at the foot of the landfill (Bjerg et al., 2011; Lian et al.,
2017; Vodyanitskii, 2016). The reduced chemical species that is leached
from the decomposing waste or mobilised from the underlying strata
will become oxidised farther downgradient by either chemical reactions
or microorganisms as the plume migrate along the aquifer. Such cyclic
chemical and biological conversions provide pools of electron acceptors
2
Science of the Total Environment 755 (2021) 143725
in the aquifer, which can result in additional attenuation of pollutants in
the leachate plume (Bjerg et al., 1995; Heron and Christensen, 1995).
Diverse microbial communities including methanogens, sulphate-
reducers, iron-reducers, manganese-reducers and denitrifiers have
been identified in landfill leachate plumes (Christensen et al., 2001;
Ludvigsen et al., 1998) and are believed to be responsible for redox pro-
cesses. They facilitate evolution of redox conditions through inter-
compound electron transfer from donors to acceptors (Jurgens et al.,
2009; Rivett et al., 2008) and their abundances correlate with the pre-
dominant redox state (Ma et al., 2019). These microorganisms fre-
quently occur as biofilms on the surfaces of aquifer materials (Fetter,
1993). Variations in site geology and geochemistry may affect the mi-
crobial redox processes in the plume due to variability in levels of sub-
strates, nutrients or electron acceptors (Ludvigsen et al., 1998). In
addition, climate and hydrology may influence redox processes through
their effect on groundwater residence time (McMahon and Chapelle,
2008). This can cause an unexpected spreading patterns despite homo-
geneous aquifer conditions (Bjerg et al., 2003), which can lead to distor-
tions of redox zones. Whether or not such distortions permanently alter
the pattern of redox zones can only be resolved with long-term data.
Majority of the data reported in the literature is dominated by short-
term observations such as risk/impact assessments while reports on
long-term studies are scarce.
The main objective of the present study was to delineate the redox
conditions of Revdalen Aquifer based on groundwater chemistry data
for a period of 24 years. Although groundwater contaminations from
landfills are common worldwide, literature on confined aquifers is
scarce, the less so from cold climates such as Norway. This reflects the
high risks associated with the pollution of unconfined aquifers, and
the high cost associated with investigating confined aquifers. Due to
lack of literature on confined aquifers as highlighted above, we chose
to compare our results with those reported for shallow phreatic aqui-
fers. In pristine aquifers, there is a remarkable difference in redox gradi-
ents between unconfined and confined aquifers, but the difference
become less pronounced when aquifers are anthropogenically influ-
enced (McMahon et al., 2011). Theoretical considerations (Bjerg et al.,
2011; Chapelle, 2001; McMahon et al., 2011) indicate that the structure
of redox zones should be comparable, although the longitudinal gradi-
ent may still be greater in confined aquifers (McMahon et al., 2011).
Parallel to the main objective was to evaluate the variations in the
redox conditions over time. Our study is based on traditional data and
enabled follow-up of the redox conditions in the aquifer on a long-
term basis, which has not been reported previously. In addition to pro-
viding literature on confined aquifers, it also provides valuable informa-
tion on site remediation; in as far as, redox framework for attenuation of
pollutants is concerned.
2. Materials and methods
2.1. Study area
The study site is an underlain of quaternary glaciofluvial delta de-
posit at an altitude of 150 m above sea level located north of Bø town
(Bø municipality) in south-eastern Norway. Two aquifer units are pres-
ent (Klempe, 2015). The upper unconfined aquifer has an unsaturated
zone of ~11 m and a saturated zone of ~3 m and comprises of unconsol-
idated sand and gravel as its aquifer matrix running longitudinally over
a moraine complex. The bottom of this aquifer is a layer of glacial till
which also is the confining unit for the lower aquifer (Klempe, 2015).
Groundwater recharge of the upper aquifer occurs by infiltration of pre-
cipitations through the unsaturated zone. The lower confined aquifer
has a dimension of 1700 × 70–100 × 5–8 m (long, wide, thick) with
the matrix comprising of unconsolidated sand and gravel. The sides of
the aquifer are limited by bedrock walls of Precambrian crystalline
rock. This aquifer is recharged by a small watershed occurring at its out-
crop upgradient (Klempe, 2015).
D. Abiriga, L.S. Vestgarden and H. Klempe
Landfilling in Revdalen started in 1958 as simply to fill up a kettle
hole in the area. This kettle hole was filled up with municipal solid
wastes from Bø and Sauherad municipalities between 1958 and 1974.
It was to be found in the geological unit of the upper unconfined aquifer,
which is not considered here, rather, the paper deals with the processes
in the lower confined aquifer. The isolation of the site prompted the mu-
nicipality to expand it as a full municipal landfill site, which over the
years 1974–1996 covered an area of 30,137 m2 (Abiriga et al., 2020).
Landfilling at the site ended in 1996 and the landfill was closed in
1997. During landfill cell opening, part of the confining layer of the
lower aquifer was excavated (Klempe, personal communication),
which has exposed the aquifer to leachate from the landfill. The risk of
contamination was exacerbated by the proximity of the landfill to the
watershed area, implying that recharge events were associated with
leaching of pollutants into the aquifer, generating plumes of contami-
nants. This impaired the water quality and the exploitation of the
groundwater for domestic use, which was serving several houses and
farms, has since been discontinued. The decision to halt the extraction
of the groundwater was to safeguard health of the surrounding commu-
nities. Although the groundwater quality has since improved greatly
over the years, the presence of legacy pollutants and heavy metals re-
ported previously (Abiriga et al., 2020) remains a concern. It is widely
acknowledged in the scientific community that landfills provide sink
to many kinds of pollutants, which can lead to sustained discharge of
such pollutants for decades to centuries. Thus, even after many years
of leaching, the landfill still presents a threat to the environment and
needs to be monitored.
2.2. Monitoring wells and groundwater sampling
The groundwater monitoring network consists of three wells R1, R2
and R4, located along the groundwater flow direction placed at the
Fig. 1. Location of the study area on map of Norway (left) and the location of the landfill cells, watershed recharging the aquifer, sampling wells R1, R2 and R4 placed along the groundwater
flow direction and site hydrogeology (right).
3
Science of the Total Environment 755 (2021) 143725
proximal, intermediate and distal positions, respectively (Fig. 1). R1,
R2 and R4 are located 26, 88 and 324 m downstream from the edge of
the landfill. R1 and R2 have been equipped with five and four multilevel
sampler respectively, using Waterloo Groundwater Monitoring System.
The elevations for the levels in R1 are 126, 125, 124, 123 and 122 m
above sea level, while those in R2 are 122, 121, 119 and 118 m above
sea level. R4 comprises of a cluster of three wells placed 0.25 m apart
drilled at depths 118, 117 and 114 m above sea level. In addition, a back-
ground well (R0, not shown) located 190 m upstream of the landfill in a
nearby aquifer was used for background water quality. Due to the loca-
tion of the landfill at the aquifer outcrop area, the resultant leachate
generated from the landfill thus discharges right at the source and
therefore, there was no provision to establish a reference well within
the confined aquifer.
Field sampling procedures have been described previously (Abiriga
et al., 2020). In 1992–2006, groundwater samples were collected from
all the levels when possible, after which the breadth of sampling was
simplified to only two levels from each well due to the associated cost
of performing chemical analysis. Also, in 1992–2002, samples were col-
lected quarterly but in 2003–2015, the frequency was reduced to bian-
nually. Groundwater sampling was performed as per International
Organisation for Standardisation (ISO) guideline 5667-11.
2.3. Chemical analysis and data handling
Chemical analysis was conducted by a commercial accredited labo-
ratory – ALcontrol Laboratories. All analyses were performed in accor-
dance with ISO and Norwegian Standards (NS): pH (NS 4720), oxygen
(NS 5813), sulphate (ISO 10304), nitrate (NS 4745), ammonium (NS
4746), bicarbonate (NS-EN ISO 9963-2), total organic carbon (TOC)
(NS 1484) and manganese (NS 4773). Iron was determined using in-
ductively coupled plasma atomic emission spectrometer (ICP-AES),
D. Abiriga, L.S. Vestgarden and H. Klempe Science of the Total Environment 755 (2021) 143725

Table 1
Summary of groundwater redox chemistry for the background well (R0), proximal well (R1), intermediate well (R2) and distal well (R4). Wells R1, R2 and R4 have been placed along the
groundwater flow direction in an increasing distance from the landfill. All units are in mg/L, except pH (pH units).

R0a R1 R2 R4

Mean n Min Max n Min Max n Min Max

pH 5.0 184 5.8 8.2 178 5.4 8.8 128 4.9 7.7
Oxygen 2.3 89 0.00 3.9 78 0.00 3.6 103 0.01 11.3
Sulphate 4.7 178 0.00 24 173 0.70 28 128 3.5 17.0
Nitrate (as N) 0.05 140 0.00 16.0d 151 0.01 11.7d 137 0.01 6.3
Nitriteb 0.00 4 0.01 0.02 4 0.00 0.01 1 0.00 0.00
Ammonium 0.02 185 0.02 40d 185 0.04 18.9d 142 0.30 14.4d
Iron 0.11 197 0.02 96d 195 0.00 99d 137 0.00 4.0d
Manganesec 0.02 134 2.0d 16.0d 133 0.28d 10.2d 88 0.06d 12.0d
Bicarbonatec 2.6 134 85 616 132 22 344 87 27 275
TOC 7.8 199 2.5 47 197 1.3 22 135 1.3 14.6

n is the number of observations for each parameter in R1, R2 and R4.

a
Groundwater monitored from 1992 to 2002.
b
Measured only once, in 1992.
c
Parameters monitored from 1992 to 2003.
d
Levels of parameters that have violated the Norwegian drinking water norms of 50 mg/L (nitrate), 0.5 mg/L (ammonium), 0.2 mg/L (iron), and 0.05 mg/L manganese.

according to the manufacturer's instruction. The groundwater chemis-
try dataset was analysed using Minitab 17 and R version 3.6.0 (R Core
Team, 2019). Minitab was used to construct two-dimensional cross-
sections, and R was used for correlation analysis to examine associations
between pairs of groundwater chemistry parameters, which was per-
formed on log10-transformed groundwater chemistry data.
3. Results
3.1. Water quality
Characteristics of the groundwater chemistry are summarised in
Table 1. The background aquifer had weakly acidic pH and slightly
high levels of both sulphate and TOC, while the other ions occurred at
very low levels. The contaminated aquifer on the other hand, was
characterised by elevated levels of reduced chemical species from the
landfill, namely ammonium, iron and manganese. There was also high
input of bicarbonate and TOC from the landfill. The discharge of highly
alkaline leachate from the landfill resulted in increase in the pH of the
groundwater to as high as 8.8 compared to the background value of
5.2. In general, all the measured parameters have deviated greatly
from the background quality and iron, manganese, nitrate, and ammo-
nium were in excess of Norwegian drinking water standards.
3.2. Oxidised redox species
varied below 5 mg/L until 2007 and in 2008–2015, values in R1 were
higher than in R2. The steep decrease in sulphate imediately after land-
fill closure was not observed at R4, but instead measurements indicate
gradual decline between 2001 and 2003. From 2008, there was a grad-
ual increase in levels of suphate detected across the sampling wells.
Nitrate showed less complex yearly distribution pattern along the
groundwater flow path, with values generally following the trend
R1 < R4 < R2 (Fig. 3C). Between 1992 and 2004, nitrate in R1 has
been close to zero. Unusual observations were recorded in 2005 and
2006, when values in R1 suddenly exceeded those in R2. Other recur-
rences were from 2010 where values in R1 continued to fluctuate
above those in R2. Nitrate concentrations in R4 fluctuated at ≤2 mg/L
throughout the study period.
3.3. Reduced redox species
3.3.1. A single observation
Two-dimensional profiles of a single-event observation in 1999
showed that concentrations of ammonium and iron (Fig. 4A–B), bicar-
bonate (Supplementary Fig. 1) and TOC (not shown) decreased sub-
stantially with distance. Plumes of ammonium, iron, bicarbonate and
TOC intruded into the aquifer from the deepest level at R1. Manganese
on the other hand, showed a distribution pattern resembling those of
oxygen and sulphate i.e., increased along the groundwater flow path
(Fig. 4C).

3.2.1. A single observation 3.3.2. Long-term observations

Two-dimensional profiles of electron acceptors; oxygen, sulphate
and nitrate for the month of June 1999 were mapped. The figure depicts
an increase in concentrations of oxygen, nitrate and sulphate with dis-
tances from the landfill (Fig. 2A–C).
3.2.2. Long-term observations
Despite the data gap for oxygen, one observation was apparent; con-
centrations increased downgradient but the yearly values indicate inco-
herent increase along the groundwater flow path (Fig. 3A). The result
also indicates that oxygen in the proximal well remained below
1 mg/L until 2013. Overall, values of oxygen fluctuated below that of
the background value, except in 1995, 1996 and 1997.
Sulphate has shown similar incoherent long-term changes in con-
centrations along the groundwater flow path as oxygen, although it
generally showed an increase with distance, i.e. R1 < R2 < R4
(Fig. 3B). There was a sharp decline after landfill closure as shown by
sulphate in R1 and R2. Since then, values in R2 fluctuated somewhat
close to the background mark until 2008 and from 2009, the values in-
creased to close to 10 mg/L. On the other hand, all values but one in R1
On a long-term observation (Fig. 5A), concentrations of ammonium
in R1 fluctuated above those in R2 and R4 until 2010, when values in R1
dropped below those in R4 but comparable to R2. Between 1992 and
2001, measurements in R2 were higher than in R4 but since 2002,
values in R4 became higher and fluctuated above those in R2. However,
these observations were all except three, below 5 mg/L.
Iron showed a remarkable decline along the groundwater flow path
(Fig. 5B). The pattern that prevailed between 1992 and 2008 was
R1 > R2 > R4. From 2009 to 2012, however, levels of iron in R2 became
higher than those in R1, but levels across the wells declined to close the
background value by 2013. Throughout the study period, levels of iron
in R4 remained close to that of the background value.
Higher manganese was recorded in R1 than in R2 and R4 between
1993 and 2000. Although there was no systematic change in concentra-
tions, most of the observations indicate an increase between R2 and R4
(Fig. 5C). Unfortunately, measurement of manganese in the groundwa-
ter samples was discontinued after 2003.
Correlations analysis between selected parameters (Fig. 6) revealed
significant associations between pairs of variables. From the analysis,

4
D. Abiriga, L.S. Vestgarden and H. Klempe Science of the Total Environment 755 (2021) 143725

Fig. 2. Two-dimensional profiles of oxygen (A), sulphate (B) and nitrate (C) from the multilevel sampling wells R1, R2 and R4 in June 1999. The vertical black dots denote the positions of
the multilevel in R1, R2 and R4. The wells are located in the contaminated aquifer and placed along the groundwater flow direction in an increasing distance from the landfill.

pairs of variable were in all cases but two, moderately to strongly corre-
lated. Strongest correlation was found for iron and ammonium, while
nitrate and oxygen had the weakest association, albeit significant.
4. Discussion
4.1. Oxidised chemical species
Concentrations of oxygen increased with distance downgradient of
the landfill, similar to previous findings for unconfined aquifers (Bjerg
et al., 1995). Suboxic and anoxic conditions were observed in R1, indi-
cating that R1 was located in the anoxic part of the plume with anaero-
bic degradation processes dominating. The availability of electron
donors for depleting oxygen in the aquifer is evidenced by the high
TOC measured in R1 (Supplementary Fig. 2). Higher levels of oxygen
in R2 and R4 indicate that these wells were located in the oxic part of
the aquifer, where aerobic oxidation predominates, which is consistent
with the high levels of sulphate and nitrate detected in these parts of the
aquifer (Fig. 2A–C). The long-term observations of dissolved oxygen
(Fig. 3A) conformed to the single-event observation in 1999 of increase

5
D. Abiriga, L.S. Vestgarden and H. Klempe
Fig. 3. Long-term variations in concentrations of oxygen (A), sulphate (B) and nitrate (C)
in the contaminated groundwater samples collected from R1, R2 and R4. R0 is the
background well, but was only monitored in 1992–2002. The data are annual mean
values. The vertical dashed line denotes the year (1997) of landfill closure. Note the data
gap for oxygen for periods 1993–1997 and 2004–2007. This was due to changes in
personnel, a typical problem experienced in such long-term monitoring programmes.
with distance until 2013, when measurements from R1 became higher
than in R2, indicating breakdown of the reducing condition at R1. This
is likely a manifestation of phase IV of landfill stabilisation, which onsets
with exceedance of microbial oxygen depletion by intrusion of molecu-
lar oxygen into the system, thus becoming aerobic ecosystem (Kjeldsen
et al., 2002; Mårtensson et al., 1999; Reinhart and Grosh, 1998). How-
ever, more years of monitoring are required to confirm if for sure the
landfill has attained this stage.
As with oxygen, concentrations of sulphate increased with distance,
a similar pattern was observed in Grindsted Landfill, and was attributed
to oxidation of sulphide (Bjerg et al., 1995). Suffice it to say the observed
increase in sulphate in Revdalen was due to oxidation, because the in-
crease in sulphate coincided with increase in oxygen. The very low sul-
phate observed at R1 between 1998 and 2007 (all except one, values
were below 5 mg/L) can be attributed to reduction processes following
closure of the landfill (Fig. 3B). This was probably due to the action of
6
Science of the Total Environment 755 (2021) 143725
sulphate-reducing bacteria. For example, the obligate anaerobe
Desulfovibrio species which use sulphate as a terminal electron acceptor
during oxidation of organic carbon (Rail, 1989). This process seemed
likely due to the high organic matter content detected in R1 environ-
ment (Supplementary Fig. 2). Some of the sulphide species generated
during such anaerobic reaction in R1 migrated downgradient and such
species will be oxidised to sulphate in the presence of oxygen
(Chapelle, 2001). More evidence in support of oxidation is the positive
correlation between sulphate and oxygen (Fig. 6A). However, sulphur
cycling appears to truncate in R2, leading to accumulation of sulphate
downgradient with additional input from further oxidation in R4 area.
In 2008, there appears what would be attainment of phase IV of landfill
stabilisation during which additional refuse oxidation is expected to
occur, leading to formation of oxidised species such as sulphate
(Mårtensson et al., 1999). This ecosystem shift towards aerobic condi-
tion is consistent with the data on oxygen, but more years of monitoring
are required to confirm this transition in the landfill ecosystem. At this
point, the TOC in the groundwater samples was less than 10 mg/L and
the organic carbon species of the TOC is likely to compose of recalcitrant
carbon molecules (Kulikowska and Klimiuk, 2008).
The spatial nitrate distribution followed the pattern of R1 < R4 < R2.
Such spatial increase downstream of landfills has been observed else-
where (Basberg et al., 1998; Bjerg et al., 1995; Chapelle, 2001; Han
et al., 2014). The near-zero nitrate quantified in R1 between 1992 and
2004 was probably due to reduction of nitrate by organic matter and
iron (II) present in the leachate. Evidence in support of in situ nitrate re-
duction is the presence of nitrite detected in R1 and R2 in 1992
(Table 1). On the other hand, the increase in levels of nitrate between
R1 and R2 was probably due to oxidation of ammonium, as supported
by significant but a weak positive correlation between nitrate and oxy-
gen (Fig. 6F), and a moderate negative correlation between ammonium
and nitrate (Fig. 6B). Because nitrate neither forms salt precipitates nor
adsorbs significantly (Appelo and Postma, 2005), it tends to accumulate
in settings where organic carbon is limiting (Bjerg et al., 1995). The fact
that TOC was detectable in R2 (Supplementary Fig. 2) is an indication
that either the amount was below that needed to strip nitrate from
the groundwater, or the TOC mainly composed of recalcitrant com-
pounds. The observed decrease in nitrate between R2 and R4 could be
due to denitrification and dilution processes. Unfortunately, nitrite anal-
ysis was discontinued after initial measurements in 1992 showed very
low levels (Table 1), thus the proposed denitrification at R4 could not
be substantiated empirically. In addition, denitrification does not consti-
tute a major process in the presence of >1 mg/L dissolved oxygen
(Pastén-Zapata et al., 2014). Dissimilatory Nitrate Reduction to Ammo-
nium (DNRA) is another pathway through which nitrate may be atten-
uated (van Niftrik and Jetten, 2012), but the pathway presents only a
temporary attenuation mechanism, because the resultant ammonium
may undergo oxidation back to nitrate (Rivett et al., 2008). Also, the
ideal condition for DNRA is anaerobic, which we did not observe in R4,
although pockets of anaerobic microenvironment might occasionally
develop and quite recently, nitrate reduction have been observed even
in the presence of ~2.5 mg/L dissolved oxygen (Herzyk et al., 2017).
The observation that ammonium in R4 fluctuated above that in R2 sug-
gests DNRA was an active process for attenuating nitrate, although the
ammonium might have originated from other alternative sources (see
text on ammonium). The unusual observations in R1 in 2005–2006
were probably due to leaching of high nitrate waste from the landfill,
while the increase from 2010 is similar to patterns observed for oxygen
and sulphate, explainable by attainment of phase IV of landfill
stabilisation as discussed above.
4.2. Reduced chemical species
The natural attenuation of ammonium in Revdalen Aquifer has been
very substantial. Similar pattern of strong attenuations have been re-
ported in the literature, and are believed to be due to cation exchange,
D. Abiriga, L.S. Vestgarden and H. Klempe Science of the Total Environment 755 (2021) 143725

Fig. 4. Two-dimensional profiles of ammonium (A), iron (B) and manganese (C) from the multilevel sampling wells R1, R2 and R4 in June 1999. The vertical black dots denote the positions
of the multilevel in R1, R2 and R4. The wells are located in the contaminated aquifer and placed along the groundwater flow direction in an increasing distance from the landfill.

biodegradation and oxidation (Bjerg et al., 2003; Cozzarelli et al., 2011).
Ammonium has high affinity for cation exchange sites in clay minerals
in sediments and is thus the most attenuated cations in leachate plumes
(Christensen et al., 2001). In spite of Revdalen Aquifer matrix being pre-
dominantly sand and gravel, there are possibilities of clay occurring. De-
posits composed of clean sand or gravel can still bare significant
contents of colloids (Freeze and Cherry, 1979). However, it is possible
that oxidation of ammonium was the predominant attenuation process
in Revdalen Aquifer, since there was an unequivocal increase in oxygen
and nitrate coinciding with remarkable decrease in levels of ammo-
nium. This is further substantiated by the negative correlations between
ammonium and nitrate (Fig. 6B) and oxygen (Fig. 6C). An alternative
ammonium attenuation is through anammox reaction (Cozzarelli
et al., 2011), a mechanism which is considered a major pathway for

7
D. Abiriga, L.S. Vestgarden and H. Klempe
Fig. 5. Long-term variations in concentrations of ammonium (A), iron (B) and manganese
(C) in the contaminated groundwater samples collected from R1, R2 and R4. R0 is the
background well, but was only monitored in 1992–2002. The data are annual mean
values. The vertical dashed line denotes the year (1997) of landfill closure. Note that
manganese was only monitored for the period 1992–2003.
loss of fixed nitrogen (Kartal et al., 2013; van Niftrik and Jetten, 2012).
This was possible at R1 area before the plume migrated and encoun-
tered aerobic condition downgradient. On long-term basis, the system-
atic decrease in ammonium along the groundwater flow path existed in
1992–2001 but in 2002–2015, levels of ammonium in R4 showed in-
crease and fluctuated above those in R2. The higher levels of ammonium
in R4 might be a result of end product of DNRA, in which nitrate serves
as an electron acceptor during an anaerobiosis. Another reason for the
increase could be release of ammonium from the aquifer sediment.
Clay-bearing sediment may constitute an important reservoir of ammo-
nium (Cozzarelli et al., 2011). The view that ammonium concentrations
should remain high in leachate from older landfills with low organic
content (Kjeldsen et al., 2002) is in contradiction to our finding, as by
2010, discharge of ammonium from the landfill had dropped below
2.5 mg/L. The relatively low ammonium concentration in our study
could probably be due to lower contents of both putrescible and recalci-
trant nitrogenous wastes dumped in Revdalen Landfill.
8
Science of the Total Environment 755 (2021) 143725
A plume of iron (II) was observed to infiltrate the aquifer from the
deepest part (Fig. 4B), which can be attributed to density effect. The
Iron is believed to originate from reduction of ferric iron by the leachate.
This is supported by the presence of other reduced species such as am-
monium, which showed a positive correlation with iron (Fig. 6D). The
correlation further suggests relatedness in source and attenuation of
these ions in the groundwater. The natural attenuation of iron was by
far the most efficient, as demonstrated by the remarkably low concen-
tration of iron in R4 (Fig. 5B). Such strong retardation of iron has been
ascribed to precipitation, cation exchange and dilution (Bjerg et al.,
1995). Besides dilution and cation exchange, precipitation as iron (II)
sulphide (pyrrhotite) and iron (II) carbonate (siderite) might have
been the main attenuation processes between R1 and R2. In classical
chemical reactions, formation of pyrrhotite is favoured to siderite due
to its lower solubility product (Fetter, 1993). By contrast, formation of
siderite might explain the strong attenuation of iron more than pyrrho-
tite, in accordance with the law of mass action, owing to the high con-
tent of bicarbonate in the leachate plume (Supplementary Figs. 1 & 3).
The bicarbonate likely originated from the landfill (Abiriga et al.,
2020), but microbial degradation of organic carbon could add to total
pool (Zhang et al., 2017). On the other hand, strong clearance of iron
midway between R2 and R4 might have been due to ferrous oxidation,
forming ferric oxyhydroxides. Oxidation is supported by the negative
correlation between iron and oxygen (Fig. 6E). Such oxyhydroxides
will provide efficient adsorbing sites for a variety of chemical species in-
cluding trace elements (Appelo and Postma, 2005; Chapelle, 2001).
However, the long-term observation (Fig. 5B) indicates there was an in-
crease in iron in R2 from 2009 to 2012, at levels higher than those in R1.
The increase was likely due to pyrite oxidation by nitrate, as data on ni-
trate seems to suggest so. This marked the beginning of breakdown in
the redox zonation with respect to iron, but the complete breakdown
was by 2013.
The highest manganese in this study was measured in samples from
R1, the closest to the landfill. Potential sources of manganese in landfills
are steel, batteries and glass, but microbial reduction of manganese ox-
ides during organic matter oxidation presents another source (Bjerg
et al., 1995). Soluble manganese undergoes similar attenuation pro-
cesses as iron (Bjerg et al., 2003), but iron is preferentially oxidised
and precipitates faster than manganese, such that manganese remains
longer in solution even under oxidising conditions (Horst et al., 2011;
Stumm and Morgan, 1996). The decrease observed between R1 and
R2 besides cation exchange, oxidation and dilution, could be due to pre-
cipitation as rhodochrosite and manganese sulphide. Like iron, much of
the precipitation reaction between R1 and R2 was possibly dominated
by formation of rhodochrosite, as the bicarbonate level in the ground-
water was high. The lack of clear pattern observed between R2 and R4
implies that manganese was under constant reaction and did not ex-
hibit truncation in its cycling. However, apparently most of the observa-
tions (Fig. 5C) indicate higher manganese in R4 than in R2. The complex
behaviour of manganese in the plume between R2 and R4, where for in-
stance, measurements in R4 were higher than in R2 could possibly be
due to reduction of sediment-associated manganese oxides by organic
matter in the plume, a reaction which increases manganese levels far-
ther out in the plume (Bjerg et al., 2003). The levels of TOC in R4 fluctu-
ated around 5 mg/L between 1992 and 2003 (Supplementary Fig. 2), but
the peak in 2001 for example coincided with a peak in manganese the
same year, which suggests reduction by the organic matter. Another
mechanism leading to reduction of manganese oxide is chemical oxida-
tion of iron (II) (Bjerg et al., 1995; van Breukelen and Griffioen, 2004), a
process that further precipitates the residual iron in the plume while
adding more manganese in solution.
4.3. Conceptual model for redox conditions in Revdalen Aquifer
The conceptual framework for redox zones in Revdalen Aquifer is il-
lustrated in Fig. 7. Complete absence of oxygen, nitrate and sulphate
D. Abiriga, L.S. Vestgarden and H. Klempe
Fig. 6. Correlations between the redox indicator species in the contaminated groundwater samples: sulphate versus oxygen (A), ammonium versus nitrate (B), ammonium versus oxygen
(C), ammonium versus iron (D), iron versus oxygen (E), and nitrate versus oxygen (F). The regression was performed on log10-transformed groundwater chemistry data. The corr(r) is the
Pearson's correlation coefficient.
observed at R1 suggests that R1 was located in sulphate-reducing envi-
ronment. This zone is expected to be within the first 30 m of a plume
(Ruegge et al., 1995), which is in agreement with our finding as R1 is lo-
cated 26 m from the edge of the landfill. Immediately after sulphate-
reducing zone is iron-reducing occurring 30–75 m (Ruegge et al.,
1995). Since the maximum iron was measured in samples from R1, it
is probable that both sulphate-reducing and iron-reducing zones
existed in the same part of the aquifer, an observation which is consis-
tent with the literature that anaerobic reduction of both redox species
may take place concurrently (McMahon and Chapelle, 2008; van
Breukelen and Griffioen, 2004). Two manganese-reducing zones were
present in Revdalen Aquifer, one upstream of R1 and another between
R2 and R4. While the first reduction was expected, the second reduction
was an interesting phenomenon, which implies that there was continu-
ous recycling of manganese in the aquifer. Nitrate-reducing environ-
ment would supposedly exist just after manganese-reducing zone, but
reduction of manganese oxide if present, should occur at about the
same redox potential as that of nitrate (Stumm and Morgan, 1996). As
9
Science of the Total Environment 755 (2021) 143725
described above, the observed decrease in nitrate at about the same
spot (R2-R4) was ascribed to nitrate reduction through DNRA. After
this there should be aerobic conditions, 250 m from the landfill
(Ruegge et al., 1995). We observed higher oxygen in R4 which is located
324 m from the landfill and presumably occupied the aerobic condition.
Such similar nitrate-reducing zone occurring in aerobic parts of the
plume has been reported (Heron and Christensen, 1995).
5. Conclusion
• The zonation of redox conditions in Revdalen Aquifer, which is a con-
fined aquifer, was found to be similar to those reported in the literature
from unconfined aquifers, partitioning in an increasing distance from
the landfill as; sulphate-reducing, iron-reducing, manganese-
reducing, nitrate-reducing, and finally aerobic condition. In the course
of delineating the redox process in the aquifer, sulphur and iron cycling
were found to be truncated, while nitrogen, manganese and carbon
underwent recycling along the groundwater flow path in the aquifer.
D. Abiriga, L.S. Vestgarden and H. Klempe
Fig. 7. Proposed distribution of redox zones in Revdalen Aquifer. The black dots denote positions of the multilevel in R1, R2 and R4, located downgradient of the landfill.
• On a long-term variation, there was an apparent breakdown in the
redox conditions of the aquifer. Concentrations of dissolved oxygen, ni-
trate and sulphate were observed to be increasing in the proximal well,
which was initially assigned to anaerobic zone. More years of monitor-
ing are required to understand if a transition to permanent oxidising
state within the landfill has been reached. To our knowledge, this is
the first study reporting long-term variation of redox chemical species
in a confined contaminated aquifer.
• Overall, the redox conditions provided a very good framework for nat-
ural remediation of Revdalen Aquifer. Within a distance of 324 m, the
redox conditions seemed to have resulted in nearly complete attenua-
tion of the landfill leachate plume. This has minimised negative envi-
ronmental impacts of the landfill leachate, which would otherwise
cause serious ecosystem degradation since the aquifer discharges into
a spring.
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.scitotenv.2020.143725.
CRediT authorship contribution statement
Daniel Abiriga: Conceptualization, Data curation, Software, Formal
analysis, Visualization, Validation, Writing - original draft, Writing - re-
view & editing. Live S. Vestgarden: Conceptualization, Resources, Super-
vision, Investigation, Writing - review & editing. Harald Klempe:
Conceptualization, Funding acquisition, Investigation, Methodology, Pro-
ject administration, Resources, Supervision, Writing - review & editing.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.
Acknowledgement
We thank Professor Andrew Jenkins for critically reviewing the man-
uscript. We also acknowledge the contributions of Tom Aage Aarnes and
all the technical staff at the department of Natural Sciences and
10
Science of the Total Environment 755 (2021) 143725
Environmental Health, University of South-Eastern Norway who partic-
ipated in fieldworks. The authors thank the five anonymous reviewers
for their extensive and insightful comments that significantly improved
the manuscript.
Funding sources
The study received financial support from the Research Council of
Norway [GRUF Project, 11139/720] and Bø Municipality. The funders
had no involvement in study design, data collection, writing of report
and decision to submit the article for publication.
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