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Use of environmental isotopes in leachate studies

through multiple isotopic analysis – a review

Anjali Bhagwat, Chandra Shekhar Prasad Ojha, Sudhir Kumar & Bhishm
Kumar

To cite this article: Anjali Bhagwat, Chandra Shekhar Prasad Ojha, Sudhir Kumar &
Bhishm Kumar (2024) Use of environmental isotopes in leachate studies through multiple
isotopic analysis – a review, Environmental Technology Reviews, 13:1, 214-234, DOI:
10.1080/21622515.2024.2315098

To link to this article: https://doi.org/10.1080/21622515.2024.2315098

Published online: 21 Feb 2024.

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ENVIRONMENTAL TECHNOLOGY REVIEWS
2024, VOL. 13, NO. 1, 214–234
https://doi.org/10.1080/21622515.2024.2315098

REVIEW ARTICLE

Use of environmental isotopes in leachate studies through multiple isotopic

analysis – a review
Anjali Bhagwata,b, Chandra Shekhar Prasad Ojhab, Sudhir Kumar a
and Bhishm Kumarc
a
National Institute of Hydrology, Roorkee, India; bDepartment of Civil Engineering, Indian Institute of Technology, Roorkee, India; cDepartment
of Nuclear Sciences and Applications, IAEA, Vienna, Austria

ABSTRACT ARTICLE HISTORY

Contamination of water resources by leachates emanating from different types of landfills and Received 1 May 2023
waste heaps is a serious concern. Proper management is possible, only after source Accepted 28 January 2024
identification. Statistical methods such as principal component analysis, Pearson correlation
KEYWORDS
coefficients and Hierarchical cluster analysis can indicate the sources of pollutants, but the Isotopes; environmental
quantification of contributions from each of the sources is not possible. Thus tracing the tracer; fractionation
movement of leachate plumes through environmental isotopes (stable and radioactive) is mechanism; leachate
gaining importance. Though the application of isotopes for source identification is an accepted
practice, the types and sources of pollution can be traced, and the various advantages and
disadvantages associated with the choice of isotopes are not well documented. Thus the review
first attempts to understand the possible use of conventional and potential isotopes under
different waste composition and try to summarize the isotopic signature of isotopes in different
sources and their variability to understand their applicability as a tracer of pollution plume. This
study shows that the applicability of δ13CDIC as a tracer is limited to subsurface environment.
Further, nitrogen isotopes δ15N-NH4 and δ15N-NO3 carry the signature of shallow aquifer and
thus cannot be applied as tracer for shallow aquifer. Isotopes of Boron, Strontium, Tritium, Lead,
Deuterium, Sulphur, Lithium and Cadmium are useful in tracing the leachate plume movement
both in surface and groundwater. The applicability of Boron, Sulphur and Lithium are limited by
adsorption. Strontium, Tritium, Lead and Cadmium show very low fractionation and thus
become potential candidate to be used as tracers.

Introduction
and industrial wastes where cities, towns and other
In developing countries where the population is amenities later develop. So, instead of a well-
growing at a rapid rate, waste disposal became a planned Landfill site what we often encounter is a
humongous task. With a lack of resources, the heap of waste dump which lacks provisions for elim-
dumping of Municipal waste is usually unplanned inating water, air and soil pollution. These waste
even in big cities like Delhi, Chennai, Mumbai, etc. dumps and the Leachate emanating from them
Another common practice is landfilling of mining have long-term consequences even after the

CONTACT Anjali Bhagwat [email protected] National Institute of Hydrology, Roorkee, Uttarakhand 247 667, India; Department of Civil
Engineering, Indian Institute of Technology, Roorkee, Uttarakhand 247 667, India
© 2024 Informa UK Limited, trading as Taylor & Francis Group
 ENVIRONMENTAL TECHNOLOGY REVIEWS 215

Landfills’ closure [1–3]. Leachate from the landfill is heterogeneous waste coming into the landfill results
generated both as a result of excess rainwater perco- in variation in the abundance of these isotopes and
lating through the waste heap and also because of thus each landfill shows a distinct isotopic signature
decompositions and compaction of waste which [21], which can be identified and thus management
lead to the generation of various acids [4–6]. These policies can be made which will help in deciding ame-
landfill leachates are a potential source of pollution liorative measures.
for surface and groundwater [6–8]. As surface pol- This review paper advocates the use of environ-
lution is easy to visualize, track and easy to control, mental isotopes both stable and radioactive to trace
the same cannot be said about the groundwater the leachate plume movement. The manuscript first
plume movement, which is both difficult to monitor attempts to understand the possible use of conven-
and estimate, and has long-term consequences. tional and potential isotopes under different waste
Various studies have been conducted to understand composition and then try to summarize the isotopic
the impact of landfill leachate on groundwater [9–14] signature of isotopes in different sources and their
and to understand the movement of leachate plumes variability to understand their applicability as a
in the subsurface environment. tracer of pollution plume. The study is an advance-
The waste disposal sites are usually located in areas ment over the existing reviews as it explains advan-
with the presence of other sources of contaminants tages and disadvantages associated with the use of
such as chemical industries, sewage treatment facili- conventional and potential isotopes as a tracer. This
ties, salt pans, packing industries, tanneries and so study provides an insight into the factors to be con-
on. In developing countries like India, the low-lying sidered while choosing an isotope as a tracer and
areas of cities are filled with municipal wastes on for determining the pollution contribution in a
which subsequent constructions are done [15], mixed contaminant scenarios.
these filled areas are subjected to long-term anaero-
bic decomposition and contribute to leachate gener-
Composition of waste in the landfill
ation [16,17]. When multiple sources of contaminants
are used to identify leachate plumes, such as heavy The relative strength and composition of environ-
metals, chloride, nitrates and hydrocarbons which mental isotopes are determined by the composition
are present near a landfill. The interpretation of of waste coming into the landfill. The relation
chemical data from monitoring well becomes compli- between various atoms and their heavier isotopes is
cated [18]. Statistical Methods such as principal com- unique to every landfill site and thus can act as a sig-
ponent analysis, Pearson correlation coefficients and nature which can be used for the identification of the
Hierarchical cluster analysis can indicate the sources source of leachate plume, its movement and the con-
of pollutants, but the quantification of contributions tribution of the plume in polluting surface and
from each of the sources is not possible. This results groundwater sources.
in both delay and lack of precision in the early detec- The composition of waste varies widely in different
tion of landfill leachate. To overcome the above limit- landfills. The various factors influencing waste com-
ation, environmental isotopes can be used along with position are economic development, culture, con-
monitoring of physio-chemical parameters of the lea- sumption pattern, climatic conditions, energy
chate plume. resources and pattern of waste collection and disposi-
Environmental isotopes are naturally occurring iso- tion [22]. Based on the difference in the composition
topes (both stable and radioactive) which vary in con- of incoming waste, landfills are categorized into five
centration and cannot be controlled by investigators types namely municipal solid waste landfill, construc-
[19]. These form the principal elements of hydrology, tion and demolition landfills, industrial landfills,
geology and biology, thus giving distinct isotopic sig- medical waste landfills and mixed waste landfill or
natures [20]. Commonly used environmental isotopes open dumps. Based on the literature reviewed,
are hydrogen (1H,2H and 3H), oxygen (16O and 18O), certain environmental isotopes are found to be
carbon (13C and 14C), boron (10B and 11B), strontium more suitable for studying leachate coming from
(86Sr and 87Sr), radon (222Rn), sulphur (32S and 34S), specific types of landfills. Table 1 enumerates
lead (206Pb, 207Pb) and nitrogen (14N and 15N). The various isotopes which are currently in use and
216 A. BHAGWAT ET AL.

Table 1. Landfill characteristics and associated isotopic investigation.

S.
No. Type of landfill Type of waste Potential Isotope used/studied
1. Municipal solid waste Waste predominantly coming from the household 3
H, δ 15N, δ 13C, δ 34S, δ H, δ
3 15
N, δ 13
C, δ 34
S
114
landfills Cd
2. Construction and Landfills accepting construction and demolition materials. E.g. wood 87
Sr/86Sr, δ 13C, δ11B 87
Sr/86Sr, δ C, δ11B
13

demolition landfills products, concrete, plasterboard, insulation materials, asphalt and

others are disposed to land
3. Industrial landfills Mostly mono fills, i.e. waste coming from specific industries δ11B, δ 114Cd δ11B
4. Mining waste Coal mining, Metal Extractions δ 34S, δ 15N, δ 114Cd δ 34S, δ 15N
4. Medical waste landfills Pharmaceuticals, organic and synthetic chemicals (Carbohydrates, 3
H, δ 15N, δ 13C, δ 34S 3
H, δ 15N, δ 13C, δ 34
S
lipids, amino acids, phenyl propane and humic acids)
5. Mixed waste landfill or Generally found in developing countries where waste segregation is (87Sr/86Sr), 3H, δ 15N, δ Strontium (87Sr/86Sr), 3H,
open dumps seldom practiced 13
C, δ 34S, δ11B, δ δ 15N, δ 13C, δ 34S, δ11B
114
Cd

those with the potential to be used as a tracer for lea- organic matter) and gaseous contaminants associated
chate movement along with the type of waste acting such as δ13CDIC, 13CCH4, 13CCO2 [26–29].
as a source. The weathering of silicate and carbonate minerals
As we can see from Table 1, various environmental is considered the primary source generating the Dis-
isotope options are available for studying each of the solved Inorganic Carbon (DIC). Reactions which lead
landfill, it becomes very important to understand to this weathering are (i) dissolution of soil CO2 with
various advantages and limitations that accompany the infiltrated rainwater which leads to the formation
the choice of these isotopes and the factors which of carbonic acid; (ii) acid rain or the presence of other
makes a particular isotope more suitable to be used strong acids [30]; (iii)CO2 dissolution from deep layers
for a particular type of landfill. (mainly in tectonically active areas). The contribution
to DIC concentrations and δ13CDIC values comes
from groundwater, uptake and release of carbon
Carbon isotopes in leachate
dioxide by plants, streams, CO2 invasion or evasion
The predominance of isotopes of carbon can be from the atmosphere and the breakdown of fat, pro-
observed in all five categories of landfill making it teins and carbohydrates present in the waste under
one of the most studied isotopes. The waste coming the methanogenesis process [18]. The δ13C values of
to municipal landfill has approximately 60–80% of DIC concentration give an idea about biogeochemis-
organic matter in it. The continuous degradation of try and carbon geochemistry of natural waters using
this organic waste leads to the enrichment of leachate Equation (1) [31]:
in dissolved inorganic carbon (DIC), volatile organic
carbon and non-volatile organic carbon. The fraction- d13 CDIC = d13 C(CO2 (aq)+ HCO−3 + CO2−
3 )
(1)
ation chart shown in Figure 1 for all three components
illustrates that a variation can be observed in the frac- The δ 13CDIC can be successfully used to trace the
tionation of organic carbon both in the case of ground- movement of leachate plumes in groundwater but
water and leachate samples [23]. Thus the plume when used for tracing the plume along the surface
movement through isotopic characterization for these water it suffers from various limitations. These limit-
is very difficult to study. However, the isotopic fraction- ations result because the contribution to δ13CDIC
ation in the case of dissolved inorganic carbon shows a values also comes from factors other than terrestrial
distinct signature of −20‰ to −10‰ in natural export of biogenic or geogenic DIC, and atmospheric
groundwater and +20‰ to +30‰ for the leachate CO2 evasion [32,33]. δ 13CDIC value of stream also
samples. Thus the dissolved inorganic carbon (DIC) carries the influence of biogeochemical processes
needs to be estimated for tracing the plume. In such as weathering of silicate-containing minerals
tracing the leachate pollution in groundwater [34–36], anaerobic metabolism [37,38], in-stream res-
sources, carbon isotope as dissolved inorganic carbon piration [39–41], photo-oxidation of DIC [42,43] and
(δ13CDIC) is widely used [24–26]. DIC is often considered photosynthesis by instream plants [44–46]. Because
in tracing different pollutants (VOCs, inorganic carbon of these multiple sources and sinks and their associ-
compounds, dissolved organic matter, xenobiotic ated isotopic effect, the δ13CDIC values in the stream
 ENVIRONMENTAL TECHNOLOGY REVIEWS 217

Figure 1. The isotopic fractionation of carbon isotope for volatile, non-volatile and inorganic in (a) groundwater and (b) leachate.

show wide variation typically from +5‰ to −35‰ [47]. The landfill leachate gets enriched in boron iso-
On the other hand, the δ13CDIC values of groundwater topes by the decomposition of end products of indus-
in the catchments generally are in the range of −5‰ to trial waste coming from glass and proclaim
−25‰ [48]. Such wide variation leads to failure in the manufacturing, leather, carpet, cosmetic, photo-
differentiation of influences and processes on δ13CDIC graphic, fertilizers, wire and metal industry, etc.
value and can result in incorrect interpretation of the which widely utilizes boric acid and borate minerals
sinks and sources of DIC in streams. [59]. In developing countries like India, bleaching
powder is readily used for the removal of microorgan-
isms from the leachate at the surface of landfill [60].
Boron in leachate These bleaching agents which are nothing but
enriched sodium perborate [61] become a source of
The two stable isotopes of Boron are 11B (80.1%) and 10B boron enrichment in landfill leachate.
(19.9%). The relatively large mass difference between The isotopic signature of boron is defined by the
the two isotopes results in a wide range of δ11B values following equation:
in natural waters, from −16% to +59% [49–52]. This ⎡
11  ⎤
makes Boron isotopes to be used extensively in report- B
sample
⎢ B10 ⎥
ing groundwater pollution such as sea water intrusion d11 B = ⎢
⎣
B11  − 1⎥
⎦ × 1000 (2)
[53,54], leachate studies from fly ash dump [55] and NBS951
landfill leachate contaminations [21,56–59]. B10
218 A. BHAGWAT ET AL.

where the SRM-NBS 951 boric acid serves as a in the isotopic signature of the strontium source
standard. [73]. This makes strontium an effective tracer for lea-
The δ11B values in leachates coming out of munici- chate migration studies.
pal landfills are −3‰ to 10‰ [56–58]; for domestic The isotopic signature of strontium coming from
waste water δ11B varies from 0‰ to 12‰, for landfill leachate is 87Sr/86Sr = 0.708457 [73], the sur-
sewage contaminated groundwater δ11B is 3–25‰ rounding groundwater is 87Sr/86Sr = 0.708175 [73],
whereas δ11B value for uncontaminated groundwater the fertilizer enriched effluents coming from agricul-
is approximately 19‰ [21,59]. Representing a signifi- tural fields 87Sr/86Sr = 0.707859 [73] and seawater is
cant variation which is outside the mass spectro- 0.7090720 ± 0.00004. [74] present a significant vari-
metric uncertainty range of 0.2–0.4‰ [62] making ation which is well outside the range of mass spectro-
boron isotopes an apt tracer. But the use of Boron metric uncertainties, which is at most 20.0187%. The
87
as a tracer is limited by factors such as half-life, Sr and 86Sr ratio thus becomes very effective in
which is of 1 day [63] and thus can be used only to detecting and differentiating the pollution caused
illustrate the mixing of fresh leachate in groundwater. by landfill, overuse of fertilizers and saline intrusion
Another limitation is its adsorption on clay minerals, responsible for increased TDS.
which is maximum at pH 8–9.7 [64,65]. The pH value
of Landfill leachate ranges from 4.5 to 9 [7]. As most
landfill leachate shows a pH of 8 or above in Indian cli- Tritium in leachate
matic conditions [66,67]. Boron adsorption becomes a Tritium is the radioactive isotope of the hydrogen
serious limitation. atom; this is the only environmental isotope which
is part of the water molecule, whereas all other iso-
Strontium in landfill leachate topes are dissolved in water. When Tritium replaces
one of the hydrogen molecules in water it is known
The four naturally occurring isotopes of Strontium are as Tritiated water (HTO). Thus the tritium content in
88
Sr, 87Sr, 86Sr and 84Sr. The approximate relative abun- water is expressed in Tritium Unit (TU), i.e. 1 TU =
dances are 82.53%, 7.04%, 9.87% and 0.56%, respect- 13H per 1018 Hydrogen atoms. In terms of radioac-
ively [68,69]. As the formation of radiogenic 87Sr tivity, one TU is 0.118 Bq/kg or 3.19 pCi/kg or 7.1 dis-
results from the natural decay of 87Rb, there is a signifi- integrations per minute/L of water [75,76].
cant variation in the isotopic abundance of strontium Since Tritium is a radioactive isotope it can be used
in nature. It is the age and Rb/Sr ratio which deter- for tracing the plume via two methods namely: (a)
mines the isotopic composition of strontium in rocks comparing the ratios of HTO to water molecule
and minerals containing rubidium [68,69]. The stable which serves as the signature of the source and (b)
isotopes of strontium undergo low biological or geo- calculating the residence time of groundwater and
logical fractionation in the environment [70]. The coupling it with chemical analysis to trace the move-
difference in isotopic ratios of strontium gives unique ment of the plume. The first method is employed in
characteristics to different Sr-containing sources. various studies as illustrated in Table 2. This method
Therefore, stable isotopes of strontium can effectively is based on the identification of various sources
be used as a tracer for identifying sources of pollution responsible for tritium production and distinguishing
and transport processes taking place in the environ- leachate plumes from the surrounding surface and
ment [65,71,72]. groundwater on basis of HTO/H2O ratios.
Since the ionic radius of Strontium is larger than In nature, the bombardment of nitrogen and deu-
calcium, strontium replaces calcium in many com- terium atoms by cosmic rays leads to the formation of
pounds. Thus wastes such as plastic, cement, plaster tritium as illustrated in the following equations:
and other manufactured products contribute to
strontium in the landfill leachate [21]. The stron- N14 + n  C 12 + H3 (3)
tium-enriched leachate plume gets attenuated as it
H12 + H12  H13 + H11 (4)
undergoes sorption or cation exchange, but very
low (0.0115) isotopic fractionation is observed. Thus The main anthropogenic cause of tritium enrich-
the little variation in mass does not cause a change ment in the environment is Nuclear Weapon Testing
 ENVIRONMENTAL TECHNOLOGY REVIEWS 219

Table 2. Tritium concentration in leachate from various landfills. is tritium enriched and the value ranges from 1700 to
Maximum Minimum 150 TU [89,90], it is easy to trace the leachate plume
Name of tritium level tritium
landfill Location (in TU) level (in TU) References by measuring tritium value which is well above the
Illinois Champaign 8001 227 [18] natural range. But in cases where the tritium value in
Municipal UK 39,270 450 [79] leachate ranges from 30 to 10 TU or less [91,92], the
Landfill site
Municipal South Korea 1196 17 [186] identification of leachate plume only through tritium
Landfill site
Municipal New York, USA 60,136 30 [86]
measurement becomes difficult.
solid Another method by which plume can be traced
Landfill site
Municipal Northern Italy 1700 400 [89] using tritium isotope is calculating the residence
Landfill site time of groundwater which will reflect its velocity
Municipal Manilla, 480 150 [90]
Landfill, Philippines and monitoring the physicochemical parameters in
Metro the surrounding area. Since most of the landfills are
Andralanitra Antananarivo– 22.82 10.83 [91]
landfill site Madagascar designed for 10–25 years of active life and 25 years
post closure, tritium can effectively be used as a
tracer for understanding plume migration.
which started in the 1950s and reached its peak in the
1960s. Thus before the 1950s the estimated tritium
level in the atmosphere was 5–10 TU [19] but the Nitrogen in landfill leachate
atmospheric testing of thermonuclear devices
increased the tritium level to hundreds and thou- Nitrogen compounds show a wide range of oxidation
sands of TU [77]. For example, the tritium levels for states (−3 to +5) and thus, have a range of isotopic
Chicago rain and snow between December 1957 compositions. Nitrogen has two stable isotopes, 14N
and July 1958 ranged from 54 to 2160 TU [78]. The and 15N and 14 radioactive isotopes with 13N having
landfills constructed between the 1950s and 1970s the highest half-live of 9.90 min among the radio-
received tritium-enriched precipitation. The presence active isotopes [93]). Thus it is mostly the stable iso-
of refuse material increased the retention time for this topes of nitrogen, which is being used for
tritium-enriched precipitation inside the body of the hydrogeological surveys, contaminant studies and
waste-dump making landfill leachate high in concen- study leaching from coalmines [94,95].
tration of tritium [79]. But tritium is short-lived having The biodegradable waste coming to the landfill
a half-life of little more than 12 years [78,80,81] forms the main source of nitrogen, as it contains
[82,83], thus the enriched precipitation can have an about 15% of protein [96]. The decomposition of
impact maximum of 40 years, i.e. the imprints of rain- protein results in the formation of ammonium as illus-
fall events will last by the year 2000. Various studies trated by Equation (5).
have assumed a direct relationship between the his- C46 H77 O77 N12 S {1kg} + H2 O {0.324kg}
torical record of tritium associated with past precipi- = C69 H138 O32 {0.563kg} + CH3 COOH{0.282} (5)
tation and the concentration of tritium in landfill + CO2 {0.26kg} + NH3 {0.183kg} + H2 S{0.033kg}
leachate [84,85]. But this method of interpreting
tritium level in leachate based on historical precipi- Though the formation of ammonium in landfill
tation is misleading [18]. The identification of landfill depends on the proportion of protein in the waste
as the source of pollution for groundwater in later composition. Wang et al. [97] reported that a high
studies is carried out where tritium is contributed by ammonium concentration of 3500 mg/L is commonly
new anthropogenic sources such as nuclear power found in landfills making these dump sites sources of
plants and some manufactured products such as ammonium. Nitrogen in the form of nitrate is con-
gaseous tritium lighting devices, GTLD [86], watches, tributed to the landfill by agricultural waste and
clocks and luminous paints [79]. industrial waste [98]. Thus the isotopic characteriz-
In recent years, the natural value of tritium in uncon- ation of landfill nitrogen present in the form of δ
taminated groundwater varies from 2–3 to 10–11 TU 15
N-NO3 or δ 15N-NH4 is done to evaluate landfill as
(where there is no evidence of post bomb signature) a source of groundwater and surface water pollution
[87,88]. For municipal landfill sites where the leachate [25,99–102].
220 A. BHAGWAT ET AL.

The δ15N-NH4 of sewage is around 3‰ [25] com- Lead isotopes in leachate

pared to the marine δ15N-NH4 value which is 7‰
In a mixed landfill site where waste segregation is not
[103], a low δ15N-NH4 value between −3‰ and 2‰
practiced, leachate gets enriched in lead isotopes
represents the source as chemical fertilizers [99], the
which are contributed by sources such as Plastics,
δ15N-NH4 value for uncontaminated groundwater is
Paints, storage batteries and other manufactured
26‰. With varying δ15N values for seawater, leachate,
goods [113]. Lead isotopes are also contributed to lea-
fertilizers and uncontaminated groundwater, nitro-
chate as a by-product of U-Th radioactive decay [114],
gen isotopes become an important tool for identify-
which is contributed to landfill by the coloured
ing the source of pollution in groundwater.
glasses which fluoresces under ultraviolet light, col-
Nitrogen isotopes are also used for tracing the lea-
ouring ceramic where uranium oxide is employed
chate plume that comes out from the mines. The
and in sandstones and soft aggregates where
emanating leachate gets enriched in nitrogen iso-
uranium vanadates (K2 (U02)2(V04)2.3H2O) is found
topes as a consequence of blasting in the mines by
as a yellow or green-yellow crust [115].
nitrogen-based explosives like ammonium nitrate
Lead is an active tracer molecule because of its
(NH4NO3) which is mixed with ammonium nitrate
stable isotopes 206Pb, 207Pb, 208Pb, which are a
fuel oil (94–98% NH4NO3 and 2–6% fuel oil)
product of U-Th radioactive decay [114] by the follow-
[104–106]. Mahmood [107] analysed the δ15N values
ing reactions as shown in Equations (6) and (7) and
for leaches emanating from a coal dump in Elk
Figure 3(a–c) [116]
valley, Canada and reported δ15N-NO3 in pre-blasted
rock, Ammonium nitrate fuel oil, freshly blasted rock 233
U  209
Pbunderclusterdecayof 7.2
samples and the leachate from the waste dump to
× 10−11 % (6)
be 2.2‰, 3.34‰ and 7.23‰ respectively. The δ15N-
NO3 value of groundwater samples below 26–57 m
below ground level (bgl) was 11.4‰ whereas the
232
U  208
Pbunderclusterdecayof 8.9
δ15N-NO3 value for samples collected from 40 to × 10−10 % (7)
80 m bgl is −2.49 ‰. Thus the mining leaches can
be considered as the source of δ15N enrichment (https://en.wikipedia.org/wiki/Isotopes_of_uranium)
(Figure 2). Though the concentration of lead isotopes varies
Though isotopes of nitrogen prove to be a success- due to the dilution and attenuation process these
ful tracer, the δ 15N-NO3ˉ and δ15N-NH4 values can ratios do not undergo a measurable change in phys-
sometimes be biased because of (a) physio-chemical ical, chemical and biological parameters and thus
or biological processes which remove or add nitrogen show a distinct isotopic signature helping in tracing
compounds within the soil and subsurface water and the plume movement [117,118].
(b) kinetic isotopic fractionation as a result of The isotopic signature of lead in the leachate of
microbial activity [108]. The denitrification process municipal landfill sites is 206Pb/207Pb = 1.189–
led to the release of lighter nitrogen isotopes to the 1.193‰ [113,119], which differs significantly from
atmosphere as N2 which led to the enrichment of δ the groundwater represented by lead isotope
15
N-NO3ˉ. Thus this enrichment should be taken into 206
Pb/207Pb range from 1.1695‰ to 1.2216‰ [120]
account whenever there is the availability of organic and the isotopic signature of lead found in the atmos-
carbon. The organic carbon acts as an electron phere 206Pb/207Pb which ranges from 1.150 to 1.16 as
donor and microbes use NO3ˉ as an acceptor of elec- reported by [113]. Thus lead can be used as a tracer
trons [38,109–111]. (c) When several distinct source for groundwater pollution movement.
mixes, for example, nitrogen enrichment occurs With negligible isotopic fractionation and degra-
both by seawater intrusion and leachates from dation during biological and physicochemical pro-
landfill the chemical measurement of ammonia and cesses lead proves to be the apt choice for
nitrate may be misleading [112]. (d) The changes in contaminant source identification but with a half-life
isotopic concentration of nitrogen are because of of 3 × 10−7, 0.52 s and 138.4 days for 208Pb, 207Pb
ammonia volatilization, nitrification, denitrification and 206Pb respectively, the study related to the move-
and plant uptakes [108]. ment of older leachate plume gets restricted.
 ENVIRONMENTAL TECHNOLOGY REVIEWS 221

Figure 2. Isotopic profile of (a) ammonia (δ 15

N-NH4) and (b) nitrate (δ 15N-NO3).

Isotopes of hydrogen and oxygen in leachate deviation from the line indicates mixing or isotopic
study exchange with other sources and thus can be used
as a tool to trace recharge sources, migration path
δ18O and δ2H correlate on a global scale by Equation
and retention time of water bodies [123].
(8) called the ‘Craig’s global meteoric line’ defining the
The rainfall which percolates through the solid
relationship of 2H and 18O in freshwater worldwide.
waste comes in contact with the organic acids result-
d2 H = 8d18 O + 10‰ ing as the by-product of waste degradation. In the
process of coming in contact with the high organic
(Craig [121]) (8) content which undergoes aerobic and anaerobic
Craig’s line which is global in the application needs decomposition the isotopic composition of percolat-
to be modified in both slope and intercept based on ing water gets modified and becomes a signature of
prevailing climatic and geographical factors to be the landfill [18,124,125]. To understand the migration
applied in the local conditions. This meteoric relation of leachate plumes in river and groundwater [126]
between δ2H and δ18O arises due to isotopic fraction- collected samples of shallow groundwater ranging
ation during evaporation and condensation processes from 0 to 40 m from ground level, leachate and
[122]. Thus the relation between δ2H and δ18O from water from the river surrounding Bantar Gebang
different water bodies, such as atmospheric water landfill site of Java. The values of δ18O and δ2H for
vapour, precipitation, surface waters, soil water and the Cibitung River ranged from −7.56‰ to −6.20‰
groundwater has a distinct figure print and a and −42.9‰ to −38.9‰ respectively as shown in
222 A. BHAGWAT ET AL.

Figure 3. Uranium–thorium decay forming isotopes of lead: (a) 206

Pb, (b) 207Pb and (c) 208Pb.

Figure 4. Their shallow groundwater close to the Cibi- for the Bantar Gebang landfill site are in the range of
tung River gave rather more enriched values of −4.21‰ to −5.58‰, −25.4‰ to +4.3‰ respectively.
−7.33‰ to −5.77‰ for δ18O and −42.8‰ to Similar enrichment in δ2H values for leachate is
−31‰ for δ2H. The δ18O and δ2H values for leachate observed in samples of three active sites in Illinois,
 ENVIRONMENTAL TECHNOLOGY REVIEWS 223

Figure 4. δ18O and δ2H isotopic distribution near Bantar Gebang landfill site.

USA, which ranges from −60.0‰ to +14.5‰ [18] and tracer for the identification of pollution coming to
the value of δ2H ranged from −47‰ to −4‰ for four groundwater and surface water from agricultural
active sites of New Zealand [127]. runoff, wastewater, mines and illustration of rock–
Thus the leachate is highly enriched in deuterium water interactions. For example, 18O is used to trace
and moderately enriched in oxygen-18 isotopes nitrate contamination of groundwater by agricultural
when compared to freshwater samples collected or wastewater sources, as expressed in coupled nitro-
from ground and surface water. This positive shift gen and oxygen isotope ratios [102], 18O isotope to
in the isotopic composition of deuterium can be trace potential sources of sulphate contamination in
attributed to huge methane production. During groundwater [129], source of nitrate and ammonia
methanogenesis isotopic fractionation occurs with pollutant in groundwater [130]. As a result, oxygen
the preferential association of lighter isotope with and deuterium isotopes are effectively used by
the gas phase, CH4, leaving the heavier isotope in various landfill studies for tracing the pollution
the liquid phase leading to the enrichment of plume [24,91,126,131]. But a certain limitation of
2 1
H/ H ratio [90,122]. The methanogenesis process using these isotopes needs to be kept in mind.
does not affect the oxygen isotopic composition The δ18O and δD values are normally preserved
[128] and thus only a moderate enrichment of after the precipitation enters the groundwater as
oxygen isotopes can be observed. It means that the oxygen and hydrogen isotopes are nonreactive
2 1
H/ H ratios from leach waterfalls outside of the in shallow groundwater systems. The conservative
ranges associated with natural groundwater. The nature of these isotopes makes them an effective
anomaly values of 2H/1H ratios in groundwater sur- tool for tracing groundwater pollution [84,132]. But
rounding landfill sites can be used as an indication the leachate transported through the river does not
of leachate migration [122]. show this distinct signature [90,126]. This was prob-
The δ2H value for leachate shows seasonal vari- ably caused by the amount of natural water in the
ation +16‰ in the dry season and +6‰ in the wet river which was comparatively large, with respect to
season both of which show deuterium excess in com- limited leachate discarded to the river. Moreover,
parison to freshwater [90]. Thus tracing the seasonal the isotopic ratio in river water represents a much
plume movement through deuterium observation closer signature of precipitation than leachate. This
becomes a possibility. Apart from this, oxygen iso- limits the use of both deuterium and oxygen isotopes
topes and deuterium are also used indirectly as a as an effective tracer of plume movement in the river.
224 A. BHAGWAT ET AL.

Isotopes of sulphur in the landfill leachate enriched in sulphate isotopes with δ34SSO2− 4
value
ranging from 10.9‰ to 25.6‰ [141,142]. Thus the
Sulphur has four stable isotopes: 32S (95.02%), 33S
enrichment in sulphate isotope in groundwater and
(0.75%), 34S (4.21%) and 36S (0.02%). The abundance
surface water will give an indication about the lea-
ratio of 34S and 32S is generally given as a δ34S
chate movement.
value, defined analogously to Equation (9)
The use of sulphur isotopes for pollution studies
R34S and for source identification depends on the
d34 S = − 1 (1000‰) (9) reasons for the fractionation of isotopes and the pro-
R32S
cesses involved in bringing the changes in isotopic
Sulphur isotopes are contributed to groundwater ratio. Two primary processes are found to be respon-
by both natural sources and anthropogenic sources. sible for the fractionation of sulphur isotopes: (i) the
The natural sources consist of atmospheric depo- anaerobic bacteria (Desulfovibrio desulfuricans) which
sition, rock–water interactions and where sulphate reduces sulphate to sulphide are more inclined to
containing mineral mainly, gypsum oxidizes to from utilize the lighter isotopes (32S) which results in the
sulphide, precipitation and volcanic activities. The enrichment of δ34S [143–145] and (ii) exchange reac-
anthropogenic contributions come from sewage tions where heavy isotope (34S) is concentrated in
infiltration, synthetic detergents, fertilizers and the compounds having the highest oxidation state or
dumping of coal combustion by-products [129]. greatest bond strength [146].
The isotopic signature of sulphur shows a distinct The municipal landfills though have a potential
value for different sources for example δ34S values source of sulphur and show a distinct isotopic ratio,
originating from atmospheric deposition are limiting the use of sulphur isotopes. The dump sites
between −3‰ and 12‰ [129], for fertilizers the are enriched in sulphur-reducing bacteria [147]
value of δ34S lies between −7‰ and 21‰, for deter- which leads to the formation of H2S gas and in this
gent, it ranges from −3.2% to 25.8% [133], the δ34S process consumes the lighter isotopes. The changing
value for evaporates, pyrites and sewage are −14‰ isotopic ratio of sulphur by anaerobic bacteria is
to 35‰, −15‰ to 4‰ and 2–12.5‰ respectively dependent on temperature profile, physio-chemical
[129,134]. conditions prevailing inside the landfill and age of
Sulphur form the major component of mineral waste thus there is no specific signature of the isoto-
forms of coal amounting to 1000 g/t of the solid pic ratio of sulphur representing the dump site. There-
fuel [135]. The use and disposal of coal combustion fore, it is safe to say that if no other sulphur-
by-products (CCBs) [i.e. fly ash, bottom ash, flue gas- contaminating source is present an enriched δ34S
desulphurization material and pressurized fluidized value can be used as an identifier of a landfill plume.
bed combustion (PFBC) material] at coalmines, thus, In the case of landfills receiving waste from coal
makes sulphurisotopes an apt choice for tracing the mines or industries which are enriched in sulphur iso-
movement of leachate coming out from coal topes and low availability of organic waste, the use of
mines [136–138]. In developing countries like India, sulphur isotopes proves to be a reliable technique for
coal is used for cooking, and the fly ash thus produced tracing the pollutant movement. In the case of indus-
is disposed of in municipal landfill [139]. Moreover, trial waste, reduction of sulphate to sulphide is
the waste to energy plants located at the landfills is restricted because of the unavailability of sulphur-
also dumping fly ash in the dump yards. This makes reducing bacteria but the adsorption of sulphur on
use of sulphur isotopes as a potential candidate for metal [129] determines the usability of sulphur iso-
tracking the plume movement of leachate from topes as a tracer.
dumping yards.
The sulphate isotopes δ34SSO2− for uncontaminated
4 Lithium isotopes in landfill
groundwater falls in a very range of 0.4–4.3‰ and for
uncontaminated river or surface water sources it lies Lithium is one of the lightest metals in its elemental
in the range of 0.5–4.4‰, since most of the sulphur form and is highly reactive as an element. Because
is added through the anthropogenic sources [140]. of its high reactivity, lithium does not occur as a
The leakages from the municipal landfills are highly pure element in nature but occurs as stable minerals
 ENVIRONMENTAL TECHNOLOGY REVIEWS 225

and salts (petalite, lepidolite and spodumene). In the −51.1 0/00 [154]. However, the rock–water interaction
environment, we found two lithium (Li) isotopes 6Li supports the isotopic fractionation leading to enrich-
(7.59‰) and 7Li (92.41‰), having a relative mass ment of 7Li and thus a high value of 850–12600/00 is
difference of up to 16%, being the largest among reported in deep aquifers of peat land, France [155].
metal elements. In natural groundwater, lithium is Further, the δ 7Li is between −37 and −44 0/00 for
found as a trace constitutes (1–100 µg/l) [148,149]. the transition zone between fresh and seawater the
But anthropogenic sources such as landfill leachate, δ 7Li ranges from −220/00 to −270/00. Thus lithium iso-
agricultural waste, fly ash and petroleum products topes can be useful in distinguishing the source of
have an elevated Li concentration of 100–500 mg/l groundwater salinization [58,156].
[55,59,150,151]. The main source of lithium in Choi et al. [152] evaluated the lithium isotopic com-
landfill leachate can be attributed to the increased position at the upstream and downstream regions of
use of electronic devices, chips and sensors in our the Bukhan River and the Namhan River passing
day-to-day useable products [152]. The dumping of Seoul, South Korea. The δ 7Li values at the upstream
the lithium–ion batteries from electric vehicle indus- are found to be greater than 25‰, when the rivers
tries, photovoltaic panels and waste generated from crossed Seoul city δ7Li values experiences a signifi-
lithium battery manufacturing units contributes to cant decrease from 30.1‰ to 19.2‰. The δ 7Li of
increased lithium concentrations in leachate emanat- effluents coming from the wastewater registers a
ing from industrial sectors [153]. value of 14.5 ± 4.3‰, indicating the impact of anthro-
Li has a low atomic weight of 6 atomic mass unit pogenic activities on rivers. Manaka et al. [157] inves-
(amu) and a high relative mass difference of 1.0009 tigated the isotopic composition of lithium in river
amu between 6Li and 7Li resulting in a significant water of Ganga–Brahmaputra (+19.1‰ and
difference in the natural abundance of the two iso- +34.2‰) and groundwater of Bengal Basin (+5.1‰
topes. Thus isotopic fractionation results in significant to +11.6‰) thus the groundwater and surface water
natural variation in the isotopic composition of interface can be easily distinguished (Figure 5).
elements containing Lithium [58]. Thus lithium Thus we can conclude that although the isotopes of
shows a distinct isotopic signature which forms the lithium have not been used so far as a tracer for plume
base of source identification. δ 7Li for shallow aquifer coming from MSW landfills it holds great potential
are highly depleted and ranges from −21.50/00 to because of (i) changing nature of waste generation,

Figure 5. δ 7Li isotopic distribution near Seoul city, indicating unique δ 7Li signature for different effluents and the groundwater.
226 A. BHAGWAT ET AL.

(ii) it does not undergo any chemical reactivity [158], Equation (10) [170,171]:
(iii) it is not affected by the phytoremediation under-
taken at the landfill sites as it is not up taken by the d114 Cd/110 Cd = [(114 Cd/110 Cd)sample /
plants as it has no know the biological role [159]), (10)
(iv) since elevated mobility of lithium is thought to (114 Cd/110 Cd)NIST SRM 3108 − 1] × 103
be related to temperature and found a high concen-
tration of lithium in thermal waters. The usability of Cadmium isotopes are associated with sulphide min-
δ 7Li isotopes as a tracer is limited because it occurs erals such as sphalerite (ZnS), pyrite (FeS2) and galena
as lithium occurs as a monovalent cation in solution (PbS), and thus the leachates associated with dumped
and thus adsorption and cation exchange reactions mining waste are heavily enriched with the cadmium
are to be expected. isotopes [172–177]. Variations of Cd isotopes in sul-
phide-rich ores ranged from (d114 Cd = −1.64–0.23‰).
The river water close to the tailing area was strongly
Cadmium isotopes in leachate studies
enriched in heavier isotopes from 0.64‰ to 1.03‰
Cadmium is a scarce non-essential element and it is [178]. The isotopic signature of Cadmium near farmland
found in an insignificant amount in natural waters was registered as δ 114Cd/110Cd 0.21–0.35‰ [169]. Thus
[160]. The average cadmium content in the world’s the cadmium isotope can successfully be used as a
oceans has been reported as 5–20 ng/L [161,162]. tracer for identifying pollution coming to the river
The amount of cadmium present in rainwater, fresh from mining and agricultural fields.
waters and surface waters in urban and industrialized In industrial processes which operate at high temp-
areas shows a significant variation and ranges from 10 eratures such as smelting, glass manufacturing and
to 4000 ng/L [161–163]. The amount of cadmium in coal-fired power plants, lighter Cd evaporates into
an industrial area is in the range of 15–150 ng/m3 the vapour phase, while heavier Cd remains in the
whereas in rural areas the concentration ranges residual phase (slag). Thus, both wastewater (0.26–
from 0.1 to 5 ng/m3, which is also reflected in Cd 0.41‰) and slug coming out (0.34–0.47‰) are
isotope enrichment in the industrial area [119]. The enriched with heavier Cd relative to the raw material
various sources considered to be responsible for [173,175,177,179].
cadmium entering the water bodies are weathering Though Cd isotopes are not used as a tracer for
and erosion of soils and bedrock, atmospheric depo- municipal leachates, they can prove as a potential
sition, direct discharge from industrial operations, candidate: (a) municipal wastes are high in humic
leakage from landfills and contaminated sites, and acid content (45–49%) and Cadmium has a natural
the dispersive use of sludge and fertilizers in agricul- affinity for humic acids which results in swift accumu-
ture [119,164–167]. The unsegregated wastes lation of cadmium onto landfill leachate [180], (b) not
coming from the landfill contains a variety of sub- affected by the phytoremediation measures carried
stances such as paints, plastics, batteries etc. contains out at the landfill site as it has no known biological
cadmium as an additive material in paints and plastics role [119,181,182] and (c) does not undergo chemical
and main constitutes of Ni–Cd batteries [168], thus reactivity.
the leachates so produced are the heavily enriched In spite of having many benefits certain points
in cadmium isotopes. Though found in an insignifi- need to be taken into consideration before using
cant amount in nature, cadmium shows a distinct sig- cadmium as a tracer: (a) Cd isotope undergoes isoba-
nature with non-contaminated and anthropogenic ric and molecular interferences from major elements
sources [169]. (e.g. Na, Mg, Ca, Fe, Al and Zn) and trace elements
There are eight stable isotopes: 106Cd (1.25%), (e.g. In, Sn and Pd) thus it is prerequisite to separate
108
Cd (0.89%), 110Cd (12.49%), 111Cd (12.8 0%), 112Cd Cd from sample matrix before mass spectrometric
(24.1 3%), 113Cd (12.2 2%), 114Cd (28.7 3%) and analysis [170]. (b) To observe the fractionation of Cd
116
Cd (7.49%) [170]. The cadmium isotopic fraction- isotopes, high-precision analysis is required
ation is expressed in terms of relative deviation w.r.t [183–185]. (c) Much of this cadmium entering the
standard reference (NIST SRM 3108 Cd solution in fresh waters from industrial sources may be rapidly
parts per 1000 (δ) 114Cd/110Cd) as described in adsorbed by particulate matter [169].
 ENVIRONMENTAL TECHNOLOGY REVIEWS 227

Table 3. Summary of isotopic signature in leachate, surface water and groundwater sources.
Isotope Symbol Leachate (‰) Surface water (‰) Groundwater (‰)
Carbon (Inorganic) δ13CDIC 20–30 −35–5 −20 to −10
Boron δ11B −3–10 10–28 19–25
Strontium δ87Sr 0.708457 0.707859 0.708175
3
Tritium H 2–11 TU 0–22 TU 10–1700 TU
Ammoniacal Nitrogen δ15N-NH4 3–7 0–26
Nitrate δ15N-NO3 2.2–7.23 −3–11
206
Lead Pb/207Pb 1.189–1.193 1.15–1.16 1.1695–1.2216
Deuterium δD −25.4–4.3 −42.9 to −38.9 −42.8 to −31
Oxygen δ18O −4.21 to −5.58 −7.56 to −6.20 −7.33 to −5.77
Sulphate δ34SSO2−
4
10.9–25.6 0.5–4.4 0.4–4.3
Lithium δ 7Li 14.5–18.8 19.1–34.2 −21.5 to −51.1
114
Cadmium d Cd 0.26–0.47 0.21–0.35

Conclusion iv Applicability of Boron, Sulphur and Lithium iso-

topes is limited by adsorption.
To understand the impact of landfill leachate on
v Strontium, Tritium, Lead and Cadmium show
surface and groundwater and to plan strategies for
very low fractionation and thus become poten-
the mitigation of leachate plumes, it becomes impor-
tial candidate to be used as tracers.
tant to trace the sources of incoming pollution. The
application of environmental isotopes is a well-estab-
Because of the various pros and cons associated
lished approach to detecting the presence of anthro-
with the single-element isotopic signature, the dual
pogenic contamination and pollution sources. The
isotope approach is preferred for robust and decisive
choice of isotope depends on the types and sources
source identification.
of pollution which can be traced and various advan-
tages and disadvantages associated with the chosen
isotopes. Further, the applicability of the isotope as
a tracer depends upon its unique signature in lea- Acknowledgement
chate, groundwater and surface water. Thus, in this This work was supported through a project titled ‘Leachate
review the isotopic ranges of different isotope are Transport Modelling for Gazipur landfill site and suggesting
documented and summarized in Table 3. Ameliorative measures’ (Grant Ref: SP-28/2019–20/PDS-19)
under National Hydrology Project.
Based on the isotopic range and various pros and
cons associated with different isotopes, following
conclusions can be drawn:
Disclosure statement
No potential conflict of interest was reported by the author(s).
i Isotopes of Boron, Strontium, Tritium, Lead, Deu-
terium, Sulphur, Lithium and Cadmium are
useful in tracing the leachate plume movement Data availability statement
both in surface and groundwater.
All data used during the study are available from the corre-
ii Among the organic, inorganic and the volatile frac- sponding author by request.
tion of carbon, only the inorganic fraction shows a
distinct isotopic signature in leachate, ground-
water and surface-water and thus δ13CDIC is
Author contribution
used as a tracer. Since, δ13CDIC value for rivers
shows a wide range thus the leachate plume can Anjali Bhagwat: Data curation, Formal analysis,
only be traced inside the subsurface environment. Investigation, Methodology, Writing – Original draft,
iii Both the isotopes of nitrogen δ15N-NH4 and Writing – Review & editing.
δ15N-NO3 fail to trace leachate plume in the Chandra Shekhar Prasad Ojha: Supervising,
shallow aquifers. However, nitrate isotope Review and editing.
(δ15N-NO3) is a good candidate for tracing the Sudhir Kumar: Supervising, Review and editing.
plume movement in the deeper aquifers. Bhisam Kumar: Supervising, Review and editing.
228 A. BHAGWAT ET AL.

Notes on contributors [8] Bhagwat A, Kumar R, Ojha CSP. Assessing efficiency and
economic viability in treating leachates emanating from
Ms Anjali Bhagwat, Scientist’C’, Groundwater Hydrology Div- the municipal landfill site at Gazipur, India. Environ Sci
ision of NIH Roorkee. Her research focuses on Groundwater Pollut Res. 2023;30. doi:10.1007/s11356-021-16724-y.
flow and contaminant Transport Modelling, Contaminant [9] El-Fadel M, Findikakis AN, Leckie JO. Modeling leachate
Hydrology, Isotope Hydrology Micro-plastic assessment & generation and transport in solid waste landfills. Environ
Hydrological Modelling. Technol. 1997;18(7):669–686. doi:10.1080/09593331808
Prof. Chandra Shekhar Prasad Ojha, Professor at Department 616586
of Civil Engineering, IIT Roorkee. He has more than 40 years [10] Sykes JF, Soyupak S, Farquhar GJ. Modeling of leachate
of experience. His field of Interest is Hydraulics, Hydrology organic migration and attenuation in groundwaters
and Environmental Engineering. He has More than 100 below sanitary landfills. Water Resour Res. 1982;18
research papers in international Journals. (1):135–145. doi:10.1029/WR018i001p00135
Dr Sudhir Kumar, Former Director and Scientist, NIH Roorkee. [11] Negi P, Mor S, Ravindra K. Impact of landfill leachate on
He is an expert Hydrogeologist and headed the Isotope Lab- the groundwater quality in three cities of North India
oratory at NIH Roorkee for more than 15 years. His main area and health risk assessment. Environ Dev Sustain.
of interest is Groundwater Flow modelling. 2020;22:1455–1474. doi:10.1007/s10668-018-0257-1
[12] Andrei F, Barbieri M, Sappa G. Application of 2H and 18O
Dr Bhishm Kumar, Former Prof Staff, IAEA, Vienna, Austria & isotopes for tracing municipal solid waste landfill con-
Advisor (IH), Former Sr Scientist & Head, NIH Roorkee, His tamination of groundwater: two Italian case histories.
expertise lies in the Application of Isotopes in Hydrology and Water (Basel). 2021;13:1065, doi:10.3390/w13081065
Water Resources. [13] Sappa G, Barbieri M, Andrei F. Isotope-based early-
warning model for monitoring groundwater–leachate
contamination phenomena: first quantitative assessments.
ORCID Water (Basel). 2023;15:2646, doi:10.3390/w15142646
[14] Srivastava SK, Mohiddin SK, Prakash D, et al. Impact of
Sudhir Kumar http://orcid.org/0000-0002-2206-0624 leachate percolation on groundwater quality near the
Bandhwari Landfill Site Gurugram, India. J Geol Soc
India. 2023;99:120–128. doi:10.1007/s12594-023-2274-4
[15] Joshi R, Ahmed S. Status and challenges of municipal solid
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