Hydrogeochemical and Isotopic Investigations On The Origins of Groundwater Salinization in Çarşamba Coastal Aquifer (North Turkey)

Environmental Earth Sciences (2022) 81:128
https://doi.org/10.1007/s12665-022-10248-5
ORIGINAL ARTICLE
Hydrogeochemical and isotopic investigations on the origins

of groundwater salinization in Çarşamba coastal aquifer (North
Turkey)
Abdourazakou Maman Hassan1 · Arzu Firat Ersoy1
Received: 31 March 2021 / Accepted: 25 January 2022

© The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature 2022
Abstract
The aim of this study is to determine the origins of salinization and the main hydrogeochemical process that controls the
chemistry of Çarşamba coastal aquifer in Turkey. Therefore, a total of 33 groundwater samples and three seawater samples
were analyzed in the coastal region of Çarşamba Plain in July 2019, and for these samples’ physical parameters, major ions
and environmental isotopes (δ18O, δ2H, and 3H) values were determined. Piper, Chadha, Gibbs diagrams and Stuyfzand
Classification Systems were used to determine the origins of salinization and the key hydrogeochemical process controlling
the groundwater chemistry. According to Stuyfzand classification system, the study showed that the freshwater and fresh-
brackish water main types are the most widespread in the study area. Six water subtypes were observed in the study area that
include CaHCO3, CaMix, NaMix, NaCl, NaHCO3, and MgHCO3. In addition, the subtypes CaMix indicated the locations
of the transition zone, where the groundwater rich in Ca and HCO3 and gradually enriched in Na changes from CaMix with
HCO3 as dominant anion to eventually CaCl and NaCl subtypes. Furthermore, the subtypes NaMix, N aHCO3, and M gHCO3
showed the locations of the transition zone where the flushing of the saline aquifer by freshwater takes place. All groundwa-
ter samples from study area had a positive cation exchange code, and show that four hydrogeochemical facies composed of
CaHCO3, Ca–Mg–Cl, NaCl, and N aHCO3. Besides, groundwater samples have been influenced by two main mechanisms:
the water–rock interaction and evaporation–crystallization. According to δ18O, δ2H, and 3H analysis, the water samples have
meteoric origin, shallow circulation, and a short residence time.
Keywords Hydrochemical process · Stuyfzand classification system · Seawater intrusion · Çarşamba coastal aquifer ·
Turkey
Introduction dissolution of halite, domestic, industrial, and agricultural

wastes. In the coastal area, seawater intrusion is the principal
Although many factors, such as excessive pumping of source of salinization of groundwater, and very often requires
groundwater, pollution, uncontrolled agricultural practices, the abandonment of wells in these zones (Al Farrah et al.
and industrialization, lead to the depletion of the world water 2011). Many research has been realized through the world
resources, salinization, especially in coastal aquifers, is the to determine the sources of salinization of groundwater. The
most important factors which pollutes groundwater resources. work carried out in Algeria by Djabri et al. (2008) and in
There are various potential sources of salinization of ground- Ghana by Kortatsi (2006) based on the physico-chemical
water, such as natural saline groundwater, seawater intrusion, analysis results of the water samples highlighted the influence
of seawater intrusion and the dissolution of evaporate for-
mations on the salinity of the coastal aquifers in their study
* Arzu Firat Ersoy area. In Syria, Abou Zakhem and Hafez (2007), using the
arzufirat@gmail.com results of physico-chemical and isotopic analysis of the water
Abdourazakou Maman Hassan samples taken from the north of Latakia and south of Tar-
abdourazakoum@gmail.com tous, demonstrated that salinization of groundwater in these
1
Department of Geological Engineering, Karadeniz Technical coastal areas is mainly due to the mixing between freshwater
University, 61080 Trabzon, Turkey and seawater; and that evaporation process has very limited
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128 Page 2 of 19 Environmental Earth Sciences (2022) 81:128
effects. In France, Veronique de Montety et al. (2008) carried to its position on the Black Sea coast, Çarşamba plain is a
out research to evaluate different salinity sources of the con- region where intense agricultural activities take place. It is
fined aquifer of the Rhône delta using chemical and isotopic assumed that the excessive pumping of groundwater in this
groundwater compositions. According to the results of their region for agricultural activities leads to contamination of the
study, seawater intrusion is the origin of increasing of Na, aquifer by the seawater intrusion. In addition, the excessive
thus promoting the process of exchange between Ca2+ and use of fertilizers, pesticides in agricultural areas as well as
Na+. In addition, this seawater intrusion also led to the reduc- industrial wastes from the industrial areas leads to pollution
O42− which is confirmed by the strongly depleted of
tion of S of groundwater in this region (Maman Hassan 2021). This
13
CTDİC values. study therefore made it possible to highlight the influence of
In Turkey, while the average annual rain precipitation in seawater intrusion caused by the agricultural and industrial
the world is around 1000 mm, the average precipitation is activities taking place in the study area on the groundwater
around 646 mm. This situation shows that Turkey in terms of chemistry in the Çarşamba aquifer.
water resources is not among the rich countries. In addition
to the scarcity and uneven distribution of water resources, General properties and geology
rapid population growth and pollution of water resources
conduct to a further worsening of the water deficit (Toklu The study area is located on the left bank of the Yeşilırmak
1999). On the other hand, unfavorable factors such as poor river and the western part of the Çarşamba plain, Turkey,
land use, urbanization and industrial organizations, wild lying between the latitudes 41° 11′ 30'' and 41° 16′ 30''
storage areas, and the discharge of untreated liquid waste and the longitudes 36° 22′ 00'' and 36° 36′ 00''; the plain
into basins cause rapid pollution of surface and groundwater. of Çarşamba is situated in the Middle of Black Sea Region
Among the sources of water pollution in most coastal areas of (Fig. 1). The climate of this region is semihumid and the
Turkey, the salinization process is one of the most worrying average annual precipitation is about 700 mm and the average
factors, which mainly threatens groundwater resources. In annual temperature is about 17 °C (Arslan 2014). The wet
general, in coastal areas, the groundwater level decreases due period is from October to the end of December. There are
to excessive pumping of groundwater. This excessive ground- three formation types in the study area, which are the Tertiary
water pumping lowers the level of the freshwater table and age Tekkeköy formation, Eocene age Sarıyurt formation, and
consequently reduces the pressure exerted by the freshwa- Quaternary age Alluvium formation (Fig. 2). The Sarıyurt
ter column, which then allows the denser saltwater to move formation consists of sandstones, siltstones, marls, and
inland lateral (Barlow 2003). Arslan et al (2012), Fırat Ersoy conglomerates. Its upper part is composed of interstratified
et al. (2020), and Fırat Ersoy et al. (2021) carried out research siltstones, sandstones, and marls, while an alternation with
to determine the influence of seawater on groundwater in sandstones is observed in the middle part. In the lower part of
the right bank of the Bafra Plain, using the results of hydro- this formation, conglomerates and sandstones are observed.
chemical and isotopic analysis. According to the results of The Tekkeköy formation consists of sandstones, mudstones,
their study, some wells have very high Electrical Conductiv- basalts, marls, and tuffites alternation and agglomerates. The
ity (EC), Total Dissolved Solids (TDS), Cl− and Na+ values, Quaternary Alluvium, which covers almost the entire study
and the isotope distributions of δ18O and δ2H showed that all area, consists of sands, gravels, clays, sandstones, muds, and
water samples were grouped around the freshwater–seawater silts (Yoldaş et al. 1985). The geology of the study area indi-
mixing line. The work carried out in Van by Özler (2001) and cates that only the Quaternary Alluvium can be considered
in Mersin by Demirel (2004) based on the results of physico- as important groundwater reservoirs. The volcanic rocks of
chemical analysis of groundwater samples taken in coastal the Çarşamba plain are geological formations which have
area highlighted the influence of seawater intrusion due to the characteristics of the secondary aquifer after the alluvial
excessive pumping of groundwater. According to the previ- deposits in terms of groundwater. In these formations, the
ous research that has been done in Çarşamba coastal aquifer, weathered basalts and in particular the interconnected cracks
excessive increases of chloride, sodium, EC, and TDS values and the fracture systems developed in the agglomerate lev-
were observed. Between 1990 and 2012, water quality in this els, facilitate transportation and accumulation of groundwater
zone was severely deteriorated due to the excessive pumping (DSI 1993). The geological cross-section of study area is
of groundwater and the resulting seawater intrusion (Arslan given in Fig. 3. In terms of hydrogeological characteristics,
2017). the Çarşamba plain can be divided into two parts: the left
This study seeks to determine the salinization origins and bank and the right bank of the Yeşilırmak River. The left
the main hydrogeochemical process controlling groundwater bank is generally composed of unconfined and semi-confined
chemistry of Çarşamba coastal aquifer based on the results aquifers, while on the right bank, semi-confined and confined
of physico-chemical and isotopic analyses (δ2H, δ18O and aquifers are the most frequent (DSI 1993). On the left bank of
3
H) of groundwater samples collected in this region. Due Yeşilırmak river where the study area is located, the aquifer
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Environmental Earth Sciences (2022) 81:128 Page 3 of 19 128
Fig. 1 Location map of the Çarşamba coastal aquifer (Samsun-NE Turkey)
begins generally at a depth varying between 4 and 40 m, and domestic use. Water sampling was taken according to the
its thickness values ranged from 1 and 20 m. The majority TS EN ISO 5667 Water Quality Sampling standard (ISO
of aquifers in the left bank of Yeşilırmak River consist of 1991) defined in Turkish Standards. According to this stand-
various layers of gravels, clayey-sands, clayey gravels, and ard, water sampling is done after 15 min of pumping in deep
silty sands within the Quaternary alluvium. The aquifer of wells. Water samples were taken into polyethylene bottles
Çarşamba plain has available discharge between 2 and 32 l/s, pre-washed with pure water. For each sampling point, 1 L
and a variable hydraulic gradient with a maximum value of bottle was used for the major ion analysis and the 100 ml bot-
0.0025 (DSI 1993; Arslan 2014). tles were used for the minor ion analysis. For the analyses of
δ18O, δ2H, and 3H, 1 L bottles were used. For these collected
samples, the physical parameters [TDS (Total Dissolved
Materials and methods Solid), DO (Dissolved Oxygen) pH and EC (Electrical Con-
ductivity)], major ions [Sulfate (SO42−), carbonate (CO3−),
For this purpose, 33 groundwater samples and three seawater chloride (Cl−), bicarbonate (HCO3), magnesium (Mg2+),
samples were taken in July 2019 in the study area. Ground- Sodium (Na+), potassium (K+), calcium (Ca2+)], ammonium
water samples were taken during the wet season from wells (NH4+), nitrite ( NO2−), nitrate ( NO3−) and environmental iso-
used in the study area for irrigation, industrial activities, and topes (Oxygen-18 (δ18O), and Deuterium (δ2H) and Tritium
13
Fig. 2 Geological map of Çarşamba coastal aquifer
(3H) values were determined. The global coordinates of all out at the Seventh Regional Directorate of Hydraulic works
the sampling points expressed in the sexagesimal system were of the State (DSI) in accordance with TS EN ISO standards.
taken and recorded with a Global Positioning System (GPS) The concentrations of H CO3− and C O3− were determined
device. The physical parameters of groundwater samples using titration method. Atomic absorption spectrometry TS
were determined in situ using HQD-Meter. The analysis and EN ISO 14911 method was used to determine the concen-
chemical parameters of groundwater samples were carried trations of Na+, Ca2+, K+, and Mg2+, while NH4+. NO2−,
13
precipitation, and evaporation. Thus, this diagram is con-

structed by plotting TDS on the Y-axis against Na/(Na + Ca)
on the X-axis for cations; and TDS on the Y-axis against Cl/
(Cl + HCO3) on the X-axis for anions (Gibbs 1970). Chadha
diagram is used in general for the classification of natural
waters as well as the identification of hydrochemical pro-
cess. This diagram is constructed by plotting on the X-axis
the difference between alkaline earths and alkali metals
[(Ca 2++Mg2+)–(Na++K+)] against weak acidic anions and
strong acidic anions [(HCO3− + CO32−)–(SO42− + Cl−)] on
the Y-axis, of water data expressed as milliequivalent per-
centage. The milliequivalent proportion differences from the
axis X and Y are prolonged further into the principal study
subfields of the proposed diagram, which defines the global
Fig. 3 The geological cross-section of the study area character of water (Chadha 1999). The δ 18O, δ 2H, and 3H
analyses were carried out to determine the origin, the relative
age of the groundwater, and whether the seawater intrusion
O3− SO42−, and Cl− analyses were carried out using ion
N into the aquifer is significant in the study area. The ground-
chromatography method. The environmental isotopes’ (δ18O, water origin and the mixing process between freshwater and
δ2H, and 3H) analyses were carried out at the Isotope Labo- seawater were determined using the relationship between δ2H
ratories of the Technical Research-Quality Control Directo- and δ 18O, Sinop Meteoric Water Line (D = 8* δ18O + 16.4)
rate of the State Hydraulic Works. The mass spectrometry (Dilaver et al. 2018) and Global Meteoric Water Line (δ
method was used to determine the value of δ2H and δ18O; and D = 8* δ18O + 10) (Craig 1961). In addition, to assess the
the values of 3H were determined using liquid scintillation seawater influence on groundwater, the cross plots of C l− vs
method. For the analysis of 18O and 2H, the precision values δ18O, EC vs δ18O, EC vs 3H, and Cl− vs 3H were used.
are ± 0.15 ‰ and ± 2 ‰, respectively. In this study, all maps The Stuyfzand classification system was developed by
were made using ArcGIS software. The spatial distribution Stuyfzand (1986) as a new system applied to aquifer sys-
maps were produced using inverse distance weighted (IDW) tems by combining the characteristics of existing classifica-
interpolation method. tion systems. This system had been improved for the first
time specifically for groundwater from coastal aquifers
Hydrochemical interpretation methods limestone systems with cation exchange phenomena caused
by the intrusion of fresh or salt water. After the system has
In this study, the determination of salinization origins and the been extended for non-calcareous aquifer systems (Stuyfzand
hydrochemical process controlling the groundwater chem- 1989). Consequently, this classification can be applied for
istry is mainly based on the classification of water types groundwater from all hydrogeological systems. This system,
according to Stuyfzand and Chadha diagram (Chadha 1999). based on the determination of different types of water by
In addition, Spearman correlation analysis method was used subdividing the principal chemical characteristics of ground-
to determine the relationships between the physico-chemical water at 4 levels, is important in determining the principle
parameters of groundwater samples. This correlation method of cation exchange in groundwater (Fırat Ersoy and Ersoy
was used in this study, because the physico-chemical param- 2009).
eters of groundwater samples collected in the study area did The first level of this classification of groundwater, which
not follow a normal distribution law. The Spearman correla- corresponds to the main type of water, is determined accord-
tion analysis method is usually used when the supposition ing to the chloride content. Therefore, depending on the chlo-
of the bivariate normal distribution is not tenable (Artusi ride concentration, there are six different main types; fresh
et al. 2002). The ratio of sodium to total sodium and chlo- (F), fresh-brackish (Fb), brackish (B), brackish-salt (Bs),
ride to total dissolved solids (TDS) was used to evaluate the hyperhaline (H), and salt (S) (Stuyfzand 1986; Fırat Ersoy
dominant ion process that occurring in groundwater of study and Ersoy 2009). The classification of water main according
area. Hydrochemical facies of water samples was classified to the Cl− is given in Table 1. The second level that represents
basis on the dominant ions using the Piper diagram (Piper the water type is determined according to the hardness val-
1944). The diagram of Gibbs was used for to determine the ues. The classification of water types according to the hard-
main mechanisms controlling the groundwater chemistry ness values is given in Table 1. The third level of this classifi-
in the study area. Groundwater chemistry is in general con- cation that corresponds to the subtype of water is determined
trolled by various mechanisms such as weathering of rocks, according to the dominant anions and cations. However, it
13
Table 1 Water type and main type classification according to Stuy- the symbol “–” often indicates the intrusion of salt water
fzand Classification System (Stuyfzand 1986) when (Mg + K + Na) corrected < − √ (0.5 Cl);
Water type the symbol “ + ” often indicates freshwater encroachment
when (Mg + K + Na) corrected > √(0.5Cl);
Type Cod Total hardness (F0)
the symbol “ϕ” often indicates an equilibrium when − √
Very soft x < 5 (0.5 Cl) ≤ (Mg + K + Na) corrected ≤ √ (0.5 Cl).
Soft 0 (5–10) The factor 1.061 of the previous formula corresponds to
Moderately hard 1 (10–20) the ratio {(Mg + K + Na)/Cl} for the average seawater. It is
Hard 2 20–40 also supposed that all chlorine ions come from the sea and
Very Hard 3 40–80 the fractionation of the main components of seawater dur-
Extremely hard 4 80–160 ing spraying can be neglected and that the Cl concentration
Extremely hard 5 160–320 behaves conservatively (Stuyfzand 1986). The water classi-
Extremely hard 6 320–640 fication according to Stuyfzand classification system is given
Extremely hard 7 640–1280 in Table 2.
Extremely hard 8 1280–2560
Extremely hard 9 > 2560
Water main type Results and discussion
Main type Cod Cl (mg/l)
Hydrochemical parameters of groundwater samples
Fresh F < 150
Fresh-Brackish Fb 150–300 The pH values of groundwater samples are between 6.5
Brakish B 300–1000 and 8, TDS value range is 2679.20–399.16 mg/L, EC
Brakish-Salt Bs 1000–10,000 range is 587–3940 µS/cm, and DO values are between
Salt S 10,000–20,000 1.37 and 8.07 mg/(Table 3). High values of EC and TDS
Hyperhaline H > 20,000 were observed in wells located towards the center, in the
northeast part, and locally in the west part of the study area,
while the lower values are observed in the northern part,
should be noted that in this classification, the cation or anion and towards the west and south part. C a2+, Mg2+, Na+, and
+
with most meq/l does not necessarily determine the name. K values are, respectively, between 52.91 and 167.2 mg/L,
The strongest hydrogeochemical family is first determined 16.65 and 114.21 mg/L, 20.01 and 609.04 mg/L, and 1.56
for both cations and anions, e.g., the families [Na + K + NH4] and 25.35 mg/L. The N H4+ value range is 0–4.39 mg/L
and [SO4 + NO3 + NO2]. The stronger member of the two with a median value of 0.92 mg/L (Table 3). Higher N a+
families is then chosen to form the combination. The theo- value was observed in well number 13 located, respectively,
retical maximum number of subtypes is 54. However, only in the center of the study area. Anion’s analysis results
16 subtypes have been discovered, namely those listed in show that the C l − value range is 18.08–1001.82 mg/L,
−
Table 2. The class of water is finally determined according to H CO 3 value range is 248.92–822.41 mg/L, and
the sum of Mg, K, and Na in meq/l, adjusted for contribution SO42− value range is 19.69–504.80 mg/L. The N O3− value
of sea salt according to the following formula: (K + Mg + Na) range is 0.25–101.68 mg/L with a median value of
−
corrected = (K + Mg + Na) measured–1.061*Cl ; where: 16.06 mg/L. The concentration of nitrate in groundwater
usually comes from the oxidation of ammonium (nitrifica-
tion) (Rajmohan et al 2009). In the presence of oxygen,
Table 2 Water classification according to Stuyfzand Classification System (Stuyfzand 1986)

Name Subdivisions Criteria Codes
Water main type 6 Cl Fb, F, Bs, B, H and S

Water type 11 Total hardness X, 0, 1, 2, 3, 4, 5, 6, 7, 8, 9
Water subtype 54 Most important cation and anion NaCl, NaMix, KNO3, CaCl, C aSO4, CaNO3, NaHCO3, CaHCO3,
CaMix, MgCl, MgMix, M gHCO3, AlSO4, NH4SO4, NaSO4,
FeSO4
Water class 3 (Mg+ K+ Na) corrected for sea salt –, + , ϕ
Where: Fb Fresh brackish, F Fresh, Bs Brackish saline, B Brackish, H Hyperhaline, S Saline
13
Table 3 Physico-chemical parameters, δ18O, δ2H, and 3H values of of the Çarşamba coastal aquifer. The high Cl− values were
groundwater samples observed towards the center, the western part, and locally
Parameters Min Max Median towards the northeast of the study area. It is observed that
in the study area, the high values of C l−, Na+, TDS, and
Ca2+ (mg/L) 52.91 186.77 115.38
EC have been observed in industrial and agricultural areas.
Mg2+ (mg/L) 16.65 114.21 37.52
These values indicate a seawater intrusion caused by an
Na+ (mg/L) 20.01 609.04 107.05
over-extraction of groundwater in these areas. The high
K+ (mg/L) 1.56 25.35 7.15
NH 4+ values observed in some wells are influenced by
NH4+ (mg/L) 0 4.39 0.92
industrial waste, the excessive use of fertilizers and pesti-
Cl− (mg/L) 18.08 1001.82 114.91
cides in the study area (Maman Hassan 2021). In Sultanate
HCO3− (mg/L) 248.92 822.41 471.26
of Oman, the work carried out by Rajmohan et al. (2009)
SO42− (mg/L) 19.69 504.8 132.11
showed that nitrogen fertilizers and farm manures, which
NO3− 0.25 101.68 16.06
are normally used for paddy and other crops, are the major
pH 6.55 8 7.22
ammonium sources in groundwater of agricultural areas.
TDS (mg/L) 399.16 2679.2 852.33
Piper classification diagram showed four different water
EC (µS/cm) 587 3940 1253.42
facies in the study area, which are C aHCO3, Ca–Mg–Cl,
DO (mg/L) 1.37 8.07 4.27
NaCl, and Ca-NaHCO3 (Fig. 4). The C aHCO3 water type,
δ18O (‰) − 8.89 − 7.21 − 8.39
which is dominant in the study area, represents around 73%
δ2H (‰) − 56.41 − 46.64 − 52.52
3
of analyzed samples. The abundance in the study area of this
H (TU) 0.96 7.15 4.68
water type that is characterized by the dominance of Ca and
HCO3 ions reveals a strong carbonate rock–water interac-
tion and strong recharge process. The Ca–Mg–Cl water type
NH4+ undergoes rapid oxidation to NO3−. It was noted that represents 18% of analyzed samples and were observed in
in general, contamination of groundwater with N O3− occurs 22, 19, 33, 5, 7, and 14 well number. The Ca-NaHCO3 water
when the input of NO3− in the soil exceeds the consumption types were observed in wells number 23 and 16, and rep-
by plants and denitrification (Mcclain et al. 1994; Abou resented around 6% of analyzed samples. NaCl water type
Zakhem and Hafez 2015). In the study area, 87% of water is only observed in 13 well number; the Ca-NaHCO3 water
samples have DO concentration greater than 2 mg/L. This types of results from the cation exchange between seawater
situation favors the oxidation of NH4+ to N
O3− in the study and fresh water during the freshening process. In addition,
area (Casciotti et al 2010; Abou Zakhem and Hafez 2015). the presence of Ca–Mg–Cl and NaCl water facies also indi-
However, it is important to clarify that DO concentration cates the seawater intrusion in the study area.
in groundwater and soils cannot be used to predict high The Piper diagram can also be used in determining of sea-
nitrate levels, since there may not be a source of nitrogen. water intrusion into groundwater using Kelly (2005) clas-
The nitrification process which leads to the oxidation of sification. Therefore, on this diagram, the fresh groundwater
ammonium to nitrate is given in the following equations samples will land near the area labeled “fresh water”, while
(Elisante and Muzuka 2016; Rajmohan et al. 2009): the water resulting from a conservative mixture (mixture
without ion exchange reactions) between freshwater and sea-
2NH+4 (aq) + O2 (aq) + 2OH− ⇒ 2NH2 OH (aq) + 2H2 O water would be drawn along the line labeled “mixed water”
(1) (Kelly 2005).
NH2 OH (aq) + 6 H2 O ⇒ NO−2 + 5H3 O + 4e− (2) According to this classification (Fig. 4), 75.76%, 21.21%,
and 3.03% of the groundwater samples fall in freshwater
NO−2 + (aq) + 3H2 O ⇒ NO3 + 2H3 O+ + e− . water area, mixed water area, and seawater intrusion area,
(3)
respectively. The water samples which fall in mixed and sea-
In the study area, high concentrations of NO 3− are water intrusion areas indicated the influence of seawater on
mainly due to discharges of industrial wastewater, urban groundwater in the study area.
domestic wastewater, and the use of nitrogen fertiliz- According to Chadha diagram, four water facies were
ers. The work carried out by Arslan et al. (2017) in the observed in the study area which are CaHCO3, Ca–Mg–Cl,
coastal plain of Çarşamba to assess the spatial and sea- NaCl, and N aHCO3 (Fig. 5). The C aHCO3 water type that
sonal changes in groundwater pollution by nitrates in the falls in field 5 of diagram is the most widespread in the
agricultural area showed that the leaching of nitrates to the study area and represents around 70% of analyzed samples.
groundwater due to excessive use of fertilizers could be the This dominant water type reveals as in the piper diagram
cause of the high concentrations of nitrates in groundwater that the weathering of host rocks and recharge process are
most important in the study area. The Ca–Mg–Cl water type,
13
Fig. 4 Groundwater types
according to Piper diagram
Fig. 5 Groundwater types
according to Chadha diagram
13
which falls in field 6 of diagram, represents around 12% of aquifer (Ghezelsofloo et al. 2021). According to Fig. 6, most
analyzed samples and were observed in wells number 22, 7, of water samples from study area fall in ion exchange area.
14, and 33. This water type indicates reverse ion exchange However, water samples from wells numbers 24, 14, and 13
process that corresponds to the beginning of the salinization fall in seawater or reverse softening area. Seawater intrusion
process in the study area. The Na–Cl water type, which falls into the aquifer is one of the most important factors which
in field 7 of diagram, represents around 9% of analyzed sam- cause the reverse ion exchange process and hence the salini-
ples and were observed in wells number 13, 31, and 28. This zation of the groundwater water (Ghezelsofloo et al. 2021;
water type indicates evaporation, mixing between freshwater, Papazotos et al. 2019).
and seawater. The C aNaHCO3 water type that falls in field Data plotted on Gibbs diagram show that in the study area,
8 of diagram represents around 9% of analyzed samples and groundwater are influenced by two main mechanisms that
were observed in wells number 1, 16, 14, and 23. This water include water–rock interaction and evaporation–crystalliza-
type shows the cation exchange reaction resulting from the tion (Fig. 7). The groundwater samples that fall in rock domi-
flushing of the saline aquifer by freshwater. nance field are the most widespread and represents around
The ratio of sodium to total sodium and chloride to 80% of analyzed samples. The rock–water interaction, which
total dissolved solids (TDS) can also be used for to evalu- is dominant, indicates that in the study area, local geological
ate the dominant ion process (ion exchange and reverse ion context and hydrogeological conditions significantly influ-
exchange) in the aquifer (Ghezelsofloo et al. 2021). Thus, ence the chemical composition of groundwater. The ground-
in this diagram, the ratio of sodium to total sodium and water samples that fall in evaporation–crystallization domi-
chloride is the main factor that determines the effects of ion nance field are the least dominant and represent around 20%
exchange in the aquifer (Fig. 6). The values of (Na/Na+ Cl) of analyzed samples. Gibbs diagram can be used to determine
less than 0.5 indicate that the ion exchange process is occur- the influence of seawater on the aquifer (Seenipandi et al.
ring in the aquifer, while those greater than 0.5 indicate that 2019). Water samples (20%) that fall in evaporation–crystal-
the reverse ion exchange is a dominant ionic process in the lization dominance field indicate predominantly evaporative
Fig. 6 (Na/Na + Cl) (meq/L) vs.

TDS (mg/L)
13
Fig. 7 Gibbs diagram
conditions leading to higher amounts of total dissolved solids by fossil seawater, probably trapped during sedimentation
and increased salinity values by increasing ionic concentra- in this area.
tions due to diffusion of saltwater through seepage movement The results of the Kolmogorov–Smirnov and Shap-
(Seenipandi et al. 2019; Chidambaram et al. 2009). Similar iro–Wilk test performed to test the normality of variables
results were observed in the work carried out by Umarani are presented in Table 4. According to Table 4, almost all
et al. (2019) where due to seawater mixture, most of water variables have no normal distribution. Thus, Spearman cor-
samples collected during the summer in coastal aquifers of relation method can be used to strength of the links between
Tamil Nadu fell into evaporative dominance field. In Malay- variables. Spearman correlation coefficient matrices for
sia, the work realized by Sefie et al. (2018) to assess the physical and hydrochemical parameters of groundwater
hydrogeochemistry and groundwater quality of lower Kelan- samples are presented in Table 5. According to this table,
tan basin shows that the water samples falling in the evapora- Cl− was highly correlated with Na+ (R = 0.816) and mod-
tion dominance zone of the Gibbs diagram were influenced erately correlated with K+ (R = 0.551), TDS (R = 0.522),
Table 4 Test of normality Tests of normality

results
Kolmogorov–Smirnova Shapiro–Wilk
Statistic df Sig Statistic df Sig
Ca 0.082 33 0.200* 0.978 33 0.711

Mg 0.178 33 0.010 0.777 33 0.000
Na 0.258 33 0.000 0.605 33 0.000
K 0.175 33 0.012 0.850 33 0.000
NH4 0.239 33 0.000 0.807 33 0.000
Cl 0.308 33 0.000 0.492 33 0.000
HCO3 0.170 33 0.017 0.923 33 0.022
SO4 0.205 33 0.001 0.750 33 0.000
NO3 0.246 33 0.000 0.732 33 0.000
pH 0.080 33 0.200* 0.983 33 0.881
TDS 0.239 33 0.000 0.713 33 0.000
EC 0.239 33 0.000 0.713 33 0.000
a
Lilliefors significance correction
*
This is a lower bound of the true significance
13
and EC (R = 0.552). Moderate correlation was observed extremely hard water types were only observed in one well
between Na+ and K + (R = 0.588), NH4+ and EC (R = 0.601), located towards the center of study area.
Mg and HCO3− (R = 0.615), Na+ and EC (R = 0.520),
2+
The determination of the third level of this classifica-
HCO3− and EC (R = 0.640), and Mg2+ and EC (R = 0.642). tion which corresponds to the water subtypes determined
Moderate negative correlations were observed between N H4+ according to the dominant anions and cations shows that
− −
and NO3 (R = − 0.513), HCO3 and pH (R = − 0.659), the water samples are distributed according to six types of
between HCO3− and NO3− (R =− 0.548), and Ca2+ and pH facies: the C
aHCO3 facies, which represents around 60.60%
(R = − 0.627). The moderate positive correlation observed of samples, the CaMix facies which represents around
between Cl− and EC, and the strong positive correlation 18.19% of the samples, the NaMix facies which represents
observed between C l− and N
a+ indicate that these ions come around 6.06% of the samples, the NaCl facies which rep-
from the common source which is seawater intrusion (Sae- resents 3.03% of samples, the CaNaHCO3 facies, which
Ju et al. 2020; El Moujabber et al. 2006). In the coastal area, represents 9.09% of samples, and, finally, the M gHCO3
the concentrations of Cl− and EC values are used as clas- facies which represents 3.03% of samples (Fig. 11). The
sic indicators of salinization of groundwater (El Moujabber facies of water samples determined according to Stuyfzand
et al. 2006). The bivariate diagram of C l−/HCO3− ratio and classification system is given in Table 6.
−
Cl is generally used to determine the mixing of ground- The spatial distribution the water subtypes shows that
water and seawater (Seddique et al. 2019). According to the subtypes C aHCO3 are widely distributed in the study
this diagram, in the study area, most of water samples that area, the subtypes CaMix are found in the west and the
have lower Cl−/HCO3− ratios can be characterized as fresh center, the subtypes NaHCO3 are found in the center and
waters (Fig. 8). However, some water samples present high extreme northwest, the subtypes NaMix occupy locally
Cl−/HCO3− ration and high Cl values. These samples indi- the north and the east, the subtypes NaCl are found in the
cate so the mixing between groundwater and seawater in the center, and finally, the subtypes MgHCO3 are found in the
study area. extreme east part of study area (Fig. 12).
The last level of this classification, which corresponds
Stuyfzand classification system to the water class, was determined according to the sum of
K+, Na+, and Mg2+ in meq/l, adjusted for the contribution
The spatial distribution of the first level of water classifica- of sea salt, shows that all groundwater samples have posi-
tion according to Stuyfzand, which corresponds to the main tive cation exchange code.
type of water determined according to the chloride content, The subtype CaMix, which occupies the west, and the
shows that the study area can be divided into three regions: center of the study area shows the transition zone location,
the fresh, fresh-brackish, and brackish-salt water regions where the groundwater rich in Ca and HCO3 and gradu-
(Fig. 9). The freshwater, which represents 84.84% of the ally enriched in Na, changes from CaMix with HCO3 as
samples, occupies a very large portion of the study area. The dominant anion, to eventually CaCl and NaCl facies. This
fresh-brackish water represents around 9% of groundwater process corresponds to the beginning of the salinization
samples, and occupies in the south, the center, north, and process in this area. In the coastal areas, cation exchange
northeast of the study area. This dominance of F and Fb can reaction is the mainly process which controls hydrochemi-
be explained by the significant recharge of the aquifer and the cal composition of groundwater affected by seawater inter-
abundant infiltration of surface water, which contributes to ference. This subtype CaMix was observed in wells number
the refreshing of aquifer and limits the mixing between salt 2, 5, 7, 14, 22, and 33. The subtype NaCl observed in well
and fresh water at least in the study area. The Bs water main number 13 also indicates the seawater intrusion in aquifer.
type was only observed in one well located towards the center Freshwater is in general considered as an infiltrating rain,
of the study area. which has dissolved calcite, and the water type in this situ-
The spatial distribution of the second level of water ation is F-CaHCO3ϕ, while the seawater type is S-NaClϕ
classification, which corresponds to the type of water, (Al Farrah et al. 2011). Therefore, in the study area, the
determined according to the total hardness values, shows salinization process is mainly caused by seawater intru-
that the study area can be divided into three regions: hard, sion which reduces the quality of groundwater. In addition,
very hard, and extremely hard water regions (Fig. 10). The the excessive use of fertilizers, pesticides in agricultural
groundwater samples’ hardness values are varying between areas, as well as industrial waste from the industrial area
21 and 85.55 °F with an average of 44.22 °F. The very leads to pollution of groundwater in this region. During the
hard water region is the most widespread in the study area salinization process, a cation exchange reaction takes place,
and represents around 67% of analyzed samples. The hard a+, Mg2+, and K
resulting in a deficit of N + and an excess of
2+
water region occupies locally the northeast, the Northwest, Ca according to the following chemical reaction:
and a small part of the center and south of study area. The
13
Table 5 Spearman correlation matrix
128
Correlations
13
Ca Mg Na K NH4 Cl HCO3 SO4 NO3 pH TDS EC
a a a b
Spearman’s rho Ca Correlation coefficient 1000 0.414 − 0.173 − 0.187 0.022 0.073 0.380 0.379 − 0.116 − 0.627 0.300 0.300
Sig. (2-tailed) 0.016 0.336 0.298 0.904 0.686 0.029 0.030 0.522 0.000 0.090 0.090
Page 12 of 19
N 33 33 33 33 33 33 33 33 33 33 33 33
Mg Correlation coefficient 0.414a 1000 0.397a 0.282 0.237 0.496b 0.615b 0.454b − 0.213 − 0.403a 0.642b 0.642b
Sig. (2-tailed) 0.016 0.022 0.112 0.185 0.003 0.000 0.008 0.235 0.020 0.000 0.000
N 33 33 33 33 33 33 33 33 33 33 33 33
Na Correlation coefficient − 0.173 0.397a 1000 0.588b 0.475b 0.816b 0.142 0.429a − 0.296 0.258 0.520b 0.520b
Sig. (2-tailed) 0.336 0.022 0.000 0.005 0.000 0.431 0.013 0.095 0.148 0.002 0.002
N 33 33 33 33 33 33 33 33 33 33 33 33
K Correlation coefficient − 0.187 0.282 0.588b 1000 0.401a 0.551b 0.018 0.180 − 0.223 0.247 0.390a 0.390a
Sig. (2-tailed) 0.298 0.112 0.000 0.021 0.001 0.920 0.316 0.212 0.167 0.025 0.025
N 33 33 33 33 33 33 33 33 33 33 33 33
NH4 Correlation coefficient 0.022 0.237 0.475b 0.401a 1000 0.396a 0.485b 0.058 − 0.513b − 0.112 0.601b 0.601b
Sig. (2-tailed) 0.904 0.185 0.005 0.021 0.023 0.004 0.747 0.002 0.533 0.000 0.000
N 33 33 33 33 33 33 33 33 33 33 33 33
Cl Correlation coefficient 0.073 0.496b 0.816b 0.551b 0.396a 1000 0.147 0.467b − 0.380a 0.101 0.522b 0.522b
Sig. (2-tailed) 0.686 0.003 0.000 0.001 0.023 0.414 0.006 0.029 0.575 0.002 0.002
N 33 33 33 33 33 33 33 33 33 33 33 33
HCO3 Correlation coefficient 0.380a 0.615b 0.142 0.018 0.485b 0.147 1000 − 0.040 − 0.548b − 0.659b 0.640b 0.640b
Sig. (2-tailed) 0.029 0.000 0.431 0.920 0.004 0.414 0.826 0.001 0.000 0.000 0.000
N 33 33 33 33 33 33 33 33 33 33 33 33
SO4 Correlation coefficient 0.379a 0.454b 0.429a 0.180 0.058 0.467b − 0.040 1000 0.122 0.132 0.304 0.304
Sig. (2-tailed) 0.030 0.008 0.013 0.316 0.747 0.006 0.826 0.498 0.464 0.085 0.085
N 33 33 33 33 33 33 33 33 33 33 33 33
NO3 Correlation coefficient − 0.116 − 0.213 − 0.296 − 0.223 − 0.513b − 0.380a − 0.548b 0.122 1000 0.159 − 0.355a − 0.355a
Sig. (2-tailed) 0.522 0.235 0.095 0.212 0.002 0.029 0.001 0.498 0.378 0.043 0.043
N 33 33 33 33 33 33 33 33 33 33 33 33
pH Correlation coefficient − 0.627b − 0.403a 0.258 0.247 − 0.112 0.101 − 0.659b 0.132 0.159 1000 − 0.415a − 0.415a
Sig. (2-tailed) 0.000 0.020 0.148 0.167 0.533 0.575 0.000 0.464 0.378 0.016 0.016
N 33 33 33 33 33 33 33 33 33 33 33 33
Environmental Earth Sciences
TDS Correlation coefficient 0.300 0.642b 0.520b 0.390a 0.601b 0.522b 0.640b 0.304 − 0.355a − 0.415a 1000 1000b
Sig. (2-tailed) 0.090 0.000 0.002 0.025 0.000 0.002 0.000 0.085 0.043 0.016
N 33 33 33 33 33 33 33 33 33 33 33 33
EC Correlation coefficient 0.300 0.642b 0.520b 0.390a 0.601b 0.522b 0.640b 0.304 − 0.355a − 0.415a 1000b 1000
Sig. (2-tailed) 0.090 0.000 0.002 0.025 0.000 0.002 0.000 0.085 0.043 0.016
N 33 33 33 33 33 33 33 33 33 33 33 33
(2022) 81:128
a
Correlation is significant at the 0.05 level (2-tailed)
b
Correlation is significant at the 0.01 level (2-tailed)
Fig. 8 Relationship between Cl
and Cl/HCO3
Fig. 9 Distribution of water main type
[aCa] − X + bNa+ + cK+ + dMg2+ Ca2+ ions, causing the move of water resulting from NaCl
water type to the CaCl water type, which is characteristic of
⇒ aCa2+ + bNa, cK, dMg − X + aCa2+ .
[ ]
salinization process. This process is generally at the origin
During this cation exchange reaction, there is an adsorp- of formation of the (Na + K + Mg) deficit in groundwater. The
tion of dominant Na+, K+ and Mg2+ ions and a release of process of salinization in groundwater can be represented
as follows:
13
Fig. 10 Distribution of water type
Fig. 11 Water subtypes accord-

ing to Stuyfzand classification
system
Table 6 Types of water Well number Types of water Well number Types of water Well number Types of water
according to Stuyfzand
classification system 1 F2-NaHCO3+ 12 F2-CaHCO3+ 23 F2-NaHCO3+
2 F3-CaMix+ 13 Bs4-NaCl+ 24 F3-CaHCO3+
3 F2-CaHCO3+ 14 Fb3-CaMix+ 25 F3-CaHCO3+
4 F2-CaHCO3+ 15 F2-CaHCO3+ 26 F3-MgHCO3+
5 F3-CaMix+ 16 F2-NaHCO3+ 27 F3-CaHCO3+
6 F3-CaHCO3+ 17 F3-CaHCO3+ 28 Bs3-NaMix+
7 F3-CaMix+ 18 F3-CaHCO3+ 29 F2-CaHCO3+
8 F3-CaHCO3+ 19 F2-CaHCO3+ 30 F2-CaHCO3+
9 F3-CaHCO3+ 20 F3-CaHCO3+ 31 Fb3-NaMix+
10 F3-CaHCO3+ 21 F3-CaHCO3+ 32 F3-CaHCO3+
11 F3-CaHCO3+ 22 Fb3-CaMix+ 33 F3-CaMix+
13
Fig. 12 Distribution of water subtypes and classes
CaHCO3 𝜙 ⇒ CaCl− ⇒ NaCl− ⇒ NaCl𝜙 F ⇒ Fb ⇒ B ⇒ Bs ⇒ S. during the freshening process can also be schematized as
follows (Stuyfzand 1986; Fırat and Ersoy 2009):
It is observed that the classes of samples number 2, 5, 7, NaClϕ ⇒ NaCl + ⇒ N aHCO 3 + ⇒ M gHCO 3 + ⇒
14, 22, and 33 affected by seawater intrusion present falsely CaHCO3 + ⇒ CaHCO3ϕ
positive cation exchange code. This false-positive cation S ⇒ Bs ⇒ B⇒ Fb ⇒ F.
exchange code is not due to cation exchange but due to Mg2+ It is observed also that the groundwater samples affected
ions which dissolved from the carbonate rocks in the study by freshening process in study area present a positive cation
area. exchange code which is due essentially to cation exchange
The subtypes NaMix, NaHCO3, and MgHCO3 observed between fresh water and salt water.
in the study area indicate the locations of the transition The high Na+ values observed in some samples could
zone where the flushing of the saline aquifer by freshwater also come from ion exchange between the clay particles
takes place. This process is observed when freshwater from and groundwater. This exchange takes place between the
coastal aquifers infiltrates into salt water, thus causing the Na+ ions of the clay particles and the Mg2+ and Ca2+ ions
following chemical reaction: of the groundwater. These ion exchanges therefore lead to
an increase in N a+ ions and a decrease in C a2+ and M
g2+
aCa2+ + bNa, cK, dMg − X + aCa2+
[ ]
ions in groundwater (Şahinci 1991).
⇒ [aCa] − X + bNa+ + cK+ + dMg2+ .
Isotopic signatures
During this cation exchange reaction resulting from
the flushing of the saline aquifer by freshwater, there is an In hydrogeological studies, the analysis of natural variations
adsorption of C a2+ ions and a release of N a+, Mg2+, and in the content of heavy isotopes of oxygen (18O) and hydro-
+
K ions, causing the formation of N aHCO3 which is typi- gen (2H) present in the structure of water is one of the meth-
cal for freshening. The freshening process is generally at ods used in the study of the origin and dynamics of ground-
the origin of formation of the (Na+ + K+ + Mg2+) surplus in water and surface water. Due to the differences in the heavy
groundwater. It is accepted that initial seawater conditions isotope content generally observed between groundwater
(SNaClϕ) dominated in the beginning of the process. Origi- and seawater, the isotope content of groundwater mixed with
nal seawater diluted gradually due to the recharge phenom- seawater can be easily separated from the isotope content
ena, and then, sea water conditions coming from S ended of meteoric water. In the study area, δ18O and δ2H content
up F (Stuyfzand 1986). The cation exchanges that occur in groundwater ranged from − 8.89 to − 7.21‰ and from
13
Fig. 13 Relationship between
δ18O and δ2H
− 56.41 to − 46.64‰, respectively. In the study area, ground- Meteoric Water Line (δ D = 8* δ18O + 10) (Craig 1961). The
water origin was determined using Sinop Meteoric Water relationship between δ2H and δ 18O allows to understand the
Line (D = 8* δ18O + 16.4) (Dilaver et al. 2018) and Global mixing process between freshwater and seawater (Nair et al
Fig. 14 Cl− (meq/l) vs. δ18O (‰) plot (a) and EC (µS / cm) vs. δ18O (‰) of groundwater samples in the study area
13
Fig. 15 Cl− (meq/l) vs. 3H plot (a) and EC (µS/cm) vs. 3H
2015). Figure 13 shows the relationship between stable iso- l− observed in these wells indicate the influence of seawater
C
topes δ2H and δ18O of groundwater and seawater. According intrusion into groundwater.
to the isotope distributions of δ18O and δ2H, all groundwa- Because tritium element is a radioactive isotope that
ter samples have meteoric origins (Fig. 13). However, it is degrades over time, it is present in low value in water with
observed that the water samples taken from wells number 13, long residence time and high value in water with a short
14, 16, 19, and 26 have more positive δ 18O and δ 2H values residence time. Due to this situation, the concentration of
than the other samples. More positive values of δ18O and δ2H tritium in young water is higher than in olds water. In the
indicate interference between seawater and groundwater in study area, groundwater values for 3H ranged from 0.96 TU
the study area. to 7.15 Tu. In this study to assess the seawater influence
To determine the level of seawater intrusion into ground- on groundwater, the cross plots of EC vs 3H and Cl− vs
3
water, important information can be obtained by examining H were also used (Fig. 15). According to Fig. 15, the
the relationships between isotope analysis results and phys- groundwater samples from wells number 15, 14, and 32
ico-chemical analysis results. There are close relationships have lower tritium content (< 3 TU) than the water samples
between the values of 18O, Cl−, SO42−, and EC of ground- from other wells. Therefore, these wells were recharged
water. In general, seawater intrusion in aquifer results in by groundwater having a longer transit time than that of
an increase in the δ18O, Cl−, SO42−, and EC values of the groundwater which recharged the other wells. In addition,
groundwater. Relatively high values of δ18O (0 ‰) as well as although the water samples from wells 15 and 32 have low
high concentrations of Cl and TDS indicate seawater origins, tritium values, its EC (< 1500 µS/cm) and Cl− (< 4 meq / l)
while low values of δ18O and low content of Cl and of TDS values are also low. This situation indicates that these wells
are characteristics of fresh groundwater origin (Wang and are not affected by seawater intrusion. High values of EC
Jiao 2012). In this study to assess the seawater influence on (> 1500 µS/cm) and Cl− (> 6 meq/l) were observed in wells
groundwater, the cross plots of Cl− vs δ18O and EC vs δ18O 13, 28, and 22 due to seawater intrusion. The majority of
were used. According to the Fig. 14, more positive δ18O val- the groundwater samples collected from study area have
ues are observed in samples with higher Cl− and EC values. tritium values greater than 4 TU. In addition, it is found
Well number 13 with the highest values of C l− and EC also that most of these wells have EC values less than 1500 µS/
has the highest value of δ O. In addition, high Cl− and EC
18
cm and C l− values lower than 6 meq/l. The high values of
values and more positive δ18O values are observed in well 3
H indicate that these wells were recharged by water from
numbers 14, 28, and 22. The high values of δ18O, EC, and recent precipitation.
13
Conclusion Declarations
This study seeks to determine the hydrochemical properties Conflict of interest The authors have not disclosed any competing in-
terests.
of the groundwater of Çarşamba coastal aquifer; one of the
most important coastal aquifers in Turkey. According to the
first level of Stuyfzand groundwater classification, the most
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Environmental Earth Sciences (2022) 81:128