Environmental Earth Sciences (2018) 77:397

https://doi.org/10.1007/s12665-018-7561-9

ORIGINAL ARTICLE

Hydrogeochemistry and groundwater quality assessment

of the multilayered aquifer in Lower Kelantan Basin, Kelantan,
Malaysia
Anuar Sefie1,2 · Ahmad Zaharin Aris2 · Mohammad Firuz Ramli2 · Tahoora Sheikhy Narany2 ·
Mohd Khairul Nizar Shamsuddin1 · Syaiful Bahren Saadudin1 · Munirah Abdul Zali3

Received: 23 December 2016 / Accepted: 14 May 2018 / Published online: 23 May 2018
© Springer-Verlag GmbH Germany, part of Springer Nature 2018

Abstract
Continual expansion of population density, urbanization, agriculture, and industry in most parts of the world has increased
the generation of pollution, which contributes to the deterioration of surface water quality. This causes the dependence on
groundwater sources for their daily needs to accumulate day by day, which raises concerns about their quality and hydrogeo-
chemistry. This study was carried out to increase understanding of the geological setup and assess the groundwater hydro-
geochemical characteristics of the multilayered aquifers in Lower Kelantan Basin. Based on lithological data correlation
of exploration wells, the study area can be divided into three main aquifers: shallow, intermediate and deep aquifers. From
these three aquifers, 101 groundwater samples were collected and analyzed for various parameters. The results showed that
pH values in the shallow, intermediate and deep aquifers were generally acidic to slightly alkaline. The sequences of major
cations and anions were N ­ a+ > C­ a2+ > M ­ + and ­HCO3− > C
­ g2+ > K ­ O42− > C
­ l− > S ­ O32−, respectively. In the intermediate
aquifer, the influence of ancient seawater was the primary factor that contributed to the elevated values of electrical con-
ductivity (EC), ­Cl− and total dissolved solids (TDS). The main facies in the shallow aquifer were Ca–HCO3 and Na–HCO3
water types. The water types were dominated by Na–Cl and Na–HCO3 in the intermediate aquifer and by Na–HCO3 in the
deep aquifer. The Gibbs diagram reveals that the majority of groundwater samples belonged to the deep aquifer and fell in
the rock dominance zone. Shallow aquifer samples mostly fell in the rainfall zone, suggesting that this aquifer is affected
by anthropogenic activities. In contrast, the results suggest that the deep aquifer is heavily influenced by natural processes.

Keywords Hydrogeochemistry · Multilayered aquifer · Sequences of major ions · Hydrochemical facies · Seawater remnant

Introduction and ensure food security (UNESCO 2012). Availability and

Groundwater plays a significant role in providing water sup-
ply for drinking, crop irrigation, industry, and construction,
with an estimated 2.5 billion people relying on it globally
(Connor 2015). It also serves to maintain the ecosystem
* Ahmad Zaharin Aris
zaharin@upm.edu.my
1
Hydrogeology Research Centre, National Hydraulic
Research Institute of Malaysia, 43300 Seri Kembangan,
Selangor, Malaysia
2 (Rao et al. 2012), adsorption–desorption (Isa et al. 2012),
Department of Environmental Sciences, Faculty
of Environmental Studies, Universiti Putra Malaysia,
43400 UPM Serdang, Selangor, Malaysia
3
Environment Section, Department of Chemistry,
46661 Petaling Jaya, Selangor, Malaysia
quality concerns pose a challenge to groundwater manage-
ment, as groundwater acts as a complement to surface water
resources (Van der Gun 2012). In recent years, the issue
of groundwater quality degradation has been gaining atten-
tion worldwide, owing to development of agricultural lands
and massive urbanization and industrialization. Currently,
groundwater quality assessment is increasing as the levels of
societal development and understanding of the importance
of groundwater resources for daily life grow. It has been
discovered that various natural processes, such as dissolu-
tion–precipitation (Amiri et al. 2015), oxidation–reduction
and physical processes including evaporation, mixing, and
dispersion (Polemio et al. 2006), as well as anthropogenic
activities, determine the groundwater chemistry (Giridharan
et al. 2008).

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397 Page 2 of 15 Environmental Earth Sciences (2018) 77:397

Owing to high permeability and hydraulic conductivity The aim of this study was to understand the geological
values of unconsolidated materials, many coastal aquifers setup and to assess the groundwater hydrogeochemical char-
are highly vulnerable to anthropogenic activities, such as acteristics of Lower Kelantan Basin using classic integrated
agricultural activities and unregulated groundwater abstrac- hydrogeochemical methods, which can lead to better under-
tion (Chidambaram et al. 2009). This has led to serious threat standing of the hydrochemical system in the study area, and
to groundwater quality, particularly via seawater intrusion, to utilization and management of groundwater resources that
water–rock interaction, weathering of silicate, dissolution of is more effective.
carbonate, and inflow of contamination from anthropogenic
sources in the study area (Sheikhy Narany et al. 2014). Sev-
eral studies have indicated the roles of the oversaturation Materials and methods
of groundwater, high permeability, rapid urbanization, and
agricultural activities in coastal areas to the deterioration of Study area
groundwater quality (Park et al. 2005; Ferguson and Glee-
son 2012; Idris et al. 2016). A recent study by Narany et al. Lower Kelantan Basin is located in the northeastern part
(2017) has shown the impact of intensive human activities of Kelantan State, Peninsular Malaysia. The study area
and deforestation in Lower Kelantan Basin, in the form of comprises the Kota Bharu, Bachok, Pasir Mas, and Tumpat
increasing nitrate contamination in the shallow aquifer over districts; lies between the latitudes of 5°53′N–6°14′N and
25 years, from 1989 to 2014. longitudes of 102°7′E–102°28′E; and covers about 880 km2.
Thus, systematic and continuous monitoring of ground- The area is bordered by the South China Sea to the east and
water quality is very important, particularly where high-den- the Golok River Basin to the west. The Quaternary deposits
sity populations are situated over coastal aquifers, owing to of coastal aquifers are quite complex because of the deposi-
the high vulnerability to saltwater intrusion, human activi- tional environment and composition of the aquifer (Ahamed
ties, and impacts on climate change of these areas (Keesari et al. 2015). The study area is a low elevation coastal plain,
et al. 2016). Lower Kelantan Basin is the biggest ground- which is characterized by surface elevations that vary from
water abstraction area and one of the largest agriculturally a few to 150 m (Bosch 1986). The entire population in the
active region in Malaysia (MWA 2011). Approximately 75% study area totaled up to 624,000 people (DOS 2010).
of the Lower Kelantan Basin population relies on ground- The study area is mainly drained by four major rivers,
water to meet their daily needs. In 2012, about 160 million namely, Kelantan, Pengkalan Datu, Kemasin and Semerak
liters per day (MLD), or 40% of the total state water usage Rivers. The Kelantan River is about 350 km long and has a
came from groundwater sources. Groundwater consumption basin that covers about 85% of the area of Kelantan State.
has increased significantly over the years and is expected All the river systems flow northwest before discharging
to continuously increase by 2.5% a year (Wan Mohd Zamri into the South China Sea. The study area comprises differ-
et al. 2012), owing to the high demand for domestic and ent types of land use: urban, industrial, rural, and intensive
industrial water supplies. However, the situation is becom- agriculture area, with sampling well screen depths rang-
ing more critical as groundwater resources are the sole water ing from about 3.0 to 127.5 m. The land use is predomi-
source for treated and untreated water. This is due to limited nantly agricultural, representing 35.9%, followed by cleared
surface water sources, many of which are exposed to severe land, built-up area, peat swamp, and forest (Table 1). The
sedimentation and high turbidity, such as rivers damaged
by logging and sand mining activities in the upstream area
(Ahmad et al. 2009). Table 1  The percentage of various land use type. Source Modified
A thorough understanding of the hydrochemical process from Ministry of Agriculture (MOA 2010)
is very important for the protection of groundwater resources Land use type Area ­(km2) Percentage (%)
and their effectiveness. It is also crucial for sustainable
Paddy 315.90 35.90
groundwater management (Tizro and Voudouris 2008). A
Mixed agricultural 249.09 28.31
study by Samsudin et al. (2008) combined hydrogeochemi-
Other crops (fruit) 75.73 8.61
cal analysis and a geophysical survey to delineate the salin-
Rubber 53.48 6.08
ity of groundwater aquifers along the coastal area of north
Coconut 47.49 5.40
Kelantan. The results indicated that the fresh water and
Cleared land 46.88 5.33
saltwater interface in the intermediate aquifer was located
Built-up area 43.57 4.95
as far as 8 km from the coast. The sulfate concentration of
Peat swamp 41.47 4.71
the second aquifer was relatively low compared to those of
Forest 6.34 0.72
the current seawater composition, which suggests that the
Total 879.95 100.00
brackish water is probably from ancient seawater.

13
Environmental Earth Sciences (2018) 77:397
dominant agricultural land uses are paddy cultivation, other
crops (fruits), rubber, coconut, and mixed agriculture such
as tobacco and vegetables.
The study area is in the equatorial region, and has a hot
and tropical climate with a mean temperature of 27 °C. The
average annual evapotranspiration rate is about 1510 mm.
The rainfall is prominently characterized by the northeast
monsoon, which starts in October and usually lasts until
March and brings heavy rain and strong wind to the coastal
area. The average rainfall during the northeast monsoon
is approximately 900 mm, accounting for 34% of the total
annual rainfall. The driest months occur from February to
April, and the average annual rainfall for 1989–2012 was
about 2,646 mm/year (MMD 2012).
Geological and hydrogeological settings
Lower Kelantan Basin consists of quaternary alluvium of
marine and fluviatile origins, which are not always possible
to differentiate (MacDonald 1967). The quaternary alluvium
is formed of various layers of sand and gravel, which make
up the productive aquifers (Ang and Mohamad 1996). The
clay layer on the top can be up to 8 m thickness and disap-
pears towards the coastal area. The alluvium is overlying
intrusive bedrock in the northern part of the study area.
Meanwhile, sedimentary or metasedimentary bedrock gener-
ally occurs in the southern and western regions, and consists
mainly of shale, sandstone, phyllite and slate (Bachik 1989).
Noor (1980) concluded that Kelantan River Basin is an
extensive plain with highly transmissive but anisotropic
aquifers, which are largely unconfined and highly variable
horizontally and vertically because of depositional pro-
cesses. The permeability ranges from 28 to 337 m/day, with
an average specific yield of 0.06. The river discharge has
diluted the salinity effect of the groundwater in the lower
reaches of the Kelantan River. The environmental isotope
data collected from wells showed high tritium values in the
shallow aquifer, suggesting that the groundwater contains
very recent water derived from local recharge (Mohamad
1983). Meanwhile, low tritium values observed in the inter-
mediate and deep aquifers suggested that the groundwater
comprises old water components and can be considered a
single system, as shown by the similarity of the environ-
mental isotopic data. However, these aquifers seemed to
be recharged through normal down-gradient water move-
ment originating from the shallow aquifer. Because none
of the three sub-systems (shallow, intermediate, and deep
aquifers) varies significantly during the dry and wet periods,
they retain low, stable isotopic levels and remain regionally
interconnected; therefore, they represent a single system.
The general groundwater level of shallow aquifer and its
flow are in the northeast direction (Fig. 1).
Page 3 of 15 397
Geological setup, groundwater sampling
and analytical procedures
Geological data from 37 exploration wells were utilized to
construct a geological cross-section and geological model.
The model helps in understanding the subsurface condi-
tions of the study area (Fig. 2). Exploration well data were
mainly obtained from the Minerals and Geoscience Depart-
ment (MGD), the Public Works Department (PWD), con-
tractors, and consultants’ reports. Samples obtained from
the exploration wells during the drilling works were geo-
logically logged, while formation samples were taken for
grain size analysis. Geophysical gamma-ray logging data
were used to produce a more accurate delineation of the
lithological boundary (Bachik 1989). The lithology data of
the exploration wells were correlated to those of other wells
that had similar lithological characteristics to interpolate the
subsurface structure for the geological model. These data are
important for segregating the groundwater aquifer types and
assisting in the hydrogeochemical interpretation.
The groundwater sampling for primary data was carried
out from 2009 to 2014. On the other hand, the secondary
data of groundwater quality during the period 1989–2012
were obtained from the MGD. After the conceptual hydro-
geological layer was defined and built, groundwater sam-
pling wells were categorized based on the screen depth, i.e.,
whether it was located in a shallow, intermediate or deep
aquifer. In this study, groundwater samples from 101 sam-
pling wells were collected and analyzed for various param-
eters (Fig. 3).
The primary groundwater samples were collected after
pumping for 15–20 min or at least three times the well’s
volume using a portable pump (Sundaram et al. 2009). The
in situ measurements were made immediately using a port-
able multiparameter instrument (YSI 556, USA). The sensor
for each parameter was calibrated using standard solutions.
Among the in situ parameters measured were pH, electrical
conductivity (EC), and total dissolved solids (TDS). The
samples were collected into two 250-mL polyethylene con-
tainers for each sampling location. One container remained
unpreserved for anion analyses. The other container was
for cation analyses and thus was filtered through a 0.45-µm
membrane filters (Milipores) and acidified with ­HNO3 to
pH < 2 to stop bacterial growth and metal oxidation (Appelo
and Postma 2004). All the samples were kept at 4 °C and
transported to the laboratory for analysis.
Major cations, namely, C ­ a2+, ­Mg2+, ­Na+, ­K+, ­Fe2+, and
2+
­Mn , were determined using Inductively Coupled Plasma
Mass Spectrometry (ICP-MS) via a NexION® 300 (Perki-
nElmer, USA). Meanwhile, major anions, such as ­CO32−,
­H CO 3−, ­C l −, ­S O 42−, and N
­ O 3−, were measured using a
DX-500 Ion Chromatography (IC) system (Dionex, USA).
All the water sampling procedures and analyses followed
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397 Page 4 of 15
Fig. 1  Groundwater level of shallow aquifer in the study area
those written by the APHA (1995). The chemical analyses
were carried out at the Chemistry Department Laboratory
in Petaling Jaya, Malaysia. Reliability of the chemical
analyses was evaluated via calculation of charge balances
between cations and anions, wherein the ionic balances
were within ± 5% (Hem 1989) and was determined using
the following calculation (Freeze and Cherry 1979).
(Σcations − Σanions)
Ionic balance (%) = × 100.
(Σcations + Σanions)
The saturation indices of groundwater samples were
determined using the geochemical modelling program
PHREEQC (Parkhurst and Appelo 1999). Hydrogeochem-
ical data were analyzed using graphical and ArcGIS 9.3
software to summarize the groundwater type and prepare
spatial distribution maps. Meanwhile, descriptive statisti-
cal analysis was performed using XLSTAT 2014.5.03.
13
Environmental Earth Sciences (2018) 77:397
Results and discussion
Geological setup
Based on the lithological data correlation of the exploration
wells, three major aquifers were recognized; shallow, interme-
diate, and deep aquifers (Fig. 4). Therefore, all 101 sampling
wells were divided into three aquifers, depending on the screen
depth. The shallow aquifer had 64 wells, the intermediate aqui-
fer had 14 wells, and the deep had aquifer 23 wells.
Geochemical evaluation
Shallow aquifer
The measured pH values ranged from 5.88 to 7.70, with
an average of 6.88. This acidification was likely due to
Environmental Earth Sciences (2018) 77:397
Fig. 2  Cross-section line of exploration wells
oxidation of iron sulfide (in the form of pyrite) and organic
matter decomposition (Mokhtar et al. 2009). Pyrite ­(FeS2)
can only be formed in inundated sediments (Shamshud-
din et al. 2013), suggesting that the area was previously
inundated by seawater (Suswanto et al. 2007). The EC and
TDS values ranged from 29 to 793 µS/cm and from 19 to
489 mg/L, respectively. However, some groundwater sam-
ples in the shallow aquifer had high values of EC and TDS,
as shown by well stations KB 38, NW 10, NW 17, and NW
19, probably owing to contamination from sewage leakage
and fertilizer application (Lim et al. 2017).
The ­Ca2+ and ­Mg2+ concentrations ranged from 0.45 to
73.34 mg/L and from 0.11 to 26.01 mg/L, respectively. The
Page 5 of 15 397
­ a+ concentration varied from 2.75 to 43.63 mg/L, whereas
N
the ­Cl− concentration value ranged from 2.75 to 64.30 mg/L.
The range of C ­ O32− and H
­ CO3− concentrations was between
0.50 and 8.33 mg/L and 4.33–245.00 mg/L, respectively. The
­SO42− and N ­ O3− values ranged from 0.50 to 67.97 mg/L and
from 0.12 to 40.00 mg/L, respectively, whereas the concen-
trations of ­Fe2+ and M­ n2+ ranged from 0.01 to 17.59 mg/L
and from 1.36 to 30.30 mg/L, respectively. The source
of ­Ca2+ could be Ca-plagioclase feldspar, amphibole and
hornblende minerals (Thivya et al. 2015). The dissolution
of micaceous, pyroxene or amphibolite minerals and mica
as well as the alteration of clays, dissolution of dolomite
and magnesium calcites, and fresh water–seawater mixing
13
397 Page 6 of 15
Fig. 3  Location of groundwater sampling wells and geology of the study area (Modified from MGD 2008)
are the main source of ­Mg2+ (Back et al. 1993; Appelo and
Postma 2004).
Intermediate aquifer
The pH values in the intermediate aquifer ranged between
6.30 and 8.15. The EC and TDS values ranged from 74
to 11,416 µS/cm (well station KB 34) and from 77 to
13
Environmental Earth Sciences (2018) 77:397
6724 mg/L, respectively, with averages of 1,498 µS/cm and
907 mg/L. The high variation in EC and TDS values was
associated with saltwater that was entrapped in the alluvial
layer during the Holocene transgression period. The con-
centrations of ­Ca2+ and ­Mg2+ showed large variations, from
1.54 to 151.46 mg/L (well station KB 34) and from 1.31 to
158.50 mg/L (well station KB 34), respectively. Meanwhile,
the ­Na+ and ­Cl− values ranged from 5.16 to 125.29 mg/L
Environmental Earth Sciences (2018) 77:397
Fig. 4  Geological fence dia-
gram of Lower Kelantan Basin
and from 2.14 to 3515.15 mg/L, respectively. The high val-
ues of ­Na+ and ­Cl− in the intermediate aquifer were prob-
ably due to the presence of ancient seawater (Karanth 1987;
Samsudin et al. 2008).
The concentrations of ­CO32− and ­HCO3− ranged from
0.50 to 6.00 mg/L and from 30.00 to 457.11 mg/L, respec-
tively, whereas the concentration of S ­ O42− ranged between
1.25 and 15.50 mg/L, with an average of 3.17 mg/L. The
­NO3− concentration ranged from 1.86 to 26.68 mg/L, with
an average of 6.15 mg/L, and about 14% of the groundwater
samples exceeded 10 mg/L of ­NO3−. The ­Fe2+ and ­Mn2+
contents ranged from 1.93 to 59.59 mg/L (well station KB
31) and from 0.01 to 1.26 mg/L, respectively.
Deep aquifer
In the deep aquifer, the pH values ranged between 3.67
and 8.30, whereas the EC and TDS values ranged from
61 to 1351 µS/cm and from 62 to 853 mg/L, respectively.
The ­Ca2+ and ­Mg2+ concentrations ranged from 1.24 to
42.00 mg/L and from 1.16 to 25.67 mg/L, respectively. The
­Na+ and C
­ l− values ranged from 5.93 to 1,830.58 mg/L (well
station KB 34) and from 2.43 to 354.86 mg/L, respectively.
The possible sources of ­Na+ were seawater, dissolution
of sodium-bearing minerals, Na-plagioclase from granite
weathering, agricultural fertilizer, K-feldspar, and micaceous
minerals (Appelo and Postma 2004; Kumar et al. 2009).
Generally, the pH values in the shallow, intermediate and
deep aquifers were acidic to slightly alkaline. Figures 5 and
6 show the spatial distributions of pH and EC in the different
aquifers, respectively.
In deep aquifer, the C ­ O32− and H ­ CO3− concentrations
ranged from 0.50 to 1.34 mg/L and from 1.79 to 82.00 mg/L,
respectively. The C­ O32− and H ­ CO3− in all the groundwater
Page 7 of 15 397
aquifers could have resulted from the oxidation of organic
matter and the dissolution of carbonate matrix minerals
(Sprinkle 1989; Appelo and Postma 2004; Jeevanandam
et al. 2007; Prasanna et al. 2010). The higher values of
­HCO3− in coastal areas have an almost similar trend with the
­Mg2+ and C ­ a2+ concentrations. S ­ O42− ranged from 1.45 to
3.81 mg/L, with the primary source the oxidation of pyrite,
which affected the mixed fresh water–seawater in the aquifer
and dissolution of sulfate-bearing minerals (Back et al. 1993;
Suratman 1997; Lakshmanan et al. 2003; Jeevanandam et al.
2007). The S ­ O42− values, particularly in the intermediate
aquifer, were quite low compared to those of the present sea-
water composition, indicating that the intermediate aquifer
was influenced by ancient seawater trapped during sediment
deposition (Samsudin et al. 2008).
The values of N ­ O3− in deep aquifer ranged between 0.88
and 4.29 mg/L, and higher ­NO3− values were found pre-
dominantly in the shallow aquifer of the eastern and central
parts of the study area. The elevated values of N ­ O3− could
be due to the direct leaching of agrochemical fertilizers and
leakage from the sewage systems (Fig. 7) (Suratman 1997;
Cheong et al. 2012). The F ­ e2+ and M­ n2+ contents in the
deep aquifer ranged from 0.06 to 1.72 mg/L and from 0.06
to 1.09 mg/L, respectively. The higher values of EC and TDS
in the intermediate aquifer, i.e., within 8 km of the coastline,
compared to those of the shallow and deep aquifers were due
to the remnants of ancient saltwater (Samsudin et al. 2008).
Acidic and anoxic conditions increase the dissolution
of Fe(II)-bearing silicates, siderite (­ FeCO 3) and mag-
netite (Fe(II,III)-oxide) (Appelo and Postma 2004). The
chemistry of F ­ e 2+ is similar to that of M
­ n 2+, yet oxida-
tion reactions of ­Mn are much slower, thus ­Mn2+ exists
2+
longer in oxygenated waters than ­Fe2+ does (Back et al.
1993). The main sources of ­F e 2+ and ­M n 2+ are Fe(II)
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397 Page 8 of 15 Environmental Earth Sciences (2018) 77:397

Fig. 5  Spatial distribution of pH in groundwater samples in a shallow, b intermediate and c deep aquifers

Fig. 6  EC distribution of groundwater samples taken from a shallow, b intermediate and c deep aquifers

and Mn(II)-bearing minerals (magnetite, ilmenite, pyrite, Hydrochemical facies

and siderite) and the dissolution of amphiboles, pyroxene,
biotite, and clay minerals. This indicates that the ­F e 2+
and ­M n 2+ in the groundwater aquifers were from natu-
ral processes and not from anthropogenic activities. The
comparison of hydrochemical parameters in the different
aquifers is shown in Table 2. Figure 8 shows the spatial
distribution of F­ e2+ in the different aquifers. The hydro-
geological profile along E–E′ in relation to EC and water
types of the study area is shown in Fig. 9.
Hydrogeochemical facies analysis is an important method
for determining groundwater type based on major ions (Piper
1944) and reflects the chemical reaction process when water
passes through pore spaces and rock fractures (Gnanachan-
drasamy et al. 2014). The sequence of the major cations
was ­Na+ > ­Ca2+ > ­Mg2+ > ­K+ and of the anions ­HCO3− >
­Cl−> ­SO42− > C­ O32−. The major groundwater facies in the
shallow aquifer were Ca–HCO3 and Na–HCO3, indicating

13
Environmental Earth Sciences (2018) 77:397 Page 9 of 15 397

Fig. 7  Spatial distribution of ­NO3− in a shallow, b intermediate and c deep aquifers

Table 2  Comparison of hydrochemical parameters for the different aquifers of the Lower Kelantan Basin
Parameters Unit Shallow aquifer Intermediate aquifer Deep aquifer
Range Average SD Range Average SD Range Average SD

pH – 5.88–7.70 6.64 0.38 6.30–8.15 7.02 0.49 3.67–8.03 6.49 0.94

EC µS/cm 29–793 195 166 74–11,416 1498 3143 61–1351 301 354
TDS mg/L 19–489 142 102 77–6724 907 1819 62–853 219 220
Ca2+ mg/L 0.45–73.34 14.86 16.05 1.54–151.46 21.77 38.61 1.24–42.00 12.19 12.44
Mg2+ mg/L 0.11–26.01 3.74 4.43 1.31–158.50 20.30 40.84 1.16–25.67 7.56 7.80
Na+ mg/L 2.75–43.63 12.10 8.81 5.93–1830.58 239.03 515.10 5.16–125.29 24.73 31.88
K+ mg/L 0.87–15.02 4.42 3.17 2.48–47.77 10.90 12.50 3.75–32.43 9.14 6.59
CO32− mg/L 0.50–8.33 0.96 1.60 0.50–6.00 1.46 1.72 0.50–1.34 0.59 0.17
HCO3− mg/L 4.33–245.00 57.05 62.69 30.00–457.11 119.57 127.00 1.79–82.00 46.55 19.22
Cl− mg/L 2.75–64.30 15.43 12.46 2.14–3515.15 414.51 977.38 2.43–354.86 62.12 101.24
SO42− mg/L 0.50–67.97 10.95 11.06 1.25–15.50 3.17 3.76 1.45–3.81 2.02 0.63
NO3− mg/L 0.12–40.00 7.12 7.71 1.86–26.68 6.15 6.85 0.88–4.29 2.19 1.01
Fe2+ mg/L 0.01–17.59 3.17 3.70 1.36–30.30 10.38 8.55 1.93–59.59 15.04 12.76
Mn2+ mg/L 0.01–1.26 0.16 0.19 0.06–1.72 0.33 0.42 0.06–1.09 0.29 0.24

SD standard deviation

fresh water and mix-water types, respectively. Na–HCO3 and
Na–Cl are the main water facies in the intermediate aquifer,
suggesting mixed-water and saltwater types, respectively.
Meanwhile, Na-HCO3 was the dominant water facies in the
deep aquifer. The Ca-HCO3 in the shallow aquifer may be
associated with calcite dissolution of seashell fragments
from fluvial-marine deposition (Appelo and Postma 2004).
Weathering of plagioclase feldspar minerals from schist
and ferruginous shale bedrock could be the cause for the
Na–HCO3 water type in the deep aquifer (Srinivasamoor-
thy et al. 2011). Groundwater samples in the intermediate
aquifer were dominated by the Na–Cl type, indicating the
effect of intruded seawater (Aris et al. 2007) that was trapped
during ancient marine transgression (Samsudin et al. 2008).
Figure 10 shows the water-type distribution and Piper trilin-
ear diagram of the shallow, intermediate, and deep aquifers
of the study area (Fig. 11).
Saturation index (SI) and mineral equilibrium
Saturation index (SI) and mineral equilibrium calculations
are essential for assessing and estimating the presence of
mineral reactivity in groundwater systems without having
to gather solid-phase samples or examine the mineralogy
(Deutsch and Siegel 1997). The SI results revealed that
for, Fe(OH)3, goethite, hematite, and manganite, SI > 0.

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Fig. 8  Fe2+ distribution of groundwater samples in a shallow, b intermediate and c deep aquifers

Fig. 9  The geological profile in relation to Electrical Conductivity, EC (µS/cm) and water type of the study area (the cross-section line E–E′ is
indicated in Fig. 1)

Fig. 10  Spatial distribution of groundwater types in a shallow, b intermediate and c deep aquifers

13
Environmental Earth Sciences (2018) 77:397 Page 11 of 15 397

Fig. 11  Piper trilinear diagram SA

of the shallow (SA), intermedi- IA
ate (IA) and deep aquifer (DA)
DA
80 80

>
60 60

4=
SO

<=
Ca
+
Cl
40 40

+M
g
20 20

Mg SO4

80 80

60 60

40 40

20 20
80

60

40

20

20

40

60

80
Ca Na+K HCO3+CO3 Cl

SI > 0 illustrates that the water is oversaturated with respect
to a specific mineral. Therefore, the SI of the water in all
the aquifers indicated oversaturation with Fe(OH)3, goe-
thite, hematite, and manganite. However, the water indi-
cated undersaturation of the anhydrite, aragonite, calcite,
dolomite, gypsum, and halite minerals (Table 3), as the
SI ≤ 0.
The existence of water samples in oversaturated states of
Fe(OH)3, goethite and hematite suggests an abundance of
iron-bearing minerals in the aquifer, because of weathering

Table 3  Saturation indices of minerals in different groundwater aquifers using PHREEQC

Parameter Shallow aquifer Intermediate aquifer Deep aquifer
Range Average SD Range Average SD Range Average SD

Anhydrite − 5.94 to − 2.01 − 3.63 0.75 − 5.09 to − 3.33 − 4.21 0.43 − 4.94 to − 3.73 − 4.29 0.35
Aragonite − 2.3 to 0.92 − 0.81 0.61 − 1.55 to 0.59 − 0.68 0.61 − 3.76 to − 0.58 − 1.24 0.77
Calcite − 2.16 to 1.06 − 0.67 0.61 − 1.41 to 0.73 − 0.53 0.61 − 3.61 to − 0.43 − 1.10 0.77
Dolomite − 4.57 to 1.81 − 1.64 1.06 − 2.3 to 1.33 − 0.93 1.13 − 7.01 to − 0.83 − 2.10 1.49
Fe(OH)3 − 0.62 to 3.79 1.36 0.89 0.18 to 3.65 1.86 0.82 1.14 to 4.17 2.50 0.80
Goethite 5.27 to 9.68 7.25 0.89 6.07 to 9.54 7.75 0.82 7.03 to 10.06 8.39 0.80
Gypsum − 5.72 to − 1.79 − 3.41 0.75 − 4.87 to − 3.11 − 3.99 0.43 − 4.72 to − 3.51 − 4.07 0.35
Halite − 9.63 to − 7.14 − 8.47 0.54 − 9.42 to − 3.91 − 7.38 1.78 − 9.20 to − 5.95 − 8.13 1.05
Hematite 12.54 to 21.36 16.51 1.78 14.15 to 21.09 17.52 1.64 16.08 to 22.12 18.8 1.60
Manganite 0.32 to 6.83 4.43 1.42 1.77 to 6.85 5.29 1.28 − 6.13 to 5.73 3.44 3.20

SD standard deviation

13
397 Page 12 of 15
processes and aerated zones formed by the variability in the
water table (Singh et al. 2015). The undersaturated state of
calcium-bearing minerals may be attributed to the weather-
ing of calcite and dolomite minerals. The SI is important in
water chemistry, particularly regarding calcium carbonate,
as its solubility equilibrium is directly associated with scale
formation on equipment and incrustation of well screens,
filter sand, and water taps (Larson et al. 1942). The SI can
also provide information about water–rock reactions, water
hydrochemistry, and rock mass composition (Drever 1988;
Yidana et al. 2010).
Hydrogeochemical process
The geochemical reaction mechanism in the aquifer between
groundwater and lithology, and understanding the water
source (Vasanthavigar et al. 2012) can be derived using a
Gibbs diagram (Gibbs 1970). Gibbs diagrams were formed
by plotting a ratio of major cations (­ Na+ + K­ +)/(Na+ + K­ +
2+ − −
+ ­Ca ) against TDS and a ratio of major anions C ­ l /(Cl +
­HCO3−) against TDS and include three main zones: pre-
cipitation, evaporation, and rock dominance. In this study,
the majority of samples from the shallow, intermediate, and
deep aquifers fell in the rock and rainfall dominance zones
(Fig. 12), which indicates that the weathering of rock-form-
ing minerals and rainwater infiltration into the aquifers were
the main factors contributing to the groundwater chemis-
try (Todd 1980; Gnanachandrasamy et al. 2014). However,
some groundwater samples from the intermediate aquifer
Fig. 12  Gibbs diagram show the mechanism governing the hydrogeochemistry of water a major cations versus TDS and b major anions versus
TDS from shallow aquifer (SA), intermediate aquifer (IA) and deep aquifer (DA)
13
Environmental Earth Sciences (2018) 77:397
fell in the evaporation dominance zone, an indication that
the water was influenced by fossil seawater, probably trapped
during sedimentation in this area (Samsudin et al. 2008).
The groundwater samples that fell outside the diagram may
have been influenced by anthropogenic activities (Srini-
vasamoorthy et al. 2008). The geochemical variations and
mechanisms in the aquifer system can also be understood
by plotting ­Ca2+ versus ­Mg2+, ­Ca2+ + ­Mg2+ versus ­SO42− +
­HCO3− and C ­ O42− (Aghazadeh and Mogaddam
­ a2+ versus S
2011) (Fig. 13). The groundwater samples mostly fell on
the ­SO42− + H­ CO3− side, indicating that carbonate dissolu-
tion was the main factor influencing the hydrogeochemical
processes in the study area. Meanwhile, the excess C ­ a2+ and
2+
­Mg could have resulted from reverse ion exchange pro-
cesses (Varol and Davraz 2014).
Conclusions
Studying groundwater hydrogeochemistry is challenging
in multilayered aquifers, such as Lower Kelantan Basin,
which consists of shallow, intermediate, and deep aquifers.
Groundwater facies change from fresh water (Ca–HCO3) in
the shallow aquifer, to saline water (Na–Cl) in the interme-
diate aquifer, and finally weathering of plagioclase feldspar
mineral (Na–HCO3) in the deep aquifer, which indicates that
seawater intrusion mostly affected the intermediate aquifer
in Lower Kelantan Basin. Based on the Gibbs diagram, most
of the water samples were in the rock and rainfall dominance
Environmental Earth Sciences (2018) 77:397 Page 13 of 15 397

(a) ◂ Fig. 13  Relationship between a ­Ca2+ versus M

­ g2+, b ­Ca2+ + M
­ g2+
4 versus ­SO42− + H
­ CO3− and c ­Ca2+ versus S
­ O42− of groundwater sam-
ples from shallow (SA), intermediate (IA) and deep aquifers (DA)

3 Carbonate zone, which indicates that dissolution of rock-forming min-

weathering erals and rainwater infiltration are the main factors gov-
erning the groundwater chemistry. The hydrogeochemical
analysis results revealed that the EC, TDS, C ­ a2+, ­Mg2+,
Ca2+ (meq/L)

+ + −
2 SA ­Na , ­K , and C ­ l had higher concentration values in the
Silicate IA intermediate aquifer owing to ancient seawater influence.
weathering DA
However, the results of the descriptive statistical analysis
1
revealed a high average concentration of nitrate in the shal-
low aquifer, which indicates the vulnerability of the shallow
aquifer to contaminate via anthropogenic activities, such as
intensive application of fertilizers in cultivated lands. This
0 study provides and contributes to the comprehensive under-
0 1 2 3 4
Mg2+ (meq/L)
standing of hydrogeochemistry in the study area. Based on
the study’s results, it is recommended that local authorities,
(b) water operators, and related agencies stringently monitor
5
groundwater abstraction, groundwater quality, as well as
4.5 agricultural activities in this area to ensure the sustainability
4
of this invaluable resource for future use.

3.5 Acknowledgements The authors would like to thank the Ministry of

Natural Resources and Environment (NRE) for providing research
Ca2+ + Mg2+ (meq/L)

3 funds to this study under the National Water Resources Council

(P23101110117300). The authors also wish to thank the Miner-
2.5 SA
als and Geoscience Department of Malaysia for allowing the use of
IA
2 their groundwater quality data and assistance during the collection of
DA groundwater samples from their monitoring wells.
1.5

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