Hydrogeochemistry and groundwater quality

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cations and anions were Na+ > Ca2+ > Mg2+ > K+ and HCO3 ... carbonate, and inflow of contamination from anthropogenic ... ing from about 3.0 to 127.5 m. .... and magnesium calcites, and fresh water–seawater mixing ... 3 Location of groundwater sampling wells and geology of the study area (Modified from MGD 2008) ...
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 © 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 hydrogeochemistry. This study was carried out to increase understanding of the geological setup and assess the groundwater hydrogeochemical 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 ­ g2+ > K ­ + and ­HCO3− > C ­ l− > S ­ O42− > C ­ O32−, respectively. In the intermediate aquifer, the influence of ancient seawater was the primary factor that contributed to the elevated values of electrical conductivity (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 Groundwater plays a significant role in providing water supply 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 [email protected] 1



Hydrogeology Research Centre, National Hydraulic Research Institute of Malaysia, 43300 Seri Kembangan, Selangor, Malaysia

2



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



and ensure food security (UNESCO 2012). Availability and quality concerns pose a challenge to groundwater management, 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 attention 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 dissolution–precipitation (Amiri et al. 2015), oxidation–reduction (Rao et al. 2012), adsorption–desorption (Isa et al. 2012), 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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Owing to high permeability and hydraulic conductivity values of unconsolidated materials, many coastal aquifers are highly vulnerable to anthropogenic activities, such as agricultural activities and unregulated groundwater abstraction (Chidambaram et al. 2009). This has led to serious threat to groundwater quality, particularly via seawater intrusion, water–rock interaction, weathering of silicate, dissolution of carbonate, and inflow of contamination from anthropogenic sources in the study area (Sheikhy Narany et al. 2014). Several studies have indicated the roles of the oversaturation of groundwater, high permeability, rapid urbanization, and agricultural activities in coastal areas to the deterioration of groundwater quality (Park et al. 2005; Ferguson and Gleeson 2012; Idris et al. 2016). A recent study by Narany et al. (2017) has shown the impact of intensive human activities and deforestation in Lower Kelantan Basin, in the form of increasing nitrate contamination in the shallow aquifer over 25 years, from 1989 to 2014. Thus, systematic and continuous monitoring of groundwater quality is very important, particularly where high-density populations are situated over coastal aquifers, owing to the high vulnerability to saltwater intrusion, human activities, and impacts on climate change of these areas (Keesari et al. 2016). Lower Kelantan Basin is the biggest groundwater abstraction area and one of the largest agriculturally active region in Malaysia (MWA 2011). Approximately 75% of the Lower Kelantan Basin population relies on groundwater to meet their daily needs. In 2012, about 160 million liters per day (MLD), or 40% of the total state water usage came from groundwater sources. Groundwater consumption has increased significantly over the years and is expected to continuously increase by 2.5% a year (Wan Mohd Zamri et al. 2012), owing to the high demand for domestic and industrial water supplies. However, the situation is becoming more critical as groundwater resources are the sole water source for treated and untreated water. This is due to limited surface water sources, many of which are exposed to severe sedimentation and high turbidity, such as rivers damaged by logging and sand mining activities in the upstream area (Ahmad et al. 2009). A thorough understanding of the hydrochemical process is very important for the protection of groundwater resources and their effectiveness. It is also crucial for sustainable groundwater management (Tizro and Voudouris 2008). A study by Samsudin et al. (2008) combined hydrogeochemical analysis and a geophysical survey to delineate the salinity of groundwater aquifers along the coastal area of north Kelantan. The results indicated that the fresh water and saltwater interface in the intermediate aquifer was located as far as 8 km from the coast. The sulfate concentration of the second aquifer was relatively low compared to those of the current seawater composition, which suggests that the brackish water is probably from ancient seawater.

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The aim of this study was to understand the geological setup and to assess the groundwater hydrogeochemical characteristics of Lower Kelantan Basin using classic integrated hydrogeochemical methods, which can lead to better understanding of the hydrochemical system in the study area, and to utilization and management of groundwater resources that is more effective.

Materials and methods Study area Lower Kelantan Basin is located in the northeastern part of Kelantan State, Peninsular Malaysia. The study area comprises the Kota Bharu, Bachok, Pasir Mas, and Tumpat districts; lies between the latitudes of 5°53′N–6°14′N and longitudes of 102°7′E–102°28′E; and covers about 880 km2. The area is bordered by the South China Sea to the east and the Golok River Basin to the west. The Quaternary deposits of coastal aquifers are quite complex because of the depositional environment and composition of the aquifer (Ahamed et al. 2015). The study area is a low elevation coastal plain, which is characterized by surface elevations that vary from a few to 150 m (Bosch 1986). The entire population in the study area totaled up to 624,000 people (DOS 2010). The study area is mainly drained by four major rivers, namely, Kelantan, Pengkalan Datu, Kemasin and Semerak Rivers. The Kelantan River is about 350 km long and has a basin that covers about 85% of the area of Kelantan State. All the river systems flow northwest before discharging into the South China Sea. The study area comprises different types of land use: urban, industrial, rural, and intensive agriculture area, with sampling well screen depths ranging from about 3.0 to 127.5 m. The land use is predominantly agricultural, representing 35.9%, followed by cleared land, built-up area, peat swamp, and forest (Table 1). The Table 1  The percentage of various land use type. Source Modified from Ministry of Agriculture (MOA 2010) Land use type

Area ­(km2)

Percentage (%)

Paddy Mixed agricultural Other crops (fruit) Rubber Coconut Cleared land Built-up area Peat swamp Forest Total

315.90 249.09 75.73 53.48 47.49 46.88 43.57 41.47 6.34 879.95

35.90 28.31 8.61 6.08 5.40 5.33 4.95 4.71 0.72 100.00

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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 disappears towards the coastal area. The alluvium is overlying intrusive bedrock in the northern part of the study area. Meanwhile, sedimentary or metasedimentary bedrock generally 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 processes. 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 intermediate 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 environmental isotopic data. However, these aquifers seemed to be recharged through normal down-gradient water movement 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).

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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 conditions of the study area (Fig. 2). Exploration well data were mainly obtained from the Minerals and Geoscience Department (MGD), the Public Works Department (PWD), contractors, and consultants’ reports. Samples obtained from the exploration wells during the drilling works were geologically 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 hydrogeological layer was defined and built, groundwater sampling 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 sampling wells were collected and analyzed for various parameters (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 portable 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 containers 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  ­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

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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

pH EC TDS Ca2+ Mg2+ Na+ K+ CO32− HCO3− Cl− SO42− NO3− Fe2+ Mn2+

Unit

– µS/cm mg/L mg/L mg/L mg/L mg/L mg/L mg/L mg/L mg/L mg/L mg/L mg/L

Shallow aquifer

Intermediate aquifer

Deep aquifer

Range

Average

SD

Range

Average

SD

Range

Average

SD

5.88–7.70 29–793 19–489 0.45–73.34 0.11–26.01 2.75–43.63 0.87–15.02 0.50–8.33 4.33–245.00 2.75–64.30 0.50–67.97 0.12–40.00 0.01–17.59 0.01–1.26

6.64 195 142 14.86 3.74 12.10 4.42 0.96 57.05 15.43 10.95 7.12 3.17 0.16

0.38 166 102 16.05 4.43 8.81 3.17 1.60 62.69 12.46 11.06 7.71 3.70 0.19

6.30–8.15 74–11,416 77–6724 1.54–151.46 1.31–158.50 5.93–1830.58 2.48–47.77 0.50–6.00 30.00–457.11 2.14–3515.15 1.25–15.50 1.86–26.68 1.36–30.30 0.06–1.72

7.02 1498 907 21.77 20.30 239.03 10.90 1.46 119.57 414.51 3.17 6.15 10.38 0.33

0.49 3143 1819 38.61 40.84 515.10 12.50 1.72 127.00 977.38 3.76 6.85 8.55 0.42

3.67–8.03 61–1351 62–853 1.24–42.00 1.16–25.67 5.16–125.29 3.75–32.43 0.50–1.34 1.79–82.00 2.43–354.86 1.45–3.81 0.88–4.29 1.93–59.59 0.06–1.09

6.49 301 219 12.19 7.56 24.73 9.14 0.59 46.55 62.12 2.02 2.19 15.04 0.29

0.94 354 220 12.44 7.80 31.88 6.59 0.17 19.22 101.24 0.63 1.01 12.76 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 (Srinivasamoorthy 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 trilinear 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

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Environmental Earth Sciences (2018) 77:397 Fig. 11  Piper trilinear diagram of the shallow (SA), intermediate (IA) and deep aquifer (DA)

397 SA IA

60

60

40

40

+M

Cl +

DA

80

Ca

80

g

20

20

Mg

SO4

80

80

60

60

40

40

80

HCO3+CO3

60

Na+K

40

20

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, goethite, hematite, and manganite. However, the water indicated undersaturation of the anhydrite, aragonite, calcite,

40

60

80

Ca

20

20

20

Cl

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

Anhydrite Aragonite Calcite Dolomite Fe(OH)3 Goethite Gypsum Halite Hematite Manganite

Shallow aquifer

Intermediate aquifer

Deep aquifer

Range

Average

SD

Range

Average

SD

Range

Average

SD

− 5.94 to −  2.01 − 2.3 to 0.92 − 2.16 to 1.06 − 4.57 to 1.81 − 0.62 to 3.79 5.27 to 9.68 − 5.72 to −  1.79 − 9.63 to −  7.14 12.54 to 21.36 0.32 to 6.83

− 3.63 − 0.81 − 0.67 − 1.64 1.36 7.25 − 3.41 − 8.47 16.51 4.43

0.75 0.61 0.61 1.06 0.89 0.89 0.75 0.54 1.78 1.42

− 5.09 to −  3.33 − 1.55 to 0.59 − 1.41 to 0.73 − 2.3 to 1.33 0.18 to 3.65 6.07 to 9.54 − 4.87 to −  3.11 − 9.42 to −  3.91 14.15 to 21.09 1.77 to 6.85

− 4.21 − 0.68 − 0.53 − 0.93 1.86 7.75 − 3.99 − 7.38 17.52 5.29

0.43 0.61 0.61 1.13 0.82 0.82 0.43 1.78 1.64 1.28

− 4.94 to −  3.73 − 3.76 to −  0.58 − 3.61 to −  0.43 − 7.01 to −  0.83 1.14 to 4.17 7.03 to 10.06 − 4.72 to −  3.51 − 9.20 to −  5.95 16.08 to 22.12 − 6.13 to 5.73

− 4.29 − 1.24 − 1.10 − 2.10 2.50 8.39 − 4.07 − 8.13 18.8 3.44

0.35 0.77 0.77 1.49 0.80 0.80 0.35 1.05 1.60 3.20

SD standard deviation

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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 weathering 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 ­ +)/(Na+ + K ­ + by plotting a ratio of major cations (­ Na+ + K 2+ − − + ­Ca ) against TDS and a ratio of major anions C ­ l /(Cl + ­HCO3−) against TDS and include three main zones: precipitation, 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-forming minerals and rainwater infiltration into the aquifers were the main factors contributing to the groundwater chemistry (Todd 1980; Gnanachandrasamy et al. 2014). However, some groundwater samples from the intermediate aquifer

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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 (Srinivasamoorthy 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 ­ a2+ versus S ­ O42− (Aghazadeh and Mogaddam 2011) (Fig. 13). The groundwater samples mostly fell on the ­SO42− + H ­ CO3− side, indicating that carbonate dissolution 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 processes (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 intermediate 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

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)

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(a)

versus ­SO42− + H ­ CO3− and c ­Ca2+ versus S ­ O42− of groundwater samples from shallow (SA), intermediate (IA) and deep aquifers (DA)

Carbonate weathering

3

Ca2+ (meq/L)

­ g2+, b ­Ca2+ + M ­ g2+ ◂ Fig. 13  Relationship between a ­Ca2+ versus M

4

SA

2

Silicate weathering

IA DA

1

0 0

1

2

3

4

Mg2+ (meq/L)

(b)

5

4.5 4 3.5

Ca2+ + Mg2+ (meq/L)

397

3 SA

2.5

IA

2

DA

1.5

zone, which indicates that dissolution of rock-forming minerals and rainwater infiltration are the main factors governing the groundwater chemistry. The hydrogeochemical analysis results revealed that the EC, TDS, C ­ a2+, ­Mg2+, + + − ­Na , ­K , and C ­ l had higher concentration values in the intermediate aquifer owing to ancient seawater influence. However, the results of the descriptive statistical analysis revealed a high average concentration of nitrate in the shallow aquifer, which indicates the vulnerability of the shallow aquifer to contaminate via anthropogenic activities, such as intensive application of fertilizers in cultivated lands. This study provides and contributes to the comprehensive understanding of hydrogeochemistry in the study area. Based on the study’s results, it is recommended that local authorities, water operators, and related agencies stringently monitor groundwater abstraction, groundwater quality, as well as agricultural activities in this area to ensure the sustainability of this invaluable resource for future use. Acknowledgements  The authors would like to thank the Ministry of Natural Resources and Environment (NRE) for providing research funds to this study under the National Water Resources Council (P23101110117300). The authors also wish to thank the Minerals and Geoscience Department of Malaysia for allowing the use of their groundwater quality data and assistance during the collection of groundwater samples from their monitoring wells.

1

References

0.5 0 0

1

2

3

4

5

HCO3- + SO42- (meq/L)

(c)

4

Ca2+ (meq/L)

3

SA

2

IA DA 1

0 0

1

2

3

SO42- (meq/L)

4

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