Ecotoxicology and Environmental Safety 253 (2023) 114665

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Ecotoxicology and Environmental Safety

journal homepage: www.elsevier.com/locate/ecoenv

The risk assessment of arsenic contamination in the urbanized coastal

aquifer of Rayong groundwater basin, Thailand using the machine
learning approach
Narongpon Sumdang a, Srilert Chotpantarat b, c, *, Kyung Hwa Cho d, Nguyen Ngoc Thanh e
a
International Postgraduate Program in Hazardous Substance and Environmental Management, Graduate School, Chulalongkorn University, Bangkok 10330, Thailand
b
Department of Geology, Faculty of Science, Chulalongkorn University, Bangkok 10330, Thailand
c
Center of Excellence in Environmental Innovation and Management of Metals (EnvIMM), Chulalongkorn University, Phayathai Road, Pathumwan, Bangkok 10330,
Thailand
d
Department of Urban and Environmental Engineering, Ulsan National Institute of Science and Technology, 50, UNIST-gil, Ulsan 44919, Republic of Korea
e
University of Agriculture and Forestry, Hue University, 102 Phung Hung Str, Hue City, Viet Nam

A R T I C L E I N F O A B S T R A C T

Edited by Dr. Hao Zhu The rapid expansion of urbanization has resulted in an insufficient of groundwater resource. In order to use
groundwater more efficiently, a risk assessment of groundwater pollution should be proposed. The present study
Keywords: used machine learning with three algorithms consisting of Random Forest (RF), Support Vector Machine (SVM),
Arsenic and Artificial Neural Network (ANN) to locate risk areas of arsenic contamination in Rayong coastal aquifers,
Machine learning
Thailand and selected the suitable model based on model performance and uncertainty for risk assessment. The
Groundwater contamination
parameters of 653 groundwater wells (Deep=236, Shallow=417) were selected based on the correlation of each
Spatial probability model
Groundwater risk assessment hydrochemical parameters with arsenic concentration in deep and shallow aquifer environments. The models
Thailand were validated with arsenic concentration collected from 27 well data in the field. The model’s performance
indicated that the RF algorithm has the highest performance as compared to those of SVM and ANN in both deep
and shallow aquifers (Deep: AUC=0.72, Recall=0.61, F1 =0.69; Shallow: AUC=0.81, Recall=0.79, F1 =0.68). In
addition, the uncertainty from the quantile regression of each model confirmed that the RF algorithm has the
lowest uncertainty (Deep: PICP=0.20; Shallow: PICP=0.34). The result of the risk map obtained from the RF
reveals that the deep aquifer, in the northern part of the Rayong basin has a higher risk for people to expose to As.
In contrast, the shallow aquifer revealed that the southern part of the basin has a higher risk, which is also
supported by the location of the landfill and industrial estates in the area. Therefore, health surveillance is
important in monitoring the toxic effects on the residents who use groundwater from these contaminated wells.
The outcome of this study can help policymakers in regions to manage the quality of groundwater resources and
enhance the sustainable use of groundwater resources. The novelty process of this research can be used to further
study other groundwater aquifers contaminated and increase the effectiveness of groundwater quality
management.

1. Introduction
The rapid urbanization increases the demand for water resources for
development caused a shortage of water resources which is mainly
influenced by land use, industrial structure, and population density
factors (Chen et al., 2019). To improve the sustainability of water used,
groundwater is a major freshwater resource that plays an important role
in terrestrial, aquatic ecosystems, and water consumption resources in
human activities such as drinking water, agricultural and industrial as­
pects (Cho et al., 2011). However, the problem of groundwater
contamination has been concerned especially arsenic (As) contamina­
tion in groundwater, that is correlated with various health risks in many
countries, such as China, Taiwan, Bangladesh, India, the USA, Vietnam,
Japan, and Thailand (Wongsasuluk et al., 2018a, 2018b). As is a major
carcinogenic element, which mostly presents in a toxic form as an
inorganic component in groundwater (Chetia et al., 2010). Arsenic can

* Corresponding author at: Department of Geology, Faculty of Science, Chulalongkorn University, Bangkok 10330, Thailand.
E-mail address: Srilert.C@chula.ac.th (S. Chotpantarat).

https://doi.org/10.1016/j.ecoenv.2023.114665
Received 13 July 2022; Received in revised form 26 December 2022; Accepted 15 February 2023
Available online 28 February 2023
0147-6513/© 2023 The Authors. Published by Elsevier Inc. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-
nc-nd/4.0/).
N. Sumdang et al.
be considered a toxic element to humans in several forms, especially
arsenate (As(V)), arsenite (As (III)), and As organic compounds. A lethal
dose in humans is 1.5 mg/kg of body weight (WHO, 2018). The acute
intoxication symptoms include vomiting, abdominal pain, muscular
pain, diarrhea, and weakness, with flushing of the skin, and chronic
intoxication symptoms, including dermal lesions such as hypo­
pigmentation and hyperpigmentation, skin cancer, peripheral neurop­
athy, lung cancers, bladder, and peripheral vascular disease (WHO,
2018). As a result of As toxicity, the monitoring strategies methods to
observe As contamination need to be developed to estimate and predict
As in groundwater. The proper method could be used to impart the
necessary information for better public health and water management
(Cho et al., 2011). However, due to lack of equipment and human re­
sources, As contamination problems remain problematic. Therefore,
modeling methods to predict As contamination using hydrogeological
and on-field measurement data can be used to evaluate and measure the
potential area of As contamination, as well as to notify necessary in­
formation to improve public health and water management (Cho et al.,
2011). The prediction information in terms of the probability and risk
map generated from the model will help to support groundwater man­
agement and to plan to install a monitoring well system for the local
government agencies. The probability map is usually used in many types
of environmental science studies to inform the general information
about a percent chance to encounter some study’s element (Sajedi
Hosseini et al., 2018).
Machine learning (ML) has been used in several fields in environ­
mental scientist studies. The ML power comes from their powerful
nonlinear modeling capability, which is usually used for assessment in
environmental science aspects including groundwater contamination
studies. The ML has been applied to predict several risk assessments in
groundwater resources (Sajedi Hosseini et al., 2018; Bindal and Singh,
2019; Podgorski et al., 2020). Many ML algorithms are usually used in
many studies, such as random forest (RF), support vector machine
(SVM), and artificial neural network (ANN). Random Forest (RF) algo­
rithm is usually used to classify many spatial distribution studies and
shows that this algorithm is very effective and has good accuracy results
with the limited data set and it could provide better stability in the
evaluation process (Liu et al., 2019). On the other hand, a support vector
machine (SVM) is mainly used to classify all data into classes with high
accuracy by constructing a hyperplane (Ghosh et al., 2020). An artificial
neural networks (ANNs) have been used in many studies to evaluate the
contamination in groundwater. and have the advantage of classifying
the complex dataset (Cho et al., 2011; Dawood et al., 2020). When
combined with the PCA technique, ANN algorithms provided a signifi­
cant result to determine the As contamination in groundwater in
Cambodia, Laos, and Thailand (Cho et al., 2011). Moreover, ANNs are
often used to model the classification of spatial distribution. In addition,
several studies have shown that the use of deep neural networks (DNN)
in the model is very effective. However, in the study, a deep neural
network (DNN) is highly effective when applied to a heterogeneous and
high-volume dataset (Sarker, 2021). But in this study, the amount of
data used was limited. That makes the study using ANN more efficient.
All three algorithms are suitable to handle a large dataset to conduct a
model, which has many variables to analyze and predict groundwater
contamination.
In many previous studies, physical parameters such as land use, soil
map, and hydrogeology parameters were mostly used with ML ap­
proaches to predict groundwater pollution risk (Winkel et al., 2008;
Podgorski et al., 2020), which is limited understanding of physical and
hydrochemical parameters to predict contamination in groundwater,
particularly As contamination in the urbanized coastal aquifer (Zubair
et al., 2015). To fulfill this research gap, this study attempted to apply
ML algorithms, including RF, SVM, and ANN to investigate and predict
the As contamination in Rayong coastal basins. The objectives of the
current study: (i) to evaluate and compare ML algorithms such as RF,
SVM, and ANN to predict As contamination in groundwater, (ii) to
2
Ecotoxicology and Environmental Safety 253 (2023) 114665
investigate various environmental factors that influence on As contam­
ination in groundwater, and (iii) to generate the As probability maps and
groundwater pollution risk maps of As contamination based on popu­
lation density and water consumption in the study area. This study can
provide appreciative predictive information for better public health
management and groundwater quality control to support
decision-makers for taking the suitable plans to preserve groundwater
quality and reduce contamination of water resources. Good ground­
water quality will reduce the providing costs to clean water for human
use, and help the sustainable development of water management, water
resources, and the environment.
2. Materials and methods
2.1. Study area
The study area is in the Rayong groundwater basin in eastern
Thailand. The study area is a significant industrial and agricultural area.
The area has undergone rapid development, leading to the potential for
many pollutants to contaminate groundwater (Sonthiphand et al.,
2019). Thailand usually experiences dry weather in winter due to the
northeast monsoon, which is the main cause that controls the climate of
this region (TMD, 2015). In Rayong province, annual rainfall averages
around 1500 mm/year, which is the average rate for annual rain in
Thailand (TMD, 2015). Hydrogeological characteristics in the study area
containing with colluvium sediment (Qc) in the quaternary age has the
largest aquifer area as compared to other hydrogeological units. Another
main hydrogeological unit is alluvium sediment in quaternary age,
which is located alongside the main river in the study area. The other
two aquifers are the consolidated aquifers, including granite (Gr) and
limestone aquifers (Pl), which are in mountainous areas distributed
around the groundwater basin. From the population density data from
the National Statistical Office in 2020, it can be classified into ten dis­
tricts with difference population density. The largest population density
district is Bang Lamung district with 643 people per square kilometer.
Mueang Rayong district is the second largest population density district
with 548 people per square kilometer, following with Si Racha, Sattahip,
Ban Chang, Nikhom Phatthana, Ban Bueng, Ban Khai, Pluak Daeng and
Nong Yai of 512, 496, 313, 208, 166, 138, 110 and 59 people per square
kilometer. The Rayong groundwater basin has been reported in many
studies to be associated with As contamination in groundwater, which
could consequently affect various health risks in local people (Kerdthep
et al., 2009; Boonkaewwan et al., 2017; Pipattanajaroenkul et al., 2018;
Boonkaewwan et al., 2020). Besides, the study area is the part of the
Eastern Economic Corridor (EEC), where is the ongoing economic plan
for Thailand’s Eastern Seaboard, and the government has been launch­
ing measures to support the economic growth in the EEC that will
develop into a new trade center in Asia (Niyomsilp et al., 2020). As a
result, the demand for the groundwater resource in this region will in­
crease dramatically, and the groundwater quality of groundwater must
be considered the priority before pumping groundwater to supply each
sector (Fig. 1).
2.2. Framework of research
The overall framework of this study is shown in Fig. 2. The preparing
data process was conducted by collecting the secondary data such as
hydrochemical data of groundwater from 653 groundwater wells (Deep
= 236, Shallow = 417), soil type, land use, geological characteristic,
aquifer types from various government agencies. The hydrogeological
data were categorized the aquifer into shallow and deep aquifers. The As
concentration was classified by the drinking water standard to further
use them in the modeling process. Other physical and hydrochemical
parameters were selected using spearman’s correlation technique to
screen out unnecessary parameters. In the modeling process, spatial
modeling uses a different algorithm to generate different probability
N. Sumdang et al. Ecotoxicology and Environmental Safety 253 (2023) 114665

Fig. 1. Rayong groundwater basin.

Fig. 2. Framework of the present study.

models such as support vector machine (SVM), random forest (RF), and used in the validation process to measure the models, consisting of
artificial neural networks (ANNs). The probability model was compared classification performance, uncertainty evaluation, and finally predic­
with each other in the validation process. There are three aspects that we tion performance by validation with the field data. The best probability

3
N. Sumdang et al. Ecotoxicology and Environmental Safety 253 (2023) 114665

map was calculated with the population density and water consumption
data in the study area to generate the risk maps.
2.3. Data preparation and field-collected data
2.3.1. Data preparation
The secondary data were collected from various Thai government
departments such as the Department of mineral Resources (DMR), Land
Development Department (LDD), Department of Groundwater Re­
sources (DGR). The data were classified into two groups, physical and
hydrochemical data. The period of hydrochemical data was collected
around 2011–2012, 2017–2018, and 2019 in the dry and rainy seasons
around the study area (DMR, 2007; DGR, 2012, 2017; LDD, 2016). The
physical data such as geological characteristics, soil properties, soil
texture, aquifer characteristics, land use and groundwater level. The
date of these data is not over 10 years as shown in Table 1. Hydro­
chemical data were collected from the DGR included concentrations of
magnesium (Mg), calcium (Ca), sodium (Na), chloride (Cl), iron (Fe),
fluoride(F-), potassium(K), carbonate (CO2- 2-
3 ), bicarbonate (HCO3 ), sul­
fate (SO2-
4 ), nitrate (NO -
3 ), phosphate (PO-
4 ), cadmium (Cd), copper (Cu),
chromium (Cr6+), mercury (Hg), nickel(Ni), manganese (Mn), lead(Pb),
selenium(Se), zinc (Zn), arsenic (As) and other on-field measurement
hydrochemical parameters consisting temperature, electrical conduc­
tivity(EC), temperature, pH, total hardness (TTH), and total dissolved
solids (TDS). There were interpreted from point data to raster data by
using the interpolation technique.
2.3.2. Collected data in the field
The groundwater samples were collected in the rainy season because
the As concentrations across the observation wells in the rainy season
were higher than those in the summer season, as previously reported. In
addition, As concentrations exceeding the drinking water standards of
the World Health Organization (WHO) were found in some shallow
wells located in the community areas within the study area. Thus, the
rainy season was the focus of this study because As contamination in
groundwater in this period is harmful to the local people, who generally
use groundwater for several purposes, especially the public water
supply.
The groundwater’s physicochemical parameters such as tempera­
ture, pH, electrical conductivity (EC) was analyzed. A plastic bailer was
then used to collect groundwater samples. All groundwater samples
were collected and preserved in 60 ML HDPE bottles that were already
cleaned with deionized water and 10% HNO3. To prevent sample
degradation, all samples were transferred to the laboratory in coolers
with ice at 4ºC and preserved with HNO3 for heavy metal analysis.
(American Public Health Association, 2012). The samples were analyzed
by the United Analyst and Engineering Consultant Co., LTD for total As
using the hydride generation AAS method (Shimadzu, AA-6200) (Fig. 3).
Table 1
Sources of physical data.
Data Data source Data
format
Geological Ministry of Natural Resources Shapefile
characteristics
Soil properties Land Development Department Shapefile
Aquifer characteristics Department of Groundwater Shapefile
Resources
Land use Land Development Department Shapefile
Elevation USGS Raster file
Population density National Statistical Office Excels
Groundwater Department of Groundwater Excels
consumption Resources
2.4. Arsenic contamination probability map
The physical and hydrochemical parameters were calculated with
nonparametric Spearman’s rank correlation using the SPSS software to
study the correlation between As and other parameters that were used to
investigate associate of variables (Sangkham et al., 2021). The param­
eters that have a correlation coefficient (rs) in excess of 0.1 with As
concentration were classified as the influence parameters that associate
with As in groundwater and selected to interpret into raster data using
the Inverse Distance Weighting (IDW) technique with the AutoMap
package in R-studio software. IDW interpolation can generate the con­
centration point data into concentration area data by averaging the
point data (Gaafar, 2019) and was used interpolations to estimate
groundwater As concentrations better than Kriging interpolation tech­
nique (Gong et al., 2014).
The framework of model probability is shown in Fig. 4. Arsenic
concentrations which obtained from the dataset were used to establish a
groundwater As probability map in the Rayong groundwater basin. The
arsenic standard following the World Health Organization, a threshold
of arsenic (10 μg/l) was used to classify the polluted and non-polluted
groundwater wells. Groundwater wells were classified into 2 types as
follows: the polluted type (As>10 μg/l), and the non-polluted type (As <
10 μg/l). After that, the datasets were divided into a training dataset
(containing 70% of the dataset) and a testing dataset (containing 30% of
the dataset) (Sajedi Hosseini et al., 2018). The training set was used to
provide the probability models along with three algorithms, consisting
of SVM, RF, and ANN through coding by SDM package in the R-studio
software (Naimi and Araújo, 2016). The default setting of SVM algo­
rithms is following by the svm function from the package ’e1071’, the
Epsilon parameter and the Algocv integer set default at 1e-08 and 3. The
RF algorithm function was used from the package ‘randomForest’, Trees
integer and Final leave integer set default to 2500 and 1. The ANN al­
gorithm uses a function from the package ’nnet’ with a maximum
number of iterations set to 500 with 12,12,12 hidden layers in deep
condition and 22,22,22 hidden layers in shallow condition (Naimi. et al.,
2016). Precession matrices such as recall, fi-score, and AUC are very
robust evaluation metrics that work great for many classification prob­
lems (Magalhaes et al., 2021). Therefore, the model performance was
assessed using the metrics of precision with the test dataset (30%
dataset). The receiver operating characteristic (ROC) is a tool to measure
the performance of the model for the classification task at various
threshold setups. The area under curve (AUC) implies a degree of
dissociation. It indicates how much the model is capable of identifying
between classed data. If the model performance is above 60% of the AUC
value, the model will be acceptable. In contrast, if the model perfor­
mance is below 60% of the AUC value, the model must be calibrated and
provide the new models until it reaches 60% AUC (Havryliuk et al.,
2018). Moreover, a Taylor diagram was used to provide a graphical
comparison, which showed the model’s performance in visualization by
combining standard deviations (SD), and correlation coefficients (Tay­
lor, 2001; Choubin et al., 2017). When the model was completed, the As
probability map was generated using the SDM package in R-studio
software (Naimi and Araújo, 2016).
2.5. Probability map validation
Year
2.5.1. Uncertainty evaluation of the models
2015 To ensure that the models are working properly and reliably, quan­
tile regression (QR) was used to evaluate the model’s predictive un­
2011 certainty value. QR methods were used to calculate the model residuals
2017
and regard uncertainty sources, that is different to the classical methods
2015 such as orthogonal regression, Monte Carlo, and inverse regression
2019 methods that usually consider only one source of uncertainty (Solo­
2019 matine and Shrestha, 2009; Meinrath and Spitzer, 2000). There are
2019 several statistical measures of uncertainty, such as mean prediction in­
terval (MPI) and prediction interval coverage probability (PICP), which

4
N. Sumdang et al. Ecotoxicology and Environmental Safety 253 (2023) 114665

Fig. 3. Groundwater sampling map.

Fig. 4. Framework of constructing the probability model of As.

were used as suggested by Shrestha and Solomatine (Shrestha and measurement of uncertainty as it indicates the number of observations
Solomatine, 2006). MPI is the average of the widths of the prediction that fall within the estimated interval (Dogulu et al., 2015). Therefore,
intervals, where the lower values of MPI indicate lower uncertainty. The MPI is used as a supplementary metric: between models with similar
best method MPI and PICP values are calculated as: PICP values, the one with a lower MPI is regarded as the better model
(Muthusamy et al., 2016).
1∑ n
MPI = (PLupper
t − PLlower
t )
n t=1 2.5.2. Validation with field data
The As concentration collected in the field was classified into 2 types
1∑ n
as follows: the polluted type (As>10 μg/l), and the non-polluted type
PICP = C, C = (1, PLlower < yt < PLupper , 0, otherwise)
(As < 10 μg/l). To compare the forecasting performance of a model, root
t t
n t=1
mean square error (RMSE) and the mean absolute error (MAE) are used
where yt is the observed value, PLlower
t and PLupper
t are lower and upper for validation as a measurement indicator by compare between the
prediction limits respectively. The PICP is the more important actual value and prediction value from the probability map in each

5
N. Sumdang et al.
model. RMSE is often used to test the prediction performance of spatial
distribution model (Rahmati et al., 2019) with the standard formula as:
√̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅
√N
√∑
√ (xi − ̂x i )2
√ a positive correlation with sodium (Na) (r = 0.642), chloride (Cl)
RMSD = i=1
N (r = 0.526), sulfate (SO4) (r = 0.428), magnesium (Mg) (r = 0.595) and
N=number of non-missing data pointsxi =actual observations time ser­
ies ̂
x i =estimated time series.
The mean absolute error (MAE) is another useful measure widely
used in model evaluations. The MAE is the average over the verification
sample of the absolute values of the differences between the forecast and
the corresponding observation.
1∑ n
MAE = |ei |
n i=1
The MAE and the RMSE can be used together to diagnose the vari­
ation in errors in a set of forecasts. the RMSE will always be greater than
or equal to the MAE; the larger the gap between the two, the more
variability there is in the sample’s individual errors. All errors will be of
the same magnitude if RMSE=MAE (Chai et al., 2014).
2.6. Groundwater pollution risk map
The risk map was created using the overlay technique in QGIS soft­
ware by overlaying the probability map with population density and
water consumption in the study area following by Eq. (1). The popula­
tion density data was derived from the Bureau of Registration Admin­
istration in 2020 (NSO, 2020) and the water consumption obtain from
the Department of Groundwater Resources (DGR, 2020). The water
consumption data was created using the pumping rate of groundwater
well, which has been used in domestic and agricultural sectors in the
study area. The pumping rate was standardized into 0–1 values to
represent the areas that were affected by the groundwater consumption.
Risk = Probability map x Population density x Water consumption (1)
These two risk maps (Deep and Shallow) were classified into five risk
levels: very high, high, moderate, low, and very low, using equal interval
mode in the classification process (Bindal and Singh, 2019).
3. Results and discussion
3.1. Mechanism of arsenic release
The spearman’s correlation was used in this process to screen un­
necessary parameters before using them in the modeling process. For
making sure the spearman’s correlation selected useful parameters, the
correlation between other parameters and total As in groundwater had
to toughly reviewed. The natural As sources in groundwater mostly
come from the weathering of certain rock types in the region and are
released into groundwater (Adithya et al., 2016). The other sources of As
in groundwater can be from anthropogenic activities such as leachates
infiltrating through municipal waste in landfills that were contaminated
with various organic and inorganic substances (Kumari et al., 2017). The
result of previous studies indicated that As sources in groundwater
probably came from both natural and anthropogenic sources (Boon­
kaewwan et al., 2020). This was in agreement with previous studies,
which revealed that high total As concentrations in groundwater were
highly positively correlated with bicarbonate (HCO3) concentrations
under the reducing condition in the groundwater environment. Calcium
(Ca) had a high positive correlation with magnesium (Mg) (r = 0.672)
and bicarbonate (HCO3) (r = 0.744) that indicates the dissolution of
calcite minerals from geological formations into groundwater. The
correlation between magnesium (Mg) and sodium (Na) (r = 0.466)
signifies that it has an ion exchange reaction in groundwater (Sae-Ju
6
Ecotoxicology and Environmental Safety 253 (2023) 114665
et al., 2019). Total dissolve solids (TDS) were correlated with electrical
conductivity (EC) (r = 0.612), Sodium (Na) (r = 0.546), Chloride (Cl)
(r = 0.50), Sulfate (SO4) (r = 0.350), Magnesium (Mg) (r = 0.611) and
Calcium (Ca) (r = 0.672). Similarly, the electrical conductivity (EC) was
calcium (Ca) (r = 0.710) as shown in Table SI1. These correlations with
the electrical conductivity (EC) indicate that the increase in salinity level
was influenced by seawater intrusion and groundwater mineralization
(Sae-Ju et al., 2019).
For the shallow aquifer shown in Table SI2, like the deep aquifer,
calcium also had a high positive correlation with magnesium (Mg)
(r = 0.650) and bicarbonate (HCO3) (r = 0.790) indicating the dissolu­
tion of calcite in aquifers. The relation between magnesium (Mg) and
sodium (Na) (r = 0.630) implied that it has an ion-exchange reaction
during seawater intrusion. Total dissolve solids (TDS) was highly
correlated with electrical conductivity (EC) (r = 0.957), sodium (Na)
(r = 0.839), chloride (Cl) (r = 0.720), sulfate (SO4) (r = 0.647), mag­
nesium (Mg) (r = 0.710) and calcium (Ca) (r = 0.799). Similarly, the
electrical conductivity (EC) was positively correlated with sodium (Na)
(r = 0.817), chloride (Cl) (r = 0.696), sulfate (SO4) (0.623), magnesium
(Mg) (r = 0.692) and calcium (Ca) (r = 0.786). These correlations with
the electrical conductivity (EC) indicate that the increase in salinity was
also caused by seawater intrusion and groundwater mineralization
(Sae-Ju et al., 2019). These can indicate that the aquifers were influ­
enced by seawater. In addition, As had a positive correlation with pH
and a negative correlation with NO3, implying that reducing conditions
might cause the release of As in the shallow aquifer in the Rayong
groundwater basin.
Many studies reported that the reducing environment is mainly
caused of As contamination in groundwater through a denitrification
process, leading to As released into groundwater (Boonkaewwan et al.,
2020). The majority of As in groundwater was usually in oxidation form
including As-rich Fe oxyhydroxide (FeOH) and As-bearing pyrite that
exists as a coating on soil particles throught an oxidation process (Bulut
et al., 2013). In addition, the reducing environment also affected to
microbial degradation of organic matter in groundwater, while
consuming O2 and NO3, the microbial release As into groundwater, and
this directly impacts As concentration in groundwater (Nickson et al.,
2000). According to the previous study (Boonkaewwan et al., 2021),
they studied As levels that increased with decreasing ORP. This indicates
that the reducing environment is widespread in the groundwater system
in this study area.
In addition, anthropogenic activities, such as agriculture field, ur­
banized wastewater, livestock area, industrial site, and municipal
landfill station, some organic pollutants, and acid from the surface area
leaches into the groundwater system, enchant the reducing environment
with a high correlation with sulfate (SO4) and nitrate (NO3). In the
reducing environment, the microorganism increases both sulfate (SO4)
and nitrate (NO3) in the groundwater system with a denitrification
process, in which NO3 is reduced to ammonia. When arsenate moves
from iron oxides reductive by the iron-reducing bacteria, and subse­
quent arsenate reduction by bacteria that produce ammonia (Fytianos
and Christophoridis, 2004). From the correlation between sulfate (SO4)
and nitrate (NO3) with negative correlation (r = − 0.086), it means that
microorganisms increased sulfate (SO4); on the other hand, nitrate
(NO3) was used to release the As (Boonkhao et al., 2017).
The physical parameters influencing total As concentrations
(Tables SI3 and SI4) in groundwater are mainly from hydrogeological
characteristics, soil types, and agricultural area. For example, in shallow
aquifer as shown in Table SI4 total As was mainly associated with sandy
(r = − 0.127), clay (r = 0.143), granite (r = 0.206) and quaternary al­
luvium (r = − 0.152). The correlation indicates that bedrock and soil
types slightly correlate with As release into the groundwater environ­
ment. Moreover, the correlation with the agricultural area (r = − 0.124)
could indicate the anthropogenic activities of agriculture in the area.
N. Sumdang et al. Ecotoxicology and Environmental Safety 253 (2023) 114665

However, although physical parameters can be screened by spearman’s Table 3

correlation technique, it does not help much in explaining the mecha­ Performances of SVM, RF, and ANN in the deep and shallow aquifers.
nism of As release in groundwater. Model Train Test
Therefore, Spearman’s correlation can be used to select hydro­
Deep AUC Recall F1 AUC Recall F1
geochemical and physical parameters that are significantly related to As.
In addition, the influence factors that affected an As mechanism in the SVM 0.73 0.49 0.61 0.69 0.32 0.38
RF 0.93 0.51 0.66 0.72 0.61 0.69
study area could come from both anthropogenic and natural sources as ANN 1.00 0.22 0.32 0.65 0.14 0.18
shown in Table 2. Shallow
SVM 0.84 0.34 0.28 0.79 0.48 0.39
RF 0.93 0.90 0.79 0.81 0.79 0.68
3.2. Evaluation of the predictive performance of models ANN 1.00 1.00 1.00 0.75 0.75 0.70

The classification performance, which showed how well the model

fits with the data were also quantified by precession matrices mea­
surements (Recall, Fi-Score and AUC). In the classification performance
(training dataset) of the deep aquifer, the ANN model produced a very
high performance of total As probability model (AUC=1.00,
Recall=0.22, F1 =0.32), followed by SVM (AUC=0.73, Recall=0.49,
F1 =0.61) and RF (AUC=0.93, Recall=0.49, F1 =0.61). This also
happened in the shallow aquifer as shown in the descending order: ANN
(AUC=1, Recall=1.00, F1 =1.00), SVM (AUC=0.84, Recall=0.34,
F1 =0.28), RF (AUC=0.93, Recall=90, F1 =0.79). Based on the classi­
fication performance (training dataset) result, by investigating preces­
sion matrices ANN showed the sign of overfitting with very high
performance in the train set and very low performance in the test set.
Commonly, the overfitting in the ANN model is found when ANN al­
gorithms work with a small dataset (Rao et al., 2018). The result can
indicate that ANN was not an appropriate model for the modeling pro­
cess in this study. However, the quality of the model cannot be estimated
by just using only the training dataset because it was considered only by
the data used to generate the model (Henseler and Sarstedt, 2013).
Therefore, the classification performance (test dataset) represents the
quality of the model. To evaluate the appropriate model, the classifi­
cation performance (test dataset) needs to be mainly considered (Bindal
and Singh, 2019). As shown in Table 3, the best deep aquifer probability
model is RF (AUC=0.72, Recall=0.61, F1 =0.69) compared with SVM
(AUC=0.69, Recall=0.32, F1 =0.38) and ANN (AUC=0.65,
Recall=0.14, 0.18). In addition, in the shallow aquifer, RF (AUC=0.81,
Recall=0.79, F1 =0.68) also the best model following by ANN
(AUC=0.78, Recall=0.75, F1 =0.70) and SVM (AUC=0.79,
Recall=0.48, F1 =0.39). The result of prediction performance indicated
that the RF had the best performance compared to those of SVM and
ANN in both the deep and shallow aquifers.
In addition, Taylor’s diagrams were conducted to describe a model’s
performance (Rahmati et al., 2019). The figure of the models’ perfor­
mance confirmed that the RF was the appropriate model to classify total
As in groundwater in the study area as presented in Fig. 5. Based on the
criteria of Taylor’s diagram, the RF had the highest correlation with the
observed total As probability and had the lowest correlation compared
to those values of the SVM and ANN models (Taylor, 2001).
The prediction performance by validation with actual field data as
shown in Table 4 revealed that RF had the lowest RMSE in both deep and
shallow aquifers (RMSE = 0.48 and 0.75) compared to those of SVM
(RMSE = 0.73 and 0.76) and ANN (RMSE = 0.67 and 0.84). Similar to
Table 2
Spearman’s correlation with Physical and hydrochemical parameters in both
deep and shallow aquifers.
Parameters Deep aquifer Shallow aquifer
MAE, RF had the lowest MAE in both deep and shallow aquifers (MAE =
0.38 and 0.57) compared to those of SVM (MAE = 0.54 and 0.57) and
ANN (MAE = 0.46 and 0.71).
The result indicated that the RF model was the appropriate model to
create a groundwater pollution risk map of total As rather than SVM and
ANN. The result is also supported by many previous studies that RF al­
gorithms have high performance and stable evaluation to predict data in
the groundwater modeling field (Liu et al., 2019; Podgorski et al., 2020;
Wang et al., 2021).
3.3. Uncertainty evaluates
The Quantile Regression (QR) technique was used to evaluate the
uncertainty for each ML model. To determine the uncertainty of ML
models, this study applied only the testing data to carry out. Two sta­
tistics approaches consist of prediction interval coverage probability
(PICP) and mean prediction interval (MPI) that were suggested by
Rahmati (Rahmati et al., 2019). MPI was the average value from the
prediction interval’s width, and the fewer values of MPI indicate the
lower uncertainty for each model. PICP was the probability that the
calculated within the prediction intervals, and the greatest value of PICP
indicates less uncertainty in each model.
The result of PICP in the deep aquifer showed that Random Forest
(RF) provided the lowest uncertainty value (PICP=0.20) compared to
that of Support Vector Machine (SVM) (PICP=0.16) and Artificial
Neural Networks (ANN) (PICP=0.05) (Table 5). In the case of shallow
aquifer, RF also provided the lowest uncertainty value (PICP=0.34)
compared with that of SVM (PICP=0.23) and ANN (PICP=0.25)
(Table 5). However, because the PICP evaluation from the three models
were indicate the uncertainty value of each model, there was no need to
use the MPI value to compare the uncertainty of each model (Rahmati
et al., 2019). When evaluating uncertainty in the models in case the PICP
was very clearly indicated the uncertainty value. Therefore, the PICP
was a more important measurement uncertainty indicator than the MPI
(Dogulu et al., 2015). However, the MPI will be used as a secondary
indicator in the case when the models provided close PICP values, a
model with a lower MPI will be considered as a low uncertainty model
(Muthusamy et al., 2016). According to QR results, the RF model pro­
vided the lowest uncertainty value compared to SVM and ANN in both
shallow and deep aquifers. The RF was the appropriate model to predict
the total As risk area based on the prediction performance and uncer­
tainty assessment in both deep and shallow aquifers. The spatial map of
probability map showed that RF and other models in Fig. 6.
3.4. Risk map assessment

Physical DEM, Silt loam, Forest, DEM, Sandy loam, Silt loam, Clay Arsenic concentrations were found in the range of 0.3–500 µg/l with
parameters Quaternary, Granite loam, Agricultural(fields), Gr, Qc,
an average of 12.85 µg/l, which was higher than the groundwater
Qmc
Chemical EC, pH, TDS, TTH, EC, pH, TDS, TTH, drinking standard (WHO, 2018). The other heavy metals in the shallow
parameters Ca, Mg, F, HCO3 Ca, Mg, Na, K, Fe, Cl aquifer had a wide range of concentrations. Cadmium, Cr, Cu, Hg, Mn,
F, HCO3, SO4, NO3, Ni, Pb, Se, Zn had a wide range from 0.4 to 0.6 µg/l, 2.40–40 µg/l,
Cd, Cr, Cu, Hg, Mn, 3–500 µg/l, 0.1–700 µg/l, 5– 18,000 µg/l, 1–180 µg/l, 0.70–60 µg/l,
Ni, Pb, Se
0.3–160 µg/l, and 5–1900 µg/l respectively. Metals that were detected

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N. Sumdang et al. Ecotoxicology and Environmental Safety 253 (2023) 114665

Fig. 5. Taylor’s diagram for a) the deep aquifer and b) the shallow aquifer.

to cause diabetic, gastro-intestinal, renal, and neurological diseases, as

Table 4 well as cardiovascular disease. Furthermore, repeated exposure to As
Validation model with field data during 31 August – 1 September 2019.
has been related to a variety of cancers. In addition, the ingestion risk
RMSE MAE from As was found to be higher than the dermal uptake risk (Çelebi et al.,
SVM RF ANN SVM RF ANN 2014a, 2014b). Because of the As toxicity, monitoring strategies and risk
Deep 0.73 0.48 0.67 0.54 0.38 0.46
estimation are required to locate the risk area. The present study used
Shallow 0.76 0.75 0.84 0.57 0.57 0.71 risk maps from the RF model with population density and water con­
sumption to indicate As contamination in groundwater regions. The
percentage of groundwater pollution risk area in the deep aquifer shown
Table 5 in Table 6 has areas in very high-level, including Sattahip and Ban Khai
Uncertainty analysis of SVM, RF, and ANN of the deep and shallow aquifers. districts of 71.9% and 28.1%, respectively. Ban Chang district was
classified as the high-level area (15.6%). The district classified as the
Models Train Test
moderate level included Si Racha, Bang Lamung, Mueang Rayong, Pluak
Deep PICP MPI PICP MPI Daeng, Nikhom Phatthana of 73.89%, 16.87%, 3.48%, 0.57%, and
SVM 0.27 0.16 0.16 0.15 0.13%, respectively. The very low-level districts were Nong Yai and Ban
RF 0.53 0.49 0.20 0.13 Bueng (2.77% and 1.52%, respectively).
ANN 0.69 1.3E-4 0.05 6.075E-10
The percentage of groundwater pollution risk area in the shallow
Shallow
SVM 0.50 0.37 0.23 0.39 aquifer was shown in Table 7, revealing that Mueang Rayong and Ban
RF 0.58 0.44 0.34 0.27 Khai districts were classified in the very high-risk level of 99.27% and
ANN 0.86 8.7E-05 0.25 1.63E-10 0.73%, respectively. For the high-level area, there was only Nikhom
Phatthana district covering 3.65%. There are two districts classified as
the moderate level consisting of Si Racha and Pluak Daeng of 41.73%
to be above the groundwater standard were Cu, Mn, Ni, Pb, and Se
and 0.29%, respectively. Ban Chang district was grouped in the low-
(WHO, 2018).
level area (0.94%). Lastly, Bang Lamung, Sattahip, Nong Yai, and Ban
Arsenic contamination in the Rayong groundwater basin appeared to
Bueng districts areas were classified in the very low-level of 8.07%,
be a potential risk, which has been mentioned in many studies (Pipat­
4.99%, 2.54%, and 1.40%, respectively.
tanajaroenkul et al., 2018; Boonkaewwan et al., 2020). Arsenic is known

8
N. Sumdang et al. Ecotoxicology and Environmental Safety 253 (2023) 114665

Fig. 6. The probability map in the deep aquifer derived from a) RF, b) SVM, c) ANN and the probability map in the shallow aquifer derived from d) RF, e) SVM and
f) ANN.

Table 6 Table 7
Percentage of groundwater pollution risk area in the deep aquifer. Percentage of groundwater pollution risk area in the shallow aquifer.
Districts Very high High Moderate Low Very low Districts Very high High Moderate Low Very low

Pluak Daeng 0.00 0.00 0.57 32.76 22.57 Pluak Daeng 0.00 0.00 0.29 9.29 26.52
Mueang Rayong 0.00 0.00 3.48 0.10 22.31 Mueang Rayong 99.27 91.62 55.22 29.76 10.66
Nong Yai 0.00 0.00 0.00 0.00 2.77 Nong Yai 0.00 0.00 0.00 0.00 2.54
Ban Chang 0.00 15.58 0.00 0.79 9.14 Ban Chang 0.00 0.00 0.00 0.94 8.54
Ban Khai 28.13 77.26 5.06 26.14 14.89 Ban Khai 0.73 4.73 1.22 0.94 18.80
Sattahip 71.87 7.16 0.00 0.02 5.03 Sattahip 0.00 0.00 0.00 0.00 4.99
Si Racha 0.00 0.00 73.89 5.94 7.44 Si Racha 0.00 0.00 41.73 16.95 8.35
Ban Bueng 0.00 0.00 0.00 0.00 1.52 Ban Bueng 0.00 0.00 0.00 0.00 1.40
Nikhom Phatthana 0.00 0.00 0.13 33.39 6.23 Nikhom Phatthana 0.00 3.65 1.55 42.12 11.23
Bang Lamung 0.00 0.00 16.87 0.87 8.10 Bang Lamung 0.00 0.00 0.00 0.00 8.07

9
N. Sumdang et al.
The result showed that Sattahip and Ban Khai districts (the north part
of Rayong Province) have the largest number of people exposed to As
contamination with a very high risk level, followed by Ban Chang dis­
trict which had a high-risk level of exposure. Other districts that might
have people exposed to As contaminated in the deep aquifer were in the
descending order as follows: Si Racha, Bang Lamung, Mueang Rayong,
Pluak Daeng, and Nikhom Phatthana district. Based on the risk map, the
exposure of local people with As contaminated in the shallow ground­
water aquifer mostly found in the south path in Rayong groundwater
basins such as Mueang Rayong and Ban Khai districts which had a very
high risk level. Following Nikhom Phatthana district (high-risk expo­
sure), Si Racha and Pluak Daeng districts also had a moderate risk level.
From Nilkarnjanakul et al. (2022), the previous study indicated that oral
exposure is the most risky exposure pathway in Ban Khai district. The
highest HQ oral level of arsenic observed in the adult group was 15.30,
which is ten times the average risk level of 1.47. Moreover, the
high-level health risk assessment area in Ban Khai district came from Gr
groundwater. This can be related to the risk map in this study and in­
dicates that in Ban Khai district, arsenic exposure has a very high-risk
assessment level in the deep aquifer.
In summary, the risk map for the deep aquifer appeared to have more
risk in the northern part of Rayong groundwater basin whereas in the
shallow aquifer it appears to have high risk in the southern part of the
Fig. 7. Groundwater pollution risk map of As contamination in a) the deep
aquifer and b) the shallow aquifer.
10
Ecotoxicology and Environmental Safety 253 (2023) 114665
Rayong groundwater basin as shown in Fig. 7. Based on various types of
land use in the Rayong groundwater basin including industrial sites,
agricultural areas, and urban areas, particularly, the landfill in the
Mueang District that is close to the estuary of the groundwater basin
(Boonkaewwan et al., 2021). As highly concentrated in industrial sites
due to anthropogenic activity (Çelebi et al., 2014a, 2014b). Therefore,
the risk areas of the shallow aquifer could be affected by anthropogenic
activity in the study area, such as landfills, agricultural areas, and in­
dustrial sites.
Given these results, it is critical to limit additional contamination of
potential drinking water sources. Therefore, groundwater monitoring
should be carried out in the Rayong groundwater basin. Moreover,
decision-makers should plan an appropriate policy following the risk
area of As risk map to locate an area suitable for installing a filter tank
that has oxide mineral material for remediation and treat As contami­
nation in groundwater before use (Aredes et al., 2012). Furthermore, the
As groundwater risk map can be used as reference information to warn
the people in the study area this will enhance the public willingness to
procure groundwater before drilling groundwater well (Das et al.,
2019).
4. Conclusions
The correlation analysis shows mechanisms in the groundwater
environment. The correlation result indicated that the sources of As in
this study area were caused by both natural and anthropogenic sources.
The results of the models’ classification and prediction performances
and uncertainty evaluation results indicated that the RF models had the
highest model performance and lowest uncertainty compared to the
SVM and ANN models. Therefore, the RF was the most suitable model
for AS contamination assessment in the Rayong groundwater basin
compared to SVM and ANN. The RF model’s risk map shows that the
northern and middle parts of the Rayong groundwater basin had a high
risk of people being exposed to As contaminated in deep aquifers. On the
contrary, the shallow aquifer indicates that the southern part of the
Rayong groundwater basin has a higher chance that people are exposed
to As in groundwater, which could be related to anthropogenic activities
in the Mueang District, which is close to the estuary of the Rayong
groundwater basin.
Therefore, long-term groundwater monitoring should be carried out
intensively in the Rayong groundwater basin. The process of this
research can be used to further study other groundwater aquifers that
are contaminated and increase the effectiveness of groundwater quality
management. Moreover, the outcome of this study can be used by the
government to manage groundwater resources and protect the envi­
ronment in the study area. Moreover, the people in the area can use the a
groundwater risk map as reference data to increase public willingness to
procure uncontaminated groundwater before drilling a new well. The
government can propose a suitable policy to procure uncontaminated
groundwater and encourage sustainable groundwater management in
the study area more effectively. Due to the industrial estate being built
as part of the EEC project, this area will experience significant ground­
water demand in the upcoming years. Overall, this study helps both
government and non-government sectors understand the risk assessment
of As-contaminated groundwater and protect groundwater resources.
CRediT authorship contribution statement
Narongpon Sumdang: Software, Validation, Formal analysis,
Investigation, Visualization, Data curation, Writing – original draft.
Srilert Chotpantarat: Conceptualization, Methodology, Validation,
Resources, Formal analysis, Investigation, Writing – review & editing,
Project administration, Funding acquisition, Data curation. Kyung Hwa
Cho: Writing – review & editing, Supervision. Nguyen Ngoc Thanh:
Data curation. All authors have read and agreed to the published version
of the manuscript.
N. Sumdang et al.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Data availability
Data will be made available on request.
Acknowledgments
The authors are very grateful for the 90th Year Chulalongkorn Uni­
versity Scholarship. We acknowledge financial supports from the Grant
for Thailand Science Research and Innovation Fund Chulalongkorn
University (CUFRB65_dis(2)_090_23_20). We are grateful for the thor­
ough reviews of anonymous reviewers. Their valuable comments
significantly improved the earlier draft of this article.
Appendix A. Supporting information
Supplementary data associated with this article can be found in the
online version at doi:10.1016/j.ecoenv.2023.114665.
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