Environmental Technology & Innovation 20 (2020) 101043

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Environmental Technology & Innovation

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

Heavy metal contamination trends in surface water and

sediments of a river in a highly-industrialized region
∗ ∗
Hong-Giang Hoang a,b , Chitsan Lin a,b , , Huu-Tuan Tran a,c , Chow-Feng Chiang d , ,
Xuan-Thanh Bui e,f , Nicholas Kiprotich Cheruiyot b , Chien-Chuan Shern b ,
Chia-Wei Lee g
a
College of Maritime, National Kaohsiung University of Science and Technology, Kaohsiung 81157, Taiwan, ROC
b
Department of Marine Environmental Engineering, National Kaohsiung University of Science and
Technology, Kaohsiung 81157, Taiwan, ROC
c
Faculty of Applied Science-Health, Dong Nai Technology University, Bien Hoa, Dong Nai 810000, Viet Nam
d
Department of Public Health, China Medical University, Taichung 40402, Taiwan, ROC
e
Key Laboratory of Advanced Waste Treatment Technology, Vietnam National University Ho Chi Minh (VNU-HCM), Linh Trung
ward, Thu Duc district, Ho Chi Minh City 700000, Viet Nam
f
Faculty of Environment and Natural Resources, Ho Chi Minh City University of Technology (HCMUT), Ho Chi Minh
City 700000, Viet Nam
g
Department of Safety, Health, and Environmental Engineering, National Kaohsiung University of Science and
Technology, Kaohsiung 82445, Taiwan, ROC

article info a b s t r a c t

Article history: Surface water and sediment samples from the most contaminated river in Taiwan,
Received 13 April 2020 Houjing River, were collected for five years (2015 to 2019) and from five locations
Received in revised form 9 July 2020 to study the contamination trends of eight heavy metals (As, Cd, Cr, Cu, Hg, Pb, Ni,
Accepted 10 July 2020
and Zn). Five locations along the river were picked based on their potential of being
Available online 15 July 2020
contaminated by nearby industrial activities. The monitoring data, geo-accumulation in-
Keywords: dex (Igeo ), contamination factor (CF ), modified degree of contamination (mCd), pollution
Heavy metal pollution load index (PLI), and metal index (MI) were used to provide a detailed assessment
Synergistic indexes of the heavy metal contamination. Demin (L3) and Chuwai (L4), two sampling sites
Modified degree of contamination (mCd) close to the Nanzih Export Processing Zone (NEPZ) discharge points, were the most
Contamination factor (CF ) contaminated. The most contaminated periods were 2015–2016 and 2018–2019 for
Geo-accumulation index (Igeo) surface water and sediment samples, respectively. The surface water showed signs of
Metal index (MI)
heavy metal contamination in 2016 with mCd > 1.5. For the sediment samples, the
heavy metal concentration fingerprints for the five years were similar. This implied
that the natural attenuation process was not adequate, and treatment technologies are
required to improve sediment quality. This study provides a basis for comprehensive risk
assessments and integrated environmental management measures for the river’s surface
water and sediment quality. Also, it would contribute to a more inclusive evaluation of
heavy metal contamination in global rivers.
© 2020 Elsevier B.V. All rights reserved.

∗ Corresponding authors.
E-mail addresses: ctlin@nkust.edu.tw (C. Lin), amur.chiang@gmail.com (C.F. Chiang).

https://doi.org/10.1016/j.eti.2020.101043
2352-1864/© 2020 Elsevier B.V. All rights reserved.
2 H.-G. Hoang, C. Lin, H.-T. Tran et al. / Environmental Technology & Innovation 20 (2020) 101043

1. Introduction

Heavy metal contamination may originate from natural sources, for example, rock weathering or from human-made
activities, including ore mining, metal-related factories, fertilizer, and pesticide usage in agriculture (Hu et al., 2015; Ji
et al., 2018). The heavy metals from anthropogenic sources are more mobile and bioavailable than those present in their
natural mineral form and hence pose greater human and environmental health risks (Benson et al., 2018; Saleem et al.,
2015; Tessier and Campbell, 1987; Zhu et al., 2015). Therefore, the extent of heavy metal contamination has increased
significantly with rapid industrialization (Ahmed et al., 2015; Vu et al., 2017b). The heavy metals released from the various
industrial activities eventually end up in the environment, especially surface waters of urban areas (Khadse et al., 2008).
Li et al. (2019) assessed the trend of heavy metal contamination in rivers and lakes around the world from 1970 to
2017. They reported an increasing trend for Fe, Mn, Ni, Cu, Cr, and Cd and a decreasing trend for Zn and Pb, with the
mean dissolved concentration higher in Asia than in Europe. Different regions had different heavy metal contamination
sources; for example, mining and manufacturing were identified as the critical sources in Asia. The Houjing River is one of
these heavily-polluted rivers in Asia that flows through a highly industrialized area in Kaohsiung city (the second-largest
city in Taiwan) and receives effluents from various industries (Vu et al., 2017a). For instance, the river receives discharges
from several industrial parks, including Renwu Industrial Parks, Dashe Industrial Parks, and Nanzih Export Processing
Zone (NEPZ) (Chen and Wu, 1995; Vu et al., 2017a). These industrial parks house a lot of metal-related plants such as
metal surface treatment and computer chip manufacturing factories, which pose as potential heavy metal contamination
sources for the river.
Before stricter environmental regulations in Taiwan, the Houjing River had notable records of heavy metal contam-
ination due to illegal discharge (Jiang et al., 2015; Lin et al., 2010). Vu et al. (2017a) reported that the sediment levels
of the river had severe contamination levels, with Cu having the highest average concentration of 432.29 mg/kg dry
wt. This concentration is twice the upper standard values of several sediment quality guidelines, including the Taiwan
Environmental Protection Agency (TEPA) and the Canadian council of ministers of the environment (CCME). However, that
study was conducted for a short period, November 2015 to June 2016, and the contamination trends were not evaluated.
It is important to study the spatial and temporal trends of heavy metal contamination in order to provide a basis for
thorough ecological and human health risk assessments.
Spatial and temporal patterns have been studied in other regions in Asia. For instance, heavy metal contamination in
Yangtze River (Gao et al., 2016), marine sediments along with river estuaries and coastal areas in the southeast part of
India (Gurumoorthi and Venkatachalapathy, 2016; Veerasingam et al., 2014), and in South Korea’s southern coast (Cho
et al., 2015). Their results identified key contamination sources, seasonal trends, spatial heavy metal distribution, and
historical environmental trends. These have provided baseline data for effective heavy metal contamination monitoring
programs in the respective regions.
Therefore, an exhaustive evaluation of spatial and temporal trends of heavy metal contamination in the Houjing River
from 2015 to 2019 is presented in this study. Aside from the heavy metal concentrations in the surface water and
sediment, geo-accumulation index (Igeo ), contamination factor (CF ), modified degree of contamination (mCd), pollution
load index (PLI), and metal index (MI) were also employed in the study. The combination of the individual (Igeo and CF )
and synergistic (mCd, PLI, and MI) assessments of the eight heavy metals will provide a more comprehensive view on
the heavy metal contamination status in the Houjing River. Five locations along the river were picked based on their
potential of being contaminated by nearby industrial activities. The sources of contamination were discussed. The results
from this study will provide an informative background for future ecological and human health risk assessments and
the development of integrated management measures for the river’s surface water and sediment quality. In addition, our
results would contribute to the attainment of sustainable development goals (SDGs), especially SDG 3, 6, 11, and 14, and
contribute to a more comprehensive evaluation of heavy metal contamination in global rivers.

2. Materials and methods

2.1. Studied area

The Houjing River is situated at the coordinates 22◦ 69′ 21.63′′ N - 22◦ 73′ 17.74′′ N latitude and 120◦ 25’74.36’’ E -
120◦ 33’74.70’’ E longitude and located in Kaohsiung city, south of Taiwan. The river originates from Dashe District and
Renwu District with the two creeks merging at Kaohsiung Metropolitan Park (formerly Si Cing Bu landfill), as shown in
Fig. 1. It flows through several industrial zones, then farmlands and fish-farming areas before flowing into the Taiwan
Strait. These industrial zones include Dashe Industrial Parks, Renwu Industrial Parks, and Nanzih Export Processing Zone,
which have many metal-related industries. The treated wastewater from these industrial zones is discharged to the river.

2.2. Sample collection

Five locations (L1 — Jingjian, L2 — Renwu, L3 — Demin, L4 — Chuwai, and L5-– Dehuei) were selected for water and
sediment sampling to evaluate the heavy metal contamination in the Houjing River (Fig. 1 & Table S1). From the upstream,
L1 was located close to the discharge point of the Dashe Industrial Park, where the main manufacturing industries are
 H.-G. Hoang, C. Lin, H.-T. Tran et al. / Environmental Technology & Innovation 20 (2020) 101043 3

Fig. 1. The studied area and sampling sites (Google map 2020).

petrochemical and electroplating industries. The L2 sampling site was close to Renwu Industrial Park, which has a high
concentration of petrochemical and metal-related industries (Kaewlaoyoong et al., 2018). L3 and L4 were near NEPZ
discharge points, which has several semiconductor packaging and metal surface processing industries (Yeh et al., 2020).
The last sampling point, L5, was located at the downstream of the three industrial parks. These characteristics were the
basis for selecting these five sampling points.
A total of 90 sediment samples and 90 surface water samples were collected in five years from 2015 to 2019 within 18
sampling seasons. An Ekman Dredge device was used to collect the sediment samples. These samples were then stored
in polyethylene bags. Surface water samples were taken by bucket then stored in plastic bottles. All samples were kept
at 4 ◦ C until analysis. The sampling procedures were referenced from surface water sampling guidelines (USEPA, 2016)
and sediment sampling guidelines (USEPA, 2014) of the United States Environmental Protection Agency (USEPA).

2.3. Analysis of heavy metals

The procedure for analyzing heavy metal concentrations in the surface water and sediment samples was carried out
according to Taiwan Environmental Protection Administration (TEPA) method NIEA M318.01C (TEPA, 2012) for Hg and
USEPA method 6010C (USEPA, 2000) for the other metals. Our previous research has the details of these procedures
(Vu et al., 2017a). Briefly, sediment samples were mixed homogeneously and lyophilized using a freeze dryer (Eyela
FDU-1200, Tokyo Rikakikai, Japan) at −50 ◦ C and 10 Pa for 24 h. Afterward, an acid mixture including 1 ml HNO3 and
3 ml HCl and sediment samples were mixed, processed with microwave digestion system (Topex, Preekem, Shanghai,
China), and purified by Whatman glass fiber filter paper before analysis. The water samples were acid digested with
HNO3 acid and then purified by Whatman glass fiber filter paper before analysis. The concentrations of heavy metals in the
surface water and sediments (except Hg) were analyzed by an Inductively Coupled Plasma-Optical Emission Spectrometer
instrument (ICP-OES, Optima 2100 DV, PerkinElmer, USA). A mercury analysis instrument (NIC MA-2, Systematic, Taiwan)
was employed to analyze the Hg concentration in the samples directly.
Quality assurance (QA) and quality control (QC) were strictly implemented following USEPA guidelines to ensure the
accuracy of the analysis. The detailed analysis and QA-QC processes were shown in our previous study (Vu et al., 2017a;
Yeh et al., 2020).

2.4. Heavy metal contamination assessments

A combination of individual and synergistic methods was employed to have a complete assessment of heavy metal
contamination trends. Geo-accumulation index (Igeo ) and contamination factor (CF ), were used for the individual assess-
ment of heavy metal contamination, while modified degree of contamination (mCd) index, pollution load index (PLI), and
metal index (MI) were chosen for the synergistic evaluation of heavy metal contamination in water and sediment.
Igeo and CF were first introduced by Muller (1979) and Hakanson (1980), respectively. Igeo and CF were calculated
based on the ratio of heavy metal concentration in the environment and the reference values. In this study, the average
shale values were used as the reference values to calculate Igeo and CF for sediment. Taiwan’s irrigation standard ((TEPA,
1992)) was used as the reference values to calculate CF for water (Table 1). The calculation results of Igeo and CF will
support and confirm each other to provide reliable individual assessments.
The mCd and PLI indexes were used to aggregately assess the contamination degree of all heavy metals relative to
their surface water quality and sediment references based on CF index (Abrahim and Parker, 2008); (Islam et al., 2015);
(Withanachchi et al., 2018). PLI presents the overall contamination status with three contamination levels, while mCd
provides seven contamination levels, as shown in Table 1.
MI was applied to assess the quality of the river’s sediment based on the ratio of heavy metal concentration in sediment
samples to the upper allowable concentration in TEPA’s sediment quality guideline (TEPA, 2010). While mCd and PLI show
4 H.-G. Hoang, C. Lin, H.-T. Tran et al. / Environmental Technology & Innovation 20 (2020) 101043

Table 1
Surface water and sediment quality assessment indexes.
Indexes Equations Classification Contamination degree References
( Csi
)
Igeo = log2 Igeo < 0 Uncontaminated
1.5Cb
i
where: Csi is the heavy metal 0 ≤ Igeo < 1 Uncontaminated to moderately
measured concentration in contaminated
Igeo Muller (1979)
sediment; 1 ≤ Igeo < 2 Moderately contaminated
Cbi is the concentration of
2 ≤ Igeo < 3 Moderately to heavily
heavy metals in average shale
contaminated
values (Turekian and
Wedepohl, 1961)a 3 ≤ Igeo < 4 Heavily contaminated
4 ≤ Igeo < 5 Heavily to extremely
contaminated
Igeo ≥ 5 Extremely contaminated
Csi
CFi = where: Csi is the heavy metal CF < 1 Low degree
Cb
i Hakanson
CF measured concentration in water and
1 ≤ CF < 3 Moderate degree (1980)
sediment; Cbi is the reference values (Cbi =
Taiwan’s irrigation standard (TEPA, 1992)b for 3 ≤ CF < 6 Considerable degree
water; Cbi = concentration of heavy metals in
average shale values for sediments (Turekian CF ≥ 6 Very high degree
and Wedepohl, 1961)a )
mCd < 1.5 Uncontaminated
∑n 1.5 ≤ mCd < 2 Slightly contaminated
mCd = 1n i=1 CFi
2 ≤ mCd < 4 Moderately contaminated Abrahim and
mCd where: CF is the
Parker (2008)
contamination factor 4 ≤ mCd < 8 Moderately to heavily
contaminated
8 ≤ mCd < 16 Heavily contaminated
16 ≤ mCd < 32 Severely contaminated
mCd ≥ 32 Extremely contaminated
PLI = (CF 1 x CF 2 x CF 3 x. . . x PLI = 0 Perfection Withanachchi
PLI CFn )1/n where: CF is the PLI < 1 Baseline level et al. (2018)
contamination factor Islam et al.
PLI > 1 Contaminated (2015)
Csi
MI < 0.3 Very pure
∑n
MI = i=1 UACi
where: Csi is the heavy metal 0.3 ≤ MI < 1 Pure
Withanachchi
MI measured concentration in 1 ≤MI < 2 Slightly affected et al. (2018)
sediment; UAC i is the upper
allowable concentration in 2 ≤ MI < 4 Moderately affected
(TEPA)’s sediment quality 4 ≤ MI < 6 Strongly affected
guideline (TEPA, 2010)c
MI ≥ 6 Seriously affected
a
Cbi values (mg/kg): As: 13, Cd: 0.3, Cr: 90, Cu: 45, Pb: 20, Ni: 30, Zn: 95, Hg: 0.4 (Turekian and Wedepohl, 1961).
b
Cbi values (mg/L): As: 0.05, Cd: 0.01, Cr: 0.1, Cu: 0.2, Pb: 0.1, Ni: 0.2, Zn: 2, Hg: 0.002 (TEPA, 1992).
c
UAC i values (mg/kg): As: 33, Cd: 2.5, Cr: 233, Cu: 157, Pb: 161, Ni: 80, Zn: 384, Hg: 0.87 (TEPA, 2010).

the synergistic contamination levels of the heavy metals in sediment compared to the average shale values, MI represents
the synergistic contamination levels of the heavy metals in sediment compared to the upper limits of the standard. MI
offers a more appropriate assessment of the local situation. The equations and classifications of these indexes are shown
in Table 1.

2.5. Statistical analysis

SPSS software (version 22) was used for statistical analysis in this study. The correlation of the heavy metal contami-
nation between sampling locations and sampling frequency based on measurement concentration and index calculation
results were analyzed. The correlations were assessed as significant when Pearson values, p, were < 0.05.

3. Results and discussion

3.1. Heavy metal concentration in surface water samples

All the studied heavy metals were detected in the surface water samples in the five years (2015–2019) and at the five
sampling locations (L1–L5), as shown in Fig. 2. Cu, Pb, Ni, Zn, and Cr were the dominant elements in all the locations
 H.-G. Hoang, C. Lin, H.-T. Tran et al. / Environmental Technology & Innovation 20 (2020) 101043 5

Fig. 2. The (a) spatial and (b) temporal variation of heavy metal concentration in the Houjing River water samples (mg/L).
6 H.-G. Hoang, C. Lin, H.-T. Tran et al. / Environmental Technology & Innovation 20 (2020) 101043

Fig. 3. The (a) spatial and (b) temporal variation of the modified degree of contamination (mCd) values in surface water.

and years. These are common heavy metals in most production and manufacturing activities, including metal surface
processing, semiconductor packaging, chemical, and petrochemical industries (Gakwisiri et al., 2012; Mirbagheri and
Hosseini, 2005). Most of these industries are present in NEPZ, Dashe, and Renwu Industrial Parks, where the Houjing
River flows through (Vu et al., 2017a; Yeh et al., 2020). Vu et al. (2017a) used positive matrix factorization (PMF) to
identify the potential sources of heavy metal contamination in the river and concluded that the industries along its banks
were the main sources. Yeh et al. (2020) also concluded that heavy metal contamination in the river was mainly from the
abundance of metal-related manufacturing activities in the nearby industrial parks. Thus, their wastewater discharges are
potential sources of heavy metal contamination in the river.
The heavy metal fingerprints for the locations (Fig. 2a) were compared and linked to their potential sources. The L1
and L2 fingerprints differed from each other, indicating that their contamination sources were different. L1 was located
near Dashe Industrial Park, where many plastic manufacturers and some electroplating factories are present (Yeh et al.,
2020). This may be the reason for higher Zn and Cd concentrations in L1 than in other locations (Hasan et al., 2007) (as
shown in Table S2). L2 was located near Renwu Industrial Park, which has several petrochemical and some metal-related
industries (Kaewlaoyoong et al., 2018), which are potential sources of heavy metal contamination in that site. L3 and L4,
located downstream, shared similar fingerprints, implying that the contamination in L3 and L4 were from similar sources.
Most of the heavy metals, including Cr, Cu, Pb, Ni, and Hg, had their highest concentrations in L3 and L4, which were
located near NEPZ’s wastewater discharge points. NEPZ houses semiconductor packaging and metal surface processing
 H.-G. Hoang, C. Lin, H.-T. Tran et al. / Environmental Technology & Innovation 20 (2020) 101043 7

factories (Yeh et al., 2020), whose wastewater discharges could be sources of those heavy metals (Al-Saydeh et al., 2017;
Venkateswaran et al., 2007; Yeh et al., 2020). Besides, L1 and L2, located upstream, shared different fingerprints from both
L3 and L4, suggesting that the heavy metal contamination contribution from the upstream was insignificant. This could be
due to lower heavy metal concentrations at L1 and L2. However, L5, located further downstream, had similar fingerprints
to L3 and L4; implying upstream heavy metal contamination from L3 and L4. In other words, the contamination at L3 and
L4, with high concentrations, affected the heavy metal concentration at L5.
The annual average values of heavy metal concentrations are presented in Fig. 2b. Most of the heavy metal concentra-
tions (except for Ni) reached their highest values in 2016 and 2017. The average heavy metal concentrations in L3 had
the highest positive correlation (p < 0.01) with the average concentrations for these years (Table S3). This implies that
the wastewater discharge from NEPZ was a significant source of heavy metal contamination in the Houjing River during
2016 and 2017. In addition, the heavy metal concentration trends varied over the five-year duration. This may be due
to illegal discharges, annual precipitation, or change in production activities (Chen et al., 2007; CWB, 2020; Foster and
Charlesworth, 1996; Yuan et al., 2001). Therefore, it was difficult to make any overall conclusions on the trends using
only their concentrations.
Compared with the TEPA irrigation standards (TEPA, 1992) (Table S2), most of the heavy metal concentrations of each
year were lower than permitted levels, except for Pb in 2016 (1.6 times higher) and Hg in 2015 and 2016 (1.9 and 3.4
times higher, respectively). However, when compared with the USEPA freshwater toxicity standard (USEPA, 1999), Cu and
Pb concentrations for each year were 3.0–52.8 times higher than the limit. This indicates that there is room to improve
wastewater discharge management.
It was difficult to draw clear conclusions on the synergistic contamination levels and trends based solely on monitoring
data. This was accomplished by employing mCd. Comparing mCd results with threshold values can provide specific
assessments of heavy metal contamination levels and trends.

3.2. The assessment of heavy metal contamination trends in surface water

To calculate mCd, the reference values of the heavy metals (Cbi ) can be proposed according to various guidelines.
Because the Houjing River supplies water further downstream for agricultural use, in this study, reference values of water
quality for irrigation (TEPA, 1992) were chosen.
According to the mCd values, there were no significant differences in the spatial trend for surface water contamination
at the sampling locations, as shown in Fig. 3a. The heavy metal contaminations in surface water for all the five sampling
locations were below the lowest threshold values (mCd = 1.5). These results were also consistent with the PLI values
(Fig. S1). At all sampling locations, Hg had the highest positive correlation with the mCd values (p < 0.05) (Table S3c),
except for L3, where Ni, Cd, and Cr had a high positive correlation with the mCd values (p < 0.05). Besides, Hg and Pb also
had high correlations with mCd value at L5 (p < 0.05). Therefore, Hg, Pb, Ni, Cd, and Cr are metals of concern for water
contamination.
The temporal trend of the synergistic contamination based on mCd values (Fig. 3b) were in the order: 2016 > 2015 >
2017 > 2019 > 2018. Although five of the eight heavy metals had their highest concentration in 2017 (Fig. 2b), based on
mCd values, 2016 was the year with the highest heavy metal synergistic contamination (mCd = 2.2). This was because the
ratio of Pb, Cu, Ni, and Hg concentrations in the surface water to their reference values were 2–10 times higher in 2016
than in 2017. The annual heavy metal contaminations in surface water, except for 2016, were below the lowest threshold
values (mCd = 1.5). The PLI values (Fig. S1) were also consistent with these results. This indicates that the surface water
of the Houjing River showed signs of contamination and may not be safe for irrigation. Thus, solutions to reduce heavy
metal concentration in the water, such as controlling discharge quality before release into the Houjing River and some
on-site remedies, such as wetland technology, should be applied to improve the water quality. Water quality monitoring
and evaluation programs should continue to be implemented.

3.3. Heavy metal concentration in sediment samples

The heavy metal concentrations in sediment samples are shown in Fig. 4. Cu, Ni, Cr, Pb, and Zn had comparatively
high concentrations. The heavy metal concentrations in sediment are generally higher than in surface water because of
their ability to settle, precipitate, accumulate, and bind strongly to sediments (Schertzinger et al., 2018). Similar to the
heavy metal concentration in the surface water samples, most of the heavy metals had their highest concentrations in L3
and L4, and their lowest concentrations in L5, as shown in Fig. 4a. However, the heavy metal concentration in sediment
did not share the same pattern as that in the surface water. Besides, the correlation between heavy metal concentrations
in surface water and that in sediment was not high, with a Pearson correlation of < 0.553 (p < 0.01) (Table S3d). This
indicates that heavy metal concentration in sediment is not only affected by the current concentration in the surface
water but also historical concentration resulting from settling, accumulation, and binding (Schertzinger et al., 2018).
Fig. 4b shows the five years had similar fingerprints, implying that the sediment quality did not improve over the years.
Thus, the natural attenuation process of the river is inadequate, and the local government should take action to improve
the quality of the river, e.g., by enforcing stringent discharge standards and steeper penalties in addition to employing
sediment cleanup operations. L3 had the highest correlation (p < 0.01) with the average heavy metal concentration in the
8 H.-G. Hoang, C. Lin, H.-T. Tran et al. / Environmental Technology & Innovation 20 (2020) 101043

Fig. 4. The (a) spatial and (b) temporal variation of the heavy metal concentration in the Houjing River sediment samples (mg/kg dry wt.).
 H.-G. Hoang, C. Lin, H.-T. Tran et al. / Environmental Technology & Innovation 20 (2020) 101043 9

Fig. 5. The (a) spatial and (b) temporal variation of the geo-accumulation (Igeo ) index in sediments.
10 H.-G. Hoang, C. Lin, H.-T. Tran et al. / Environmental Technology & Innovation 20 (2020) 101043

sediment samples for all the five years, which implies that L3 was the main contributor to the heavy metal contamination
(Table S3e).
At each sampling site, Cd, Cu, Ni, and Zn concentration values are higher 1.1–5.9 times than the upper value of the
TEPA’s sediment quality guideline (TEPA, 2010) and the effects range median (ERM) values of National Oceanic and
Atmospheric Administration (NOAA)’s (Long et al., 1995). Other heavy metals, such as As, Cr, Pb, and Hg, were less
significant with concentrations lower than the upper limit of those standards.
However, the contamination degree, as well as the synergistic assessment of heavy metal contamination in the
sediment samples, could not be concluded based on these monitoring data. Therefore, assessment indexes Igeo , CF, mCd,
PLI, and MI were employed for individual and synergistic contamination assessment of heavy metals. Based on these
indexes, the contamination trends of heavy metals in the sediment samples were discussed as follows.

3.4. The assessment of heavy metal contamination trends in sediment

The individual assessment by the geo-accumulation index (I geo ) and the contamination factor (CF)
The geo-accumulation index (Igeo ) was employed for the quantitative measurement of an individual heavy metal in the
sediment samples. Unlike monitoring data, the individual indexes take into consideration the background levels of the
heavy metals. Fig. 5a shows the Igeo values of the heavy metals at different sampling locations. Most of the heavy metals
had their highest Igeo at L3 and L4, while L5 had the lowest. Cd had the highest Igeo values in all the sampling locations
(except L4), with all sites having moderately or moderately to heavily contaminated levels of Cd. Meanwhile, all locations
had uncontaminated levels of As, Cr, and Hg, which had Igeo values < 0. Fig. 5b shows the temporal variation of Igeo values
of the heavy metals. Most of the heavy metals had their highest Igeo values in recent years (2018–2019). This indicates
the accumulation of heavy metal in the sediment. For instance, 2019 had heavily contaminated levels of Cd, while 2018
had moderately contaminated levels of Cu.
The conclusions about the spatial and temporal trends of Igeo values are also consistent with the spatial and temporal
trend assessments based on CF values (Fig. S2). Therefore, strategies and technologies to improve sediment quality, such
as washing, thermal extraction, and bioremediation (Mulligan et al., 2001) are necessary and urgent. The government
needs to act promptly to improve the Houjing River sediment quality. In addition to the individual indexes, mCd and PLI
were employed to provide a more comprehensive evaluation of the heavy metal contamination in the river.
The synergistic assessment by the modified degree of contamination (mCd) index, the pollution load index (PLI), and
the metal index (MI)
The mCd index was employed to assess the synergistic contamination of the eight studied heavy metals in the sediment.
The average mCd value of the five locations in five years was 7.1, indicating that the sediment samples of the Houjing
River were moderately to heavily contaminated. The average PLI value in five years of the five sampling locations also
showed that sediment quality was contaminated (PLI = 2.1).
As shown in Fig. 6a, the spatial trends were in the order: L4 > L1 > L3 > L2 > L5. L4 had the highest mCd value
of 8.7, indicating the site was heavily contaminated with heavy metals. While L5 had the lowest mCd of 5.0, presenting
moderately to heavily contaminated level. The PLI calculation results also confirmed that L4 had the highest heavy metal
contamination (Fig. S3a). In all sampling sites, Cd had the highest positive correlation with mCd (p < 0.05) (Table S3f). This
confirms that Cd was the metal of concern in the Houjing River, and minimizing the concentration in discharge sources
should be a priority.
The temporal trend of the mCd and PLI values were in the same descending order: 2018 > 2019 > 2015 > 2017
> 2016 (Fig. 6b & Fig. S3b). In recent years (2018 and 2019), mCd values ranged from 8 to 16, which indicated that
the sediment was heavily contaminated during those periods. The mCd values for sediment from 2015 to 2017 were
moderately to heavily contaminated with heavy metals. Based on mCd and PLI values, the sediment samples of all the
five years and five sampling sites were contaminated with heavy metals. The heavy metal concentration in sediment
samples is affected by physicochemical processes (e.g., adsorption, desorption, and complexation) (Olivelli et al., 2018),
biological uptake (Ogundiran and Fawole, 2017), and meteorological conditions (typhoons and heavy rains) (Tsai et al.,
2016). These processes would affect the temporal trends of heavy metals in the sediment samples.
In addition to mCd and PLI indexes, MI was used to assess the heavy metal contamination level of sediment quality
based on the upper limit values of the TEPA’s sediment quality guideline. The average MI value in the five years and five
sampling sites was 8, indicating that the sediment quality was seriously affected.
As shown in Fig. 7, the spatial and temporal trends were similar to those from the mCd index. The sediment qualities for
L1, L3, and L4 were classified as seriously affected and strongly affected for L2 and L5. 2016 was classified as moderately
affected; 2015, 2018, and 2019 seriously affected; and 2017 strongly affected by heavy metal contamination. This indicated
that compared to the upper values of TEPA’s sediment quality guideline, heavy metals in the sediment sample had
contaminated and negatively affected the sediment quality. Therefore, the sediment quality of the Houjing River needs to
be urgently improved.
In summary, the Houjing River showed signs of heavy metal contamination, especially in sediments. Therefore, there
is a need for urgent and necessary action to clean and protect the water and sediment of the river, especially since the
water is used for irrigation downstream. These actions should be sustainable and in-line with the SDGs. As an emergency
measure, the use of water for irrigation should be stopped to protect human health. Wastewater from the industrial parks
 H.-G. Hoang, C. Lin, H.-T. Tran et al. / Environmental Technology & Innovation 20 (2020) 101043 11

Fig. 6. The (a) spatial and (b) temporal variation of the modified degree of contamination (mCd) values in sediment.

should be strictly monitored by environmental management agencies to meet the standards before discharging, and illegal
discharge should be severely punished. Continuous water and sediment quality monitoring and periodic evaluation of
wastewater discharge standards should be strictly observed. On-site remediation technologies such as wetland technology,
chemical treatment, and dredging (James and Pollman, 2011) should be applied to improve the water and sediment quality
and protect life underwater. Also, further plans to balance economic, social, and environmental aspects of a sustainable
city should be proposed and implemented.

4. Conclusions

The monitoring data, Igeo , CF, mCd, PLI, and MI indexes were used to evaluate heavy metal contamination in the surface
water and sediment of the Houjing River, located in a heavily industrialized area. Cu, Pb, Ni, Zn, and Cr were the five
dominant metals in the water and sediment samples of the Houjing River. Most of the heavy metals had their highest
concentrations and mCd values at L3 and L4, which were located near Nanzih Export Processing Zone (NEPZ) discharge
12 H.-G. Hoang, C. Lin, H.-T. Tran et al. / Environmental Technology & Innovation 20 (2020) 101043

Fig. 7. The (a) spatial and (b) temporal variation of the metal index (MI) in sediments.

points. The heavy metal in the surface water showed signs of contamination. For the sediment samples, heavy metal
contamination was alarming. The heavy metal concentration fingerprints of sediment for the five years were similar,
implying that the natural attenuation process was not adequate to remediate the sediments. Therefore, immediate and
long-term necessary treatment strategies and technologies to enhance surface water and sediment quality are warranted.
The results of this study will be an important basis for proposing solutions to improve the water and sediment quality
as well as for future studies on ecological and human health risk assessment due to heavy metal contamination in the
Houjing River.

CRediT authorship contribution statement

Hong-Giang Hoang: Writing - original draft, Writing - review & editing. Chitsan Lin: Supervision, Visualization. Huu-
Tuan Tran: Methodology. Chow-Feng Chiang: Supervision, Visualization. Xuan-Thanh Bui: Writing - review & editing.
Nicholas Kiprotich Cheruiyot: Writing - review & editing. Chien-Chuan Shern: Project administration, Data curation.
Chia-Wei Lee: Project administration, Data curation.

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.
 H.-G. Hoang, C. Lin, H.-T. Tran et al. / Environmental Technology & Innovation 20 (2020) 101043 13

Acknowledgments

The authors acknowledge the enthusiastic support from the Center of Environmental Analysis Services (CEAS), National
Kaohsiung University of Science and Technology, and financial support of the Advanced Semiconductor Engineering, Inc.

Appendix A. Supplementary data

Supplementary material related to this article can be found online at https://doi.org/10.1016/j.eti.2020.101043.

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