Ecological Indicators 143 (2022) 109347

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Ecological Indicators
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Original Articles

Appraisal of heavy metal pollution in alluvial aquifers. Study case on the

protected area of Ronișoara Forest, Romania
Thomas Dippong a, Maria-Alexandra Hoaghia b, *, Marin Senila b
a
Technical University of Cluj-Napoca, North University Centre at Baia Mare, Faculty of Science, 76 Victoriei Street, 430122 Baia Mare, Romania
b
INCDO-INOE 2000, Subsidiary Research Institute for Analytical Instrumentation, 67 Donath Street, 400293 Cluj-Napoca, Romania

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

Keywords: This study was carried out in a protected area (Ronișoara Forest) in Romania. A combined approach of quality
Alluvial aquifer assessment of alluvial aquifers is employed, by determining the chemistry and applying two pollution indices
Water quality index based on heavy metals concentrations (HPI- Heavy metal Pollution Index and HEI- Heavy metal Evaluation
Durov
Index), a quality assessment index based on specific physico-chemical indicators (WQI- the Water Quality Index)
TIS
and different plots (Durov, Schoeller and TIS-Total Ion Salinity). The study revealed that waters are rich in
Schoeller plots
manganese, calcium, sodium, sulphate, ammonium, manganese, iron, total dissolved solids, dominated by bi­
carbonates. The chemicals’ sources are related to the water–rock interactions and to mine exploitation activities.
Correlations were observed between the electrical conductivity and sulphate, total dissolved solids and sulphate,
and total hardness and electrical conductivity. The results based on the levels of heavy metals pollution indicate
that the studied water samples are characterized by low, medium and high pollution levels, with values ranging
between 0.40 and 234. The WQI scores vary from 8.6 to 54, generally indicating excellent and medium quality,
and low quality for two samples. This research, one of the first in the area, can serve as a reference for the
protection of natural water resources and for the contamination control of alluvial aquifers in the protected area
of Ronișoara Forest.

1. Introduction pathogens’ transition to the population causing a variety of disorders,

Alluvial aquifers are easily explored and thus used as drinking water
sources, however, they are characterized by high vulnerability to nat­
ural pollution through weathering, biologic, ion exchange processes,
precipitation, and anthropogenic pollution caused by diverse industrial,
mining, agricultural and household activities (Rupias et al., 2021).
Therefore, nowadays, >50 % of the world’s population rely on
aquifers as drinking water and irrigation sources, especially the in­
habitants of rural areas (Ibrahim et al., 2019). Because a large portion of
the population in developing nations lacks access to safe drinking water,
they are forced to rely on untreated water from sources such as streams,
rivers, springs, and groundwater or aquifers. Water is not only essential
for survival, but it is also one of the most important vectors of disease
transmission in humans and a leading cause of infant mortality in many
impoverished nations (Adesakin et al., 2020). Pathogenic microorgan­
isms (protozoa, fungus, viruses and bacteria) have been linked to diverse
illnesses that negatively affect human health. Worldwide, at all levels of
economic development, unsanitary water is a pathway of microbial
such as hepatitis, cholera, dysentery; every year, thousands of adults and
children are killed (Adesakin et al., 2020).
The assessment of the quality of groundwater or aquifers (determi­
nation of the biological, hydrological and physico-chemical character­
istics) represents a significant issue for scientists and the population, as
it is a source of drinking water with a direct impact on human health
(Alshehri et al., 2021; Ibrahim et al., 2019). The chemical composition
of groundwater is determined by long-term interactions between
groundwater and the surrounding environment (Liu et al., 2021).
Agricultural wastes (fertilizers, insecticides, pesticides) could cover
large areas, causing negative effects on aquifers and ecosystems through
infiltration (Alshehri et al., 2021; Ibrahim et al., 2019).
Pollution with heavy metals has an impact on the normal functioning
of the groundwater system and on the human body by entering through
various channels and causing serious health issues. The persistence,
difficulty in degradation, concealment, bioaccumulation potential and
toxicity characterize heavy metal pollution, considered as one of the
most significant types of pollution (Long et al., 2021). Due to the toxicity

* Corresponding author.
E-mail address: alexandra.hoaghia@icia.ro (M.-A. Hoaghia).

https://doi.org/10.1016/j.ecolind.2022.109347
Received 7 July 2022; Received in revised form 10 August 2022; Accepted 20 August 2022
Available online 27 August 2022
1470-160X/© 2022 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-
nc-nd/4.0/).
T. Dippong et al. Ecological Indicators 143 (2022) 109347

level, some heavy metals, such as Pb, Hg and Cd, are non-essential to
living organisms, whereas others, such as Fe and Z,n are essential for
maintaining health and growth development. Accumulating in water,
heavy metals are harmful to the biota (Adeyemi and Ojekunle, 2021; Ali
et al., 2022). Natural (active volcanos, atmospheric precipitation,
bedrock erosion, climate, geology) and anthropogenic (mining wastes)
activities enrich the natural water bodies with heavy metals affecting the
hydrochemistry (Liu et al., 2021; Ali et al., 2022). Metal mobility and
bioavailability are influenced by several reactions, such as precipitation
and sorption; therefore, metals exceeding the allowable limits,
becoming toxic, accumulate in living tissues and cause potential damage
to aquatic biota, biodiversity, ecosystems and implicitly to humans
(Adeyemi and Ojekunle, 2021; Krisham et al., 2021).
The quality of aquifers is influenced by the flow direction, hydro­
logical processes, topography features and bedrock composition, which
also has an impact on heavy metal pollution. Nonetheless, water purifies
through precipitation and evaporation (Adeyemi and Ojekunle, 2021;
Arulnangai et al., 2021). The vulnerability of aquifers is related to the
migration of pollutants through the fast flow of the aquifer allowed by
the soil and unconsolidated sediments which characterize the alluvial
aquifers (Rupias et al., 2021). Natural hydrological factors influencing
the quality of aquifers include water effluent supply, flow rate, water
source and contribution of groundwater sources. Water temperature is
Fig. 1. Map of the aquifer levels on the Ronișoara Forests sites.
the main characteristic affecting water quality by catalyzing, stimu­
lating, activating, controlling and inhibiting life in the ecosystem, as
well as guiding the zooplankton migration on a vertical path (Aliu et al., chemical indicators from aquifers localized in the protected area of
2011). The main factors related to the natural structure of aquifers Ronișoara Forest; 2.) Identifying potential anthropogenic pressures
influencing temperature are water depth, turbidity, orientation, geol­ (tourism and pasture activities) in the protected area; 3.) Applying, for
ogy, slope and topographic characteristics (Munteanu et al., 2011). The the first time, a pollution and quality assessment with the help of
quality and chemical composition of soils and geology load the aquifers comprehensive indices, contributing with basic data (water pollution
with quality parameters and heavy metals, characterized by high prevention and environmental risk management) and scientific evidence
toxicity, bioaccumulation and persistency (Cadar et al. 2015; Moldovan regarding the studied aquifers from Ronișoara Forest. The obtained re­
et al., 2020). This way, the depollution of aquifers is difficult (Ibrahim sults will be used in applying conservation rules toward the ecological
et al., 2019). and biological diversity related to the alluvial aquifers situated in the
According to several hydro-geochemical studies on heavy metal protected area. This study is valuable and significant due to the
pollution, such as Krisham et al. (2021) and Long et al (2021), water perspective that it offers on the environmental protection, identifying
resources need to be monitored to maintain safe drinking water sources, diverse and toxic metals in small and high amounts in the studied
and therefore, to be assessed (quality alteration due to the increase of aquifers, which are used as drinking water sources, presuming potential
chemical substances concentrations implies the increase of environ­ health issues through ingestion.
mental and human health risks).
Water decontamination represents an important process that follows 2. Materials and methods
water systems monitorization and prevention. Diverse processes can be
applied, adsorption being one of the most used. Adsorption is a process Ronișoara Forest is situated in a forest massif (the most important
occurring between two phases (solid and liquid). The salt ions are and compact massif from the Romanian side of the Maramureș
adsorbed through chemical bonding and physical interactions. This Depression) between Tisa Superioara and the upper course of Ronișoara
process is related to the interactions between the adsorbent surface and river. Here, a significant habitat of large mammals (bears, wolves, links
guest molecules (Qiu et al., 2022). Natural or synthetic zeolites, indus­ and deer) blossomed. The fauna and flora of this relatively high massif
trial and agricultural wastes or activated carbon are applied in water (600–900 m altitude) is less studied and it deserves special consider­
decontamination, adsorbing different contaminants, such as heavy ation. The protected area of Ronișoara Forest is a forest reservation for
metals, As, NH+ germplasm with a surface of 62 ha, situated on the territory of Rona de
4 , salts, dies (Rashed, 2013; Yao and Yang, 2020).
Hence, the aim of the present study was to assess the quality of al­ Sus village, part of Sighetu Marmatiei forestry. The rich forest is less
luvial aquifers from a protected area (Ronișoara Forest). The physico- influenced by the anthropogenic activities, for now. The wheat habitats
chemical composition was determined and analyses, including pH, are represented by temporary and semi-permanent puddles, forest
electrical conductivity (EC), redox potential (ORP), temperature, dis­ drainage ditches and trenches generated by forestry machinery. Roni­
solved oxygen (DO), saturation degree with oxygen (SO), turbidity, total șoara Forest consists of remarkable sessile trees. The “Ronișoara Sessile”
alkalinity (At), total hardness (Ht), bicarbonate, nitrogen compounds is well known for its valuable seeds with exceptional genetical confor­
(ammonium, nitrate, nitrite), chloride, phosphate, sulphate, trace ele­ mation (straightness, cylindricality and good lopping). The forest is
ments and heavy metals (Li, B, Na, Mg, Al, Si, K, Ca, Ti, V, Cr, Mn, Fe, Co, situated in the district of Columbidae, rich in ornithologic fauna. The
Ni, Cu, Zn, As, Se, Rb, Sr, Zn, Mo, Cd, Sb, Ba and Pb). Also, the water geological substrate of Ronișoara Forest contains sedimentary forma­
typology was determined and the heavy metal pollution degree was tions represented by rhythmic sequences of thin Paleocene-Eocene
analysed with the help of pollution indices (Heavy metal Pollution sandstone, thin clays and marl with 50 cm sandstones visible in the
Index- HPI and Heavy metal Evaluation Index- HEI) and the water central part, especially in the Picuiatu way and alongside DN18. Sand­
quality index (Water Quality Index- WQI). stones have sometimes a micro-conglomerate character. On the upper
The originality and novelty of the paper extend to the following as­ side of Cornet Valley, Hrabnic Valley, rhythmic deposits of diagenized
pects: 1). Determining and analysing the chemical composition of allu­ sandstones and marls are noticed. The mud samples correspond to the
vial aquifers and mud based on the distribution of substantial physico- aquifer samples 4, 5 and 8, while the rest of the sampling points of water

2
T. Dippong et al. Ecological Indicators 143 (2022) 109347

have no mud. The soil formation in the Tisa Superioara/Ronișoara
Forest occurred on sedimentary lithological substrate represented by
rocks with varied granulometry from clays, gray and red marls, siltites,
sandstones, conglomerates (with volcanic origin- Badenian deposits of
AqQa, GWChart and XLStat Microsoft Excel (demo versions). Durov,
Schoeller and TIS (Total Ionic Salinity) diagrams were used in order to
determine the typology of the water sources. Schoeller was based on the
SO2- -
4 , HCO3, Cl , Mg, Ca and Na + K concentrations and the trilinear
–

tuff) to metamorphic rocks. Durov diagram on the ions amounts (Cl-, SO2- 4 , HCO3, Na + K, Ca, Mg),
–

Fig. 1 shows the study area of Ronișoara Forest and the results pH and TDS concentration. Schoeller diagram is used for showing the
regarding the measurement level of shallow aquifers determined on composition of water and comparing the water analyses (Dauda and
field, starting with May 2020 to February 2021. In the protected areas of Habib, 2015), while with help of the composite Durov plot, the chem­
Tisa Superioara and Ronișoara Forest aquifers can be found at several istry of water is characterized (Durov, 1948). TIS plot is used for
levels: aquifers situated at depths between 0 and − 1 m; − 1 and − 2 m determining the ionic salinity of samples based on the Cl-+HCO–3 and
and − 1 and − 5 m. The area is rich in aquifers with levels deeper than − 1 SO2-4 content expressed in meq/L.
m. This level is specific to the areas situated along the Tisa River or
nearby the tributary (Săpânța, Șugatag, Viseu and Ronișoara rivers). 2.3. Water quality index (WQI)
There are also areas near the Tisa River with aquifers characterized by
levels near the surface (>− 1 m). This level is vulnerable to the infil­ The water quality index (WQI) represents a numerical expression of
tration of surface waters and torrents (e.g. water wells from Teceu lo­ quality. This index is based on the allowable concentrations of physico-
cality situated at the bottom of a hill and near Tisa River). In the case of chemical indicators set by national or international Regulations and on
water wells localized farther the Tisa River, the levels of aquifers specific constants and sub-indices (Yadav et al., 2010; Das et al., 2017).
decrease at levels between − 1 and − 5 m, with a tendency to dry out The WQI is calculated by using the following equations (Eqs. (1)–(3)):
during the dry seasons characterized by high temperatures and intensive ∑n
Wi × Qi
evapotranspiration. WQI = i=1 (1)
Wi
2.1. Experimental methods k
Wi = (2)
Si
The chemical composition of alluvial aquifers and mud samples was
analysed. Twelve aquifer samples (1–12) and three mud samples (I-III) (
Vi − V0
)
were collected in Ronișoara Forest. qi = 100 × (3)
Si − Vo
Nine physico-chemical indicators were analysed (pH, EC- electrical
conductivity, TDS- total dissolved solids, ORP - oxidation–reduction where,
potential, DO - dissolved oxygen, OS - oxygen saturation, turbidity, At -
total alkalinity and Ht - total hardness) and 34 quality parameters (NH+ 4, Wi and qi represent the unit weight and the sub-index; k (k = 1.0) and
NO–2, NO–3, Cl-, PO3- 2-
4 , SO4 , HCO3, Li, B, Na, Mg, Al, Si, K, Ca, Ti, V, Cr, Mn,
–
Si are a proportional constant and standard values of the used
Fe, Co, Ni, Cu, Zn, As, Se, Rb, Sr, Zr, Mo, Cd, Sb, Ba and Pb). physico-chemical parameters, established by national or interna­
Analyses were performed following standard procedures, as follows: tional Regulations, while V0 and V1 are the actual values of the in­
SR ISO 10523/2012 for the pH determination, SR EN 27888–1997 for dicators and the monitored concentrations of the physico-chemical
EC, using pH and EC meters (Hanna Instruments, U.S.A. and WTW, indicators (Yadav et al., 2010; Srinivas et al., 2011; Das et al., 2017).
Germany), SR ISO 10523/2012 and SR EN ISO 5814:2013 for the redox Five quality classes of water were established, based on the WQI
potential and oxygen saturation, dissolved oxygen content. The At, scores: 1. excellent (WQI < 25), 2. good (26 < WQI < 50), 3. poor
HCO–3, Ht and turbidity were determined according to SR EN ISO (51 < WQI < 75), 4. very poor (76 < WQI 〈1 0 0) and 5. unsuitable
9963–1/1996, SR ISO 6059–2008 and SR EN ISO 7027/2001, applying for drinking (WQI > 100) (Yadav et al., 2010; Das et al., 2017).
titrimetric methods and using a turbidimeter (WTW, Germany). PO3- 4
and NO–2 were determined by using a portable equipment Lange SL 1000 2.4. Pollution assessment
(Hach, U.S.A.), applying STAS 3265–86 and SR ISO 6059–2008. NH+ 4
was determined using spectrophotometry, based on SR ISO 7150–1/ In order to assess the pollution status, different pollution indices
2001 and using a Specord 50 UV–VIS spectrophotometer (Analytik Jena, were used. Two of the efficient tools in metal pollution evaluation of
Germany). The anion content (Cl- and SO2- 4 ) was determined by ion water are the heavy metal pollution index (HPI) and the heavy metal
chromatography with the help of an IC Compact 841 (Metrohm, evaluation index (HEI). The concept of heavy metal pollution index was
Switzerland), according to SR EN ISO 15586–2004, after the samples proposed by Horton in 1965, followed by Mohan et al. in 1996.
were filtered through 0.45 µm acetate cellulose filters. The rest of the
water quality parameters were analysed after digestion at 200 ◦ C for 40 2.4.1. Heavy metal pollution index (HPI)
min, with 65 % HNO3 (Merck) in precleaned closed-vessel microwave HPI is based on evaluating the weightage (Wi) for all studied heavy
system (Berghof, Germany). After digestion and cooling, the samples metals (Yazidi et al., 2017). The HPI is computed with the help of two
were filtered, diluted to 50 ml and measured by inductively coupled equations (Eqs. (4) and (5)):
plasma optical emission spectrometry, using an Optima 5300 DV ICP- ∑i=n
OES (Perkin Elmer, Canada). HPI = i=1
(Qi × Wi )
(4)
∑i=n
For the quality assurance of the determinations, duplicate samples, i− 1 Wi
blank and certified standards were analysed (Ions in waste water SPS-
NUTR WW1– Spectrapure and ICP Multi Element Standard Solution IV ∑
n
Ci − Ii
Qi = 100 × (5)
CertiPUR). Calibration was applied with the help of diluted stock stan­ i=1
Si − Ii
dard solutions. The recovery of anions ranged between 87.5 % and 103
% and for metals between 97 % and 105 %, while the accuracy is lower where,
than 20 %.
Wi is the weight for each chemical indicator (heavy metal) and Qi is
2.2. Statistical analysis the sub-index of the ith parameter, Ci, Ii and Si are the determined,
the ideal and the standard values of the parameter (heavy metal); n is
The statistical data was obtained after using the free versions of the total number of the heavy metals of interest. Si for each heavy

3
T. Dippong et al. Ecological Indicators 143 (2022) 109347

Table 1
Quality index parameters of the studied Ronișoara Forest (1–12).
1 2 3 4 5 6 7 8 9 10 11 12 MAC

EC 651 643 414 2640 557 412 399 653 637 440 158 373 2500
μS/cm ±70 ±69 ±37 ±201 ±52 ±40 ±33 ±59 ±61 ±37 ±13 ±31
pH 7.63 7.91 8.37 6.9 8.25 8.05 8.28 7.25 8.27 7.42 7.62 7.41 6.5–9.5
±0.35 ±0.43 ±0.51 ±0.18 ±0.61 ±0.57 ±0.83 ±0.19 ±0.42 ±0.33 ±0.29 ±0.32
ORP 197 191 182 110 169 275 266 206 234 224 212 284 –
mV ±30 ±28 ±28 ±14 ±24 ±26 ±21 ±33 ±36 ±28 ±30 ±23
DO 5.48 9.36 9.25 0.93 9.06 5.58 8.76 5.87 9.01 6.71 9.14 7.19 –
mg/L ±3.02 ±3.13 ±3.01 ±0.23 ±2.82 ±2.31 ±2.47 ±2.34 ±3.02 ±3.06 ±3.25 ±2.61
OS 100 88.8 101 8.70 99.7 98.6 102 68.4 107 73.9 87.3 84.4 –
% ±12 ±3.8 ±12 ±1.72 ±4.0 ±3.7 ±10 ±2.5 ±13 ±2.8 ±3.6 ±3.6
T 4.27 15.2 50.0 15.3 14.7 86.7 213 20.1 34.8 0.92 2.29 13.7 <5
NTU ±2.71 ±1.6 ±2.4 ±1.2 ±1.3 ±3.8 ±32 ±2.1 ±2.2 ±0.15 ±0.31 ±1.4
NH4 mg/L 0.375 0.166 0.243 0.578 0.246 0.081 0.138 0.263 0.179 0.113 0.072 0.159 0.5
±0.112 ±0.116 ±0.201 ±0.411 ±0.121 ±0.001 ±0.101 ±0.321 ±0.132 ±0.091 ±0.001 ±0.013
NO–3 mg/L 1.17 1.11 0.483 0.432 0.274 0.315 0.316 0.493 0.438 0.365 0.172 0.381 50
±0.25 ±0.15 ±0.111 ±0.031 ±0.021 ±0.031 ±0.022 ±0.061 ±0.022 ±0.031 ±0.032 ±0.051
Ht 21.8 17.8 12.4 92.4 13.0 12.7 12.7 19.7 16.3 16.4 3.90 10.5 >5
Go ±3.2 ±0.2 ±0.1 ±6.2 ±0.4 ±0.4 ±0.4 ±0.2 ±0.2 ±0.1 ±0.1 ±0.2
At 367 315 227 750 223 216 230 285 254 256 88.0 225 –
mg/L ±17 ±15 ±18 ±51 ±12 ±15 ±17 ±19 ±13 ±15 ±4.0 ±16
PO3-
4 mg/L 0.02 0.07 0.03 0.40 0.03 0.07 0.03 0.04 0.04 0.08 0.14 0.09
±0.01 ±0.02 ±0.01 ±0.01 ±0.01 ±0.02 ±0.01 ±0.01 ±0.01 ±0.02 ±0.08 ±0.01
Cl- 10.6 10.8 7.28 56.9 45.4 5.03 4.61 49.9 51.7 7.55 4.83 5.29 250
mg/L ±1.2 ±1.1 ±0.31 ±3.0 ±2.8 ±0.31 ±0.22 ±5.1 ±4.7 ±2.31 ±0.34 ±0.44
SO2-4 mg/L 30.0 55.0 34.0 2080 38.0 17.1 8.73 17.0 62.0 9.14 23.0 22.0 250
±3.2 ±4.7 ±2.9 ±17 ±2.6 ±0.9 ±5.4 ±2.0 ±3.9 ±0.73 ±2.0 ±1.8

metal of interest was established by national or international Regu­
lation considering the studied type samples (Horton, 1965; Mohan
et al., 1996). The HPI results classify the alluvial aquifer samples into
one of the three categories of heavy metal pollution levels, namely
high pollution level (HPI > 30), medium pollution level (15 < HPI <
30) and low pollution level (HPI < 15) (Horton, 1965; Mohan et al.,
1996; Edet and Offiong, 2002).
2.4.2. Heavy Metal Evaluation Index (HEI)
HEI is generally used for an overall quality assessment of water
samples regarding the heavy metal content and it is calculated with the
help of the following equation (eq (6)) (Edet and Offiong, 2002; Gha­
derpoori et al., 2018):
∑n Ci
HEI = i=1 S
(6)
i
deviation, together with the MACs regarding the drinking water quality
of alluvial aquifers from the protected area of Ronișoara Forest.
Varied values for EC were determined, the highest value was ob­
tained for sample 4–158 and µS/cm source of sulfurous water) and the
lowest for sample 11–2640 µS/cm. The highest value exceeds the MAC
(2500 µS/cm) with 140 µS/cm. A high EC is related to the presence of
dissociated ionic species, dissolved ionic substances, organic and inor­
ganic salts, which through dissociation assures the mobility of ionic
species in water corelated with the fixed water residue and influenced by
groundwater chemistry, climate (precipitation), developing cycle of the
terrestrial vegetation and geological substrate type (Timpano et al.,
2018). In the east part of USA, the studies of water bodies flowing
through the forests indicate a correlation between the high EC and the
low diversity of aquatic insects (Timpano et al., 2018). However, this
could not be associated with the fixed water residue, due to the errors
caused by the transformation of CO2/HCO–3 species through evaporation

where, at 105 ◦ C. High values of EC are harmful to the benthic communities of

n, Ci and Si are the total number, the monitored concentration and
the standard value of the studied heavy metals. The HEI scores
indicate one of the quality classes for the studied aquifer samples,
such as high (HEI > 20), medium (10 < HEI < 20) and low pollution
level (HEI < 10) (Ghaderpoori et al., 2018).
2.4.3. Mud to water transfer
The transfer of metals (Cd, Co, Cr, Fe, Mn, Ni, Pb, Zn, Ca, K, Mg and
Na) was calculated based on dry weight with the help of the transfer
factor (Tf). The following equation was used, according to Cui et al.
(2005):
Tf =
Cwater
(7)
Cmud
3. Results and discussions
3.1. Chemical composition
In Table 1, the results for the physico-chemical indicators are pre­
sented as the mean value for all 12 months of 2021 plus the standard
macro vertebrates and lead to the decrease of Ephemeroptera in the
water bodies, especially in waters rich in salts (Armstead et al., 2016).
The benthic communities of macro vertebrates are the base for the
aquatic trophic level, which, if affected, perturb the entire aquatic
ecosystem. High turbidity and excess of fine sediments caused by intense
soil erosion are other negative effects of high EC (Armstead et al., 2016).
The EC of water is influenced by diverse factors, such as the precipitation
regime, chemistry of aquifer, substrate type oof the water body, the
development cycle of terrestrial vegetation.
The studied aquifers are characterized by pH ranging from 6.9 to 8.3.
The pH varies due to anthropic activities and pollution degrees (sulfur
and nitrogen oxides, nitrogen and fossil fuels), the water gaining a salty
taste and leading to eyes and skin irritation. The increase of water
temperature and defrosting lead to the transition of pH from acid to
neutral conditions (Faithful et al., 2016). The level of pH in water could
significantly affect the life supporting capacity of ecosystems. A low pH
is given by the increase of CO2, HCO3 and alkalinity of water, also
caused by the presence of weak base salts in the spoil (Arulnangai et al.,
2021; Mohammed et al., 2022). Swain et al. (2021) reported that low pH
is also caused by low flow, richness in organic matter, remineralization
of organic matter and degradation of vegetation. As the organic matter is
decomposing, CO2 is released and it reacts with water producing

4
T. Dippong et al.
carbonic acid (Adesakin et al., 2020). If the aquifers geology contains
carbonic rocks (sandstones, metamorphic granitic gneisses, volcanic
rocks), the groundwater remains acidic (Jain et al., 2022).
The ORP varied between 110 and 284 mV. It indicates the potential
of oxidizing the organic matter, including the inactivation of microor­
ganisms. The presence of hypochlorite, chloramine, organic matter (dirt
and dust), urine, fecal matter, microorganisms, acting as reductors, in­
crease the ORP of water.
The content of dissolved oxygen (DO- dissolved oxygen gas in
aquatic environment) is related to the biological and physical processes
occurring in the aquatic systems, the stratification of water bodies,
photosynthesis process, metabolic activities of microorganisms and the
pollution level caused by organic matter decomposition (Adesakin et al.,
2020; Ali et al. 2022; Jain et al., 2022). DO is produced through
photosynthesis or comes from direct diffusion from the atmosphere
(Adesakin et al., 2020). In the studied samples, DO ranged between 0.93
(sample 4) and 9.36 mg/L (sample 2) (Table 1). As the dissolved oxygen
increases, water is richer in organic matter and the possibility to develop
pathogenic flora increases, indicating the predominant biological and
physical processes in water. The values of dissolved oxygen indicate the
pollution degree, caused by the excess decomposition of organic matter,
temperature, oxygen sources, light, and salinity (Dimri et al., 2021).
Dissolved oxygen is influenced by the air pressure, temperature and the
presence of microorganisms (Jain et al., 2022). The presence of oxygen
favors deferrization and demanganization of water, forming a protection
layer in the pipeline system, altering the freshness of water (Jain et al.,
2022). Low values of DO indicate a water rich in bacteria, which
consume the dissolved oxygen and lead to microbial reduction of NO–3 to
NO–2 and of SO2-4 to S, imprinting a specific smell to the water (Ali et al.,
2022; Jain et al., 2022).
Water turbidity ranges between 0.92 and 213 NTU, the lowest value
was obtained in sample 10 and the highest in sample 7, probably due to
soil erosion and deforested areas. Erosion is intensified in areas
vulnerable to wind and precipitation (crops, land covered by short size
vegetation). Turbidity is caused by suspended, organic and colloidal
matter coming from sediments or soil, as well as by the presence of
sludge, plankton, Fe(OH)2, Al(OH)3 and bacteria (Serban et al., 2020).
Water characterized by high turbidity affects the photosynthesis of
phytoplankton, therefore diminishing the oxygen content. Turbidity
increases during precipitation (dust and air particles), especially in the
shallow aquifers (Chatanga et al., 2019; Serban et al., 2020). High
turbidity favorizes the development and increase of pathogens in water,
causing intestinal diseases (Mohammed et al., 2022). The presence of
sludge, organic and inorganic matter, algae, microorganisms and clay
enriches the water’s turbidity. A high turbidity water could cause health
problems, and warping, sedimentation in aquatic habitats (Mohammed
et al., 2022).
The nitrogen compounds are lower than the MACs (0.5 mg/L NH+ 4 development (Adesakin et al., 2020). Sources of PO3-
and 50 mg/L NO–3), except NH+ 4 in sample 4 (0.58 mg/L). The com­
pounds range between 0.07 and 0.58 mg/L NH+ 4 and between 0.17 and
1.17 mg/L NO–3. The low variation of NO–3 is caused by the use of fer­
tilizers from agricultural practices and by the variances in hydro­
geological regimes (Adesakin et al., 2020). NO–3 is characterized by high
mobility in water and soil, due to the lack of absorption in soil,
precipitating under dry conditions as a mineral (Arulnangai et al.,
2021). The antibacterial properties of NO–3 play a significant role in
protecting the gastrointestinal tract against various gastrointestinal
pathogens (Adesakin et al., 2020). Methemoglobinemia or the “blue
baby” syndrome is one of the most known negative effects of contami­
nation with NO–3. NO–3 reacts with hemoglobin, decreasing the trans­
portation of oxygen through blood towards all the tissues and organs (Yu
et al., 2020).
NH+4 is an indicator of contamination due to incomplete organic
matter decomposition (protein decomposing), leakage from septic tanks,
domestic sewer residues (urea hydrolysis in nitrification of NH+ 4 ) and is
oxidized by atmospheric oxygen and microorganisms from water
5
Ecological Indicators 143 (2022) 109347
(nitrifying bacteria) (Teodorescu et al., 1980; Rupias et al., 2021). The
incomplete oxidation of NH+ 4 in the presence of nitrifying bacteria is a
source of NO–2 (Adesakin et al, 2020). High amounts of nitrogen and
phosphorus in water systems assure conditions for the eutrophication
process, increasing the pathogen flora, viruses and parasites.
The high amount of NH+ 4 (sample 4) is due to the oxidized NH4 ions
+
by the oxygen from air and by the microorganisms in water (nitrification
bacteria). NH+ 4 is present in water due to complete and incomplete
organic waste and to the decomposition of organisms containing nitro­
gen (protein decomposition) (Laha et al, 2019; Chai et al., 2021). The
organic matter is not only a natural source of NH+ 4 , but also a booster for
microbial activities, generating a reduction environment (Laha et al.,
2019). NH+ 4 is not toxic, but in relation with other chemicals and bac­
teria leads to water pollution with negative effects on human health
(Goi, 2020). The accumulation of a high amount of NH+ 4 in blood could
lead to hepatic encephalopathy. Studying and knowing the NH+ 4 content
is important in assessing the pollution degree and determining the
manure load degree (Laha et al., 2019).
Ht helps reducing the Ca and Mg salts deposition and the negative
effects of the toxic elements and compounds (Adesakin et al., 2020). Ca
and Mg, the two most important ions reflecting the total hardness of
water, are found in a variety of sedimentary rocks, the most common of
which are limestone and chalk (Mohammed et al., 2022). According to
the total hardness (Ht), the studied waters are characterized as soft and
very hard waters, ranging from 3.90 to 94.4 German degrees (G◦ ). The
high values of Ht (sample 4) could be due to the dissolved polyvalent
metal ions from sedimentary rocks, and infiltrations and leaks from the
soil. If used as drinking water source, a water with high Ht is charac­
terized by an unpleased taste and could lead to salt depositions (bones,
kidneys and gallbladder) and indigestion (Adesakin et al., 2020; Jagaba
et al., 2020). Hard waters present no concern to human health, but affect
household and industrial activities (Arulnangai et al., 2021; Jain et al.,
2022; Adesakin et al., 2020). The high values of total hardness are
caused by abundant precipitation, high flow of water sources, and speed
of current. Also, the geology and sedimentary composition of limestone
increases the total hardness (Mohammed et al., 2022). The total hard­
ness influences the physico-chemical characteristics of waters (superfi­
cial tension, fluidity, dynamic viscosity), significant in many
technological processes, in which emulsifiable and industrial washing
fluids are used in metal processing (Mohammed et al., 2022). Samples
with low total hardness (sample 11) are characterized by insufficient
contact with rocks. A soft water is corrosive, could dissolve heavy metals
and form foam, leading to cooling systems instability and warping of
filters (Adesakin et al., 2020; Mohammed et al., 2022).
The studied water samples are characterized by low PO3- 4 concen­
trations, lower than 0.4 mg/L. The mean value is 0.08 mg/L. The pres­
ence of PO3-4 in water affects the taste and colour and encourages algae
4 are represented by
detergents and fertilizers based on phosphates and also rocks degrada­
tion (Adesakin et al, 2020). The occurrence of PO3- 4 increases the number
of algae, affecting the sensorial capacity of water sources, by changing
the taste and colour (Adesakin et al., 2020).
Total alkalinity (At) is caused by the presence of PO3- 4 and HCO3. The
–
studied samples are characterized by At ranging from 88.0 to 750 mg/L
CaCO3. Low alkalinity levels indicate low HCO–3, OH and CO2– 3 levels,
caused by anthropogenic runoffs and geology (Adesakin et al., 2020).
This buffering effect is due to the presence of weak acids and their
conjugated bases (Adesakin et al., 2020). High alkalinity is a protection
mechanism of the environment that limits the damage to aquatic fauna
and flora, caused by waste waters or acid rain capable of modifying the
pH (McKibbin et al., 2008).
Chloride concentrations were lower than the MAC (250 mg/L), with
the highest value obtained for sample 4 (56.9 mg/L) and the lowest for
sample 7 (4.61 mg/L). The high amounts of chloride are related to the
natural occurrence in the geological strata of aquifers and it is largely
distributed in all types of rocks (Adesakin et al., 2020). The Cl- anions
T. Dippong et al. Ecological Indicators 143 (2022) 109347

Fig. 2. TIS diagram based on the Cl- + HCO–3 vs SO2-

4 content in samples 1–12.

Table 2
Metals and heavy metals characteristics of the studied Ronișoara Forest (1–12).
µg/ 1 2 3 4 5 6 7 8 9 10 11 12 MAC
L

Li 5.9 ± 1.2 8.9 ± 2.0 3.3 ± 0.9 52 ± 12 2.2 ± 0.3 3.1 ± 1.0 2.3 ± 0.6 ± 0.2 1.7 ± 0.3 1.4 ± 0.1 0.9 ± 0.1 1.4 ± –
0.4 0.2
Na 24950 ± 22340 ± 7105 ± 53310 ± 18200 ± 5859 ± 4249 ± 17830 ± 18250 ± 6348 ± 2827 ± 4012 ± 200,000
3254 3001 796 5296 2650 530 561 2480 7995 665 215 504
Mg 61580 ± 19830 ± 11950 ± 64990 ± 14140 ± 10930 ± 8505 ± 11070 ± 12850 ± 8528 ± 3193 ± 9502 ± –
7165 7965 1835 7024 1635 1351 932 1354 1364 865 324 804
Al 1.2 ± 0.2 1.1 ± 108 ± 10 32.2 ± 2.9 35.9 ± 3.2 164 ± 22 111 ± 0.9 ± 0.3 13 ± 1.0 2.4 ± 1.2 16.3 ± 127 ± 200
0.09 10 1.4 19
K 370 ± 53 1772 ± 1487 ± 5337 ± 1367 ± 1150 ± 720 ± 1117 ± 1496 ± 529 ± 46 358 ± 37 919 ± –
201 139 503 211 199 78 96 120 93
Ca 40080 ± 94050 ± 70100 ± 669900 ± 107600 ± 72170 ± 81380 91020 ± 93180 ± 78190 ± 27460 ± 56840 100,000
563 863 8201 59005 96541 896 ± 799 835 8697 6785 1965 ± 604
Cr 2.4 ± 0.5 1.2 ± 0.1 1.1 ± 0.1 1.7 ± 0.2 1.3 ± 0.2 0.3 ± 0.1 0.6 ± 1.1 ± 0.1 0.8 ± 0.2 1.0 ± 0.3 0.7 ± 0.2 0.8 ± 50
0.1 0.2
Mn 3.5 ± 0.5 7.8 ± 58.6 ± 206 ± 27 36.2 ± 4.3 166 ± 19 93 ± 21 2840 ± 76 ± 13 5.5 ± 1.3 4.1 ± 0.6 574 ± 50
0.59 4.7 198 87
Fe 4.8 ± 0.6 16 ± 1 135 ± 19 221 ± 29 229 ± 33 204 ± 18 231 ± 334 ± 47 24.3 ± 4.0 ± 1.1 40.8 ± 270 ± 200
40 2.9 4.3 30
Ni 0.3 ± 0.5 ± 0.2 1.0 ± 0.4 5.3 ± 1.8 0.9 ± 0.2 1.4 ± 0.3 1.2 ± 0.8 ± 0.2 0.3 ± 0.1 0.4 ± 0.1 0.3 ± 0.1 0.6 ± 20
0.01 0.2 0.2
Cu 1.0 ± 0.3 0.6 ± 0.2 3.1 ± 0.5 5.6 ± 1.1 5.5 ± 1.0 5.3 ± 1.0 1.1 ± 0.5 ± 0.1 0.6 ± 0.1 0.3 ± 0.1 4.4 ± 0.6 2.8 ± 100
0.2 1.1
Zn 1.2 ± 0.4 1.8 ± 0.2 20.7 ± 45.7 ± 5.8 40.7 ± 3.8 25.3 ± 3.6 ± 2.3 ± 0.3 5.8 ± 0.4 3.5 ± 0.7 14.5 ± 16.4 ± 5000
2.8 3.4 0.4 0.3 0.1
Sr 231 ± 21 1240 ± 315 ± 51 7524 ± 614 ± 75 360 ± 59 132 ± 428 ± 53 561 ± 62 263 ± 26 26.3 ± 154 ± –
201 704 43 2.9 13
Cd 0.03 ± 0.02 ± 0.04 ± 0.4 ± 0.1 0.3 ± 0.1 0.3 ± 0.2 0.03 ± 0.02 ± 0.06 ± 0.05 ± 0.04 ± 0.05 ± 5
0.01 0.01 0.01 0.01 0.01 0.02 0.03 0.01 0.03
Ba 11.6 ± 22.8 ± 46.3 ± 21.1 ± 1.8 33.9 ± 3.5 55.4 ± 36.3 ± 45.8 ± 33.5 ± 133 ± 12 2.7 ± 0.6 13.0 ± 700
2.9 3.2 3.5 6.0 3.8 4.1 3.7 0.2
B 16.6 ± 37 ± 4 22 ± 2 90.3 ± 16.6 ± 1.9 23.2 ± 7.8 ± 10.5 ± 14.5 ± 6.8 ± 0.4 3.9 ± 0.5 10.7 ± 1000
0.2 19.2 2.8 0.9 1.0 1.7 1.0
Si 1066 ± 4466 ± 2942 ± 7347 ± 1736 ± 2635 ± 3 3266 ± 1776 ± 1839 ± 3092 ± 3571 ± 2929 ± –
110 453 301 722 165 378 186 190 410 26 302
Ti 0.10 ± 63.3 ± 88.1 ± 555 ± 49 66 ± 7 50.9 ± 52.1 ± 0.42 ± 42.5 ± 43.8 ± 1.5 ± 1.0 39.9 ± –
0.01 6.9 7.5 6.0 5.3 0.02 3.8 4.1 2.3
V 4.0 ± 0.5 5.6 ± 0.7 2.3 ± 0.3 14.5 ± 1.8 12.5 ± 1.0 7.0 ± 1.0 7.1 ± 7.2 ± 0.6 10 ± 1.2 7.7 ± 0.8 5.2 ± 0.6 1.9 ± –
0.7 2.8
Co 0.04 ± 0.03 ± 0.40 ± 1.10 ± 0.20 ± 1.01 ± 0.40 ± 0.30 ± 0.20 ± 0.02 ± 0.03 ± 0.40 ± –
0.01 0.01 0.03 0.86 0.01 0.03 0.01 0.01 0.01 0.01 0.01 0.02
As 2.1 ± 0.2 1.8 ± 1.2 2.2 ± 0.1 8.2 ± 0.4 7.4 ± 4.2 3.6 ± 0.4 2.3 ± 3.2 ± 0.3 3.1 ± 0.2 2.0 ± 0.1 1.6 ± 0.2 5.1 ± 10
0.2 1.9
Se 5.8 ± 1.6 8.6 ± 3.3 6.9 ± 1.6 3.0 ± 0.8 10.7 ± 1.2 0.6 ± 0.2 0.6 ± 10.8 ± 12.8 ± 8.5 ± 3.0 5.4 ± 1.9 3.4 ± 10
0.2 2.8 3.2 0.9
Rb 0.20 ± 0.64 ± 0.30 ± 4.70 ± 0.51 ± 0.40 ± 0.20 ± 0.33 ± 0.41 ± 0.10 ± 0.20 ± 0.40 ± –
0.01 0.19 0.01 0.12 0.08 0.01 0.01 0.01 0.02 0.01 0.01 0.02
Mo 0.70 ± 0.61 ± 0.40 ± 2.43 ± 0.03 ± 0.02 ± 0.02 ± 0.20 ± 0.03 ± 0.04 ± 0.02 ± 0.03 ± –
0.03 0.02 0.01 0.99 0.01 0.01 0.01 0.01 0.02 0.01 0.01 0.02
Sb 0.03 ± 0.02 ± 0.31 ± 0.50 ± 0.03 ± 0.20 ± 0.22 ± 0.03 ± 0.05 ± 0.03 ± 0.2 ± 0.2 ± 5
0.01 0.01 0.01 0.01 0.01 0.01 0.01 0.02 0.01 0.01 0.01 0.01
Pb 0.05 ± 0.03 ± 2.7 ± 0.4 7.2 ± 1.8 4.5 ± 1.1 6.6 ± 1.3 1.4 ± 0.03 ± 0.02 ± 0.05 ± 1.5 ± 0.1 5.0 ± 10
0.03 0.02 0.9 0.01 0.01 0.02 2.1

6
T. Dippong et al.
are mobile, present in the geological strata of boreholes, commonly
distributed in all types of rocks, consequently increasing in water sam­
ples as a result of water–rock (magmatic rocks dissolution) and water-
soil interaction and of the application of disinfectants used in water
purification, chemical fertilizers in agriculture, a result of irrigation,
waste water infiltration, domestic sewage and waste deposits leakage
(Hanraha et al., 2012; Adesakin et al., 2020; Zakaria et al., 2020; Rupias
et al., 2021; Sargazi et al., 2021). Using a water rich in Cl- could lead to
health issues, such as congenital anomalies, unpleasant taste and smell,
asthma symptoms, allergies or even bladder cancer (Rupias et al., 2021).
HCO–3 and SO2- 4 ranged between 107 and 915 mg/L and 8.73 and
2080 mg/L. The highest amounts were obtained in sample 4, which is
the only sample with concentrations exceeding the MAC (250 mg/L
SO2- 2-
4 ) more than eight times. The low amount of SO4 characterizing the
majority of samples reflects the lack of anthropogenic activities, while
the high concentration in sample 4 is caused by sulphide dissolution
from fertilizers, urban residues or pyrite, gypsum matter, sedimentary
rocks or decomposition of animals and plants (Adesakin et al., 2020;
Rupias et al., 2021; Mohammed et al., 2022). The presence of lignite and
gypsum in soil, as well as the decomposition of organic matter, minerals
in water, or the burning of organic matter, such as volcanic activities and
acid rain, are all sources of SO2-4 (Loucif et al., 2020).
Sources of HCO–3 in waters are represented by silicate and CO–3
minerals dissolution, chemical reactions between silicate minerals and
aquifers, and also by the atmospheric CO–2 and CO–2 from the soil matrix
(Masoui and Ali, 2020; Rupias et al., 2021).
Based on the Cl-, HCO–3 and SO2- 4 content, a Total Ionic Salinity (TIS)
plot was implement indicating and classifying the water samples based
on the salinity content. Comparable salinity values are indicated in
Fig. 2 between 6 meq/L and 24 meq/L. The majority of samples have a
TIS below 18 meq/L, from which three groups are formed; samples 1, 2,
5, 8, 9 with TIS between 12 and 18 meq/L, samples 3, 6, 7, 10, 12 with
TIS between 6 and 12 meq/L and sample 11 with TIS as low as 6 meq/L.
Sample 4 is characterized by the highest TIS (>100 meq/L). It was
noticed that sample 4 is the richest water in Cl-, SO2- 4 , TDS, EC, NH4 ,
+
HCO–3, PO3-4 and has the highest values for the EC, ORP, H t and A t.
Sample 4 is also characterized by the lowest pH. It is also rich in Mg and
Ca (the highest values in the sample series).
The metal content is indicated in Table 2. Results are presented as the
mean value of all 12 results sets obtained in every month of 2021,
together with the standard deviation. Generally, samples are rich in
certain elements, especially in Fe, Mn and Se, which exceed the MACs,
one time for Fe, one to 50 times for Fe and one and up to three times for
As. The studied heavy metals are below the MACs. The content of As, Co,
Cr, Cd, Ni, Mo, Pb, Sb, Se, Rb, Li, Zr and V are below 10 µg/L.
The lowest Fe concentration was obtained in sample 10 and the
highest in sample 8. The high amount indicates the presence of fine
particles of humid materials or organic colloids. Rich water in Fe gives a
red or brown colour, modifying the taste and increasing the turbidity
(Sutton, 2010; Rupias et al., 2021). In water, Fe has two forms, soluble
and insoluble. Soluble Fe is colourless and clear, because it is completely
dissolved. Once the dissolved Fe has contact with oxygen or chloride, it
oxidizes and becomes ferric, insoluble. Insoluble Fe alters the colour of
water, becoming brown–red and turbid (Rupias et al., 2021). In the
water system, Fe(III) prevails due to the thermodynamic stability
compared to Fe(II). Fe (II) is oxidized to Fe (III) as a result of the contact
with oxygen from air or of iron bacteria action (natural organisms which
consume iron and other minerals forming a brown slime) (Rupias et al.,
2021). Fe (III) is insoluble in water hydroxides, which can affect skin and
hair in the long term. Iron easily participates in redox reactions and in
certain conditions could lead to the affections of smell and taste. In
geochemical conditions, Fe helps remediate some chemical substances
which suffer chemical transformations associated with redox reactions
(Rupias et al., 2021). The active centre structure of redox enzymes,
protein and haemoglobin are dependent on Fe, although, exposure to Fe
could cause health issues, such as neurologic, cardiovascular,
7
Ecological Indicators 143 (2022) 109347
respiratory, liver disorders, Alzheimer, Parkinson’s or pigmentation
changes (Krisham et al., 2021).
Mn is a significant nutrient for animals and humans, a transition
metal, which in high amounts can have negative effects (Krisham et al.,
2021). In the studied samples, almost 60 % exceeded the MAC (sample 8
exceeds 58 times the MAC). Sources of Mn are represented by water­
–rock interactions, especially from metamorphic and igneous rock
minerals, as amphibole, olivine or pyroxene (Rupias et al., 2021). The
studied waters are rich in Fe and Mn due to the geological origin
(goethite and hematite) (Eslami et al., 2022). The major cations are
below the MACs, ranging from 2.8 to 53 mg/L Na, 0.9–164 µg/L Al,
0.36–5.3 mg/L K, and 3.2–65 mg/L Mg, except for Ca, with values be­
tween 27 and 670 mg/L (sample 6 exceeds the MAC six times).
Waters rich in Na could alter the osmotic pressures in the organisms,
having negative effects on aquatic life. Sources of Na are natural erosion
of salt deposits and dissolution of rocks containing Na, or the use of salt
in defrosting the roads, irrigation and pluvial waters which interact with
soils rich in Na, waste waters infiltration or effluents coming from the
sewage system (Adimalla and Qian, 2019; Ramachandran et al., 2021).
Contribution of silicate and igneous minerals weathering indicated the
dominance of Ca-Na-HCO-3 waters. The sources of Na in the Na-HCO-3
waters are represented by igneous minerals and by the reverse ionic
exchange processes between Ca and Na (Rupias et al., 2021). Sources of
Ca in aquifers are represented by cation exchange and geogenic pro­
cesses implying igneous rocks (feldspars, pyroxene or amphibole)
(Rupias et al., 2021). Ca is an important mineral that helps prevent
cancer, increase bone mass, and prevent toxic elements from entering
the body (Arulnangai et al., 2021). Alteration processes of minerals
(amphiboles, micas, olivine) are natural sources of Mg in the ground­
water samples (Rupias et al., 2021). Waters rich in Mg present positive
effects on human health (cardiovascular functions) (Arulnangai et al.,
2021).
The free ion Cu is the toxic form of Cu with the highest bioavail­
ability. Although, the dissolved Cu in water is in balance with the Cu
from sediments, not all Cu species are bioavailable for aquatic organ­
isms. Cu was lower than the MAC (100 µg/L), with a mean value of 2.6
µg/L. Potential sources of Cu could be the presence of industrial and
agricultural waste and deposits containing Cu (Adeyemi and Ojekunle,
2021). Cu-sulphide ores, such as chalcocite, bornite, aquifer bedrock’s
geological characteristics imply chemical reactions that release Cu into
aquifers (Eslami et al., 2022). Cu exploration in the mines near the study
area also represents a significant source of Cu. Cu in high amount could
be dangerous in water, leading to nose, mouth, eyes irritation, and could
cause cerebral damage, stomach aches, diarrhea and vomiting (Adeyemi
and Ojekunle, 2021).
Samples 4 (8.2 µg/L) and 5 (7.4 µg/L) are characterized by relatively
high amounts of As, slightly reaching the MAC (10 µg/L). There are
anthropogenic (mining and industrial activities) and natural
(geochemical bedrock and volcanic rocks) sources of As (Alshehri et al.,
2021; Krisham et al., 2021; Eslami et al., 2022). Contaminated waters
with As could harm human health if consumed or used in irrigation
practices, causing cancer, vascular and skin illnesses or other acute ef­
fects (Ali et al., 2022).
There are natural (weathering processes involving mobilization and
mineralization of carbonate rocks) and anthropogenic sources (metal
industry, mining exploitation, the use of fertilizers and pesticides in
agricultural practices) of Pb in the aquifer systems (Eslami et al., 2022).
Surficial aquifers are mainly affected and altered by human activities
(Ali et al., 2022). Due to its oxidative degradation, high toxicity, and bio-
accumulative characteristics, Pb causes irreversible health issues (mal­
formations, anemia, cancer affecting numerous systems and main or­
gans) (Krisham et al., 2021; Ali et al., 2022; Eslami et al., 2022).
The dissolution of ore-bearing rocks rich in Ni and the metals
leaching increase the aquifers in Ni, the exposure to Ni leading to risk of
cancer (Krisham et al., 2021).
The release of Zn into the environment is caused by coal combustion
T. Dippong et al. Ecological Indicators 143 (2022) 109347

Table 3
Metal content of mud samples (I, II, III) in mg/kg dry matter (DM) collected near samples 4, 5 and 8 in Ronișoara Forest.
Element

Sample Fe Ni Cr Cu Zn Pb Mn Ca Na Mg K

mg/kg DM

I 23,620 27.1 25.6 38.3 88.6 16.4 239 13,940 390 5290 5371
II 19,510 31.3 16.8 28.5 33.9 7.10 187 2889 114 4482 1821
III 34,700 0.31 0.42 1.20 34.3 7.90 2718 15,800 178 1476 724

Fig. 3. Schoeller -a) and Durov -b) diagrams applied for studied water samples in Ronișoara.

and metal processes. Zn is a mineral important for the well functioning The metal content of the mud samples is mostly represented by Fe,
of the human body. In developing countries, the population presents Zn followed by Ca > Mg > K > Mn > Na > Zn > Cu > Ni > Cr > Pb
deficiency. On the other hand, a high intake of Zn causes acute and (Table 3). Co and Cd are under the detection limits of the methods.
chronic health issues, such as vomiting, cramps or anemia (Krisham
et al., 2021).
3.2. Variation of the physico-chemical and chemical compounds
Natural sources of Cr are represented by geogenic processes implying
mafic and ultramafic rocks (Krisham et al., 2021). Cr is cytotoxic and
The water types were determined using the Durov and the Schoeller
genotoxic for eukaryotic cells and bacteria, therefore waters rich in Cr, if
plots. According to Ravikumar et al. (2015), the Durov diagram indi­
used for drinking, can lead to liver, intestinal, and gastric diseases
cated that generally samples are characterized as Ca-HCO-3 types, in the
(Krisham et al., 2021).
current study, sample 4 is classified as Ca-Cl- type, as shown in Fig. 3.

8
T. Dippong et al. Ecological Indicators 143 (2022) 109347

Fig. 4. HPI and HEI results a) and the contribution of heavy metals to the HPI calculated for samples 1–12b).

Likewise, according to the Durov plot, there are two main

geochemical processes affecting the genesis of the studied alluvial
aquifer samples, namely infiltration waters of Ca-HCO–3 type (1–3, 5–12)
and cation exchange reactions (sample 3). The Schoeller diagram indi­
cated the trend of the chemical composition with respect to the seven
chemical indicators which was based on. Generally, according to the
plot, HCO–3 and Ca dominated, followed by SO2- -
4 , Mg, Cl and Na + K
(Fig. 3).

3.3. Heavy metal pollution index (HPI) and heavy metal Evaluation
index (HEI)

For the calculation of HPI and HEI, Si for each heavy metal is ac­
cording to international and national regulation concerning the quality
of water, more specifically to the Directive 98/83/EC, WHO guidelines
(WHO, 2006; WHO, 2011) and to Law 311 (2004).
HPI scores ranged between 5.6 and 234 (Fig. 4), with a mean value of
41. Water samples were classified into three heavy metal pollution
levels. Samples R1-R3, R9-R11 were characterized by a low level of
pollution, ranging between 5.6 and 16.4. Samples 4–6, 8 and 12 were
characterized by a high pollution level, and sample 7 was characterized
by a medium level of pollution with heavy metals (As, Cd, Cr, Cu, Fe,
Mn, Ni, Pb and Zn).
Given the HPI scores, the pollution trend increases from sample 2 to
10 < 1 < 11 < 9 < 3 < 7 < 5 < 6 < 4 < 12 < 8, directly proportional with
the heavy metal content. Sample 8 is characterized by a high amount of
Mn and Fe, exceeding the maximum allowable limit established by the
Fig. 5. The quality clasification of samples (1–12), according to the
WQI scores.
national and international Regulation. Generally, the high HPI scores
are attributed to the high content of Mn, Fe, As and Pb, as indicated in
Fig. 4. Generally, the main contribution is given to Mn and Fe, which
characterized samples 7, 8, 9 and 12. According to Fig. 5, samples 1, 2,
10, 11 present variation in the content of heavy metals (As, Cd, Cr, Cu,
Fe, Mn, Ni, Pb and Zn).
Other studied indicated HPI scores ranging from − 18.9 to 2103 in
Daraa Tafilalet (Morocco), indicating that the studied waters were
characterized by high pollution level with heavy metals, generally
attributed to mining and industrial activities (Khadija et al., 2021). Also,
in Narayanganj City (Bangladesh), water was characterized by a high

9
T. Dippong et al. Ecological Indicators 143 (2022) 109347

Table 4
The transfer factor calculated for samples I-III based on the metal content.
Sample Transfer factor

Cd Co Cr Fe Mn Ni Pb Zn Ca K Mg Na

I 2.0*10-3 5.5*10-3 6.6*10-5 9.4*10-6 8.6*10-4 2.0*10-4 4.4*10-4 5.2*10-4 4.8*10-2 9.9*10-4 1.2*10-2 1.4*10-1
II 1.5*10-3 1.0*10-3 7.4*10-5 1.2*10-5 1.9*10-4 2.9*10-5 6.3*10-4 1.2*10-3 3.7*10-2 7.5*10-4 3.1*10-3 1.6 *10-1
III 5.0*10-4 1.5*10-3 2.6*10-3 9.6*10-6 1.0*10-3 2.6*10-3 1.3*10-5 6.7*10-5 5.8*10-3 1.5*10-3 7.5*10-3 1.0*10-1

Table 5
The correlation matrix (Pearson) applied for the WQI scores and the physico-chemical parameters.
Variables pH EC Cl- SO2-
4 TDS NH+
4 NO–3 NO–2 Ht WQI

pH
EC − 0.557
Cl- − 0.144 0.505
SO2-4 − 0.569 0.975 0.396
TDS − 0.551 0.999 0.510 0.968
NHþ 4 − 0.475 0.870 0.492 0.801 0.874
NO–3 − 0.061 0.091 − 0.106 − 0.052 0.107 0.312
NO2 –
− 0.167 − 0.267 − 0.264 − 0.118 − 0.295 − 0.292 − 0.252
Ht − 0.593 0.995 0.440 0.980 0.994 0.862 0.082 − 0.248
WQI − 0.475 0.861 0.482 0.803 0.862 0.996 0.298 − 0.212 0.853

pollution level. HPI was higher than the critical value of 100 for all the
studied surface waters (Rahman et al., 2020).
HEI scores ranged between 0.4 and 59 (Fig. 5). The highest score was
determined in sample 8, which is positively corelated with the highest
HPI score for the same sample. High score was obtained for samples 12
< 4 < 6, similarly correlated with the HPI scores. According to the HEI
scores, samples were classified in three pollution classes, namely: low
polluted (1–7, 9–11), medium polluted (12) and high polluted (8) with
the studied heavy metals. Different studies observed similar results for
waters, HEI scores ranging between 0 and 1139 in Morroco and 16.4 and
273 in Bangladesh, indicating high pollution level (Rahman et al., 2020;
Khadija et al., 2021).
Three samples were analyzed from the metal content point of view
and their transfer from the mud to water samples. The results are indi­
cated in Table 4.
Generally, the highest transfer factor was noticed for Na followed by
Ca > Mg > Co > Cd > K > Cr > Ni > Zn > Mn > Pb > Cu > Fe. Sample 8
is characterized by the lowest transfer factors for most of the major
cations and part of the heavy metals (Cd, Pb and Zn). Fe is characterized
by the lowest transfer factor for all samples, followed by Ni, Cr and Zn in
the case of sample 4.
3.4. Water quality index (WQI)
The WQI was based on the results of 12 physico-chemical parameters
(pH, EC, NH+ -
4 , NO2, NO3, Cl , Ht, turbidity, Na, Ca, Mg, and K) and on the
– –
standard values established by the International and National Regula­
tions (Law 311, 2004; WHO 2004 and WHO, 2011) concerning water
quality.
The WQI results indicated that the studied water samples were
classified in three quality levels. Generally, water samples were char­
acterized with excellent quality, while samples 4 and 1 with poor and
good quality, respectively (Fig. 5).
The WQI scores were ranging between 8.6 and 54, with an average of
22. Other studied found higher results, ranging between 89.9 and 325,
indicating poor quality due to industrial activities (Rahman et al., 2020).
While in Mokopane (South Africa), the anthropogenic activities alter the
quality of water. WQI scores ranged from 120 to 4644, indicating poor
quality for the studied aquifer samples to unsuitable for drinking pur­
poses (Molekoa et al., 2021).
The lowest values were obtained for sample R6, followed by 10 < 11
< 7 < 12 < 2 < 9 < 5 < 3 < 8 < 1 < 4. The last two categories are linked
to the high concentrations of NH+ 4 , CE, total hardness and TDS. The
mentioned physico-chemical indicators exceeded the maximum allow­
able concentrations regarding the water quality. Results considering the
correlation between the WQI scores and the physico-chemical charac­
teristics are indicated with the help of the correlation matrix (Table 5).
Positive correlations can be observed between EC and SO2- 4 , EC and TDS,
TDS and SO2- 4 , TDS and EC, Ht, EC and TDS.
4. Conclusions
The chemistry of studied water samples from the Ronișoara Forest
protected area is impressive. Although the alluvial aquifers are located
in a protected area, they are rich in diverse chemicals coming from
2-
natural or anthropogenic sources. Mn, Fe, NH+ 4 and SO4 expressed as the
mean value of all 12 samples sets, exceed the MACs regarding the
drinking water quality, mainly caused by water–rock interactions,
dissolution of fertilizers in agricultural practices.
The typology of aquifers is of Ca-HCO–3 type, characterized by HCO–3
and Ca dominated, followed by SO2- -
4 , Mg, Cl and Na + K.
Generally, waters are also rich in Ca and heavy metals, Pb, As, Al,
Mn, Fe and Se. Two pollution evaluation indices (Heavy metal Pollution
Index, HPI and Heavy metal Evaluation Index, HEI) were used in order
to evaluate the pollution status with heavy metals (As, Cd, Cr, Cu, Fe,
Mn, Ni, Pb and Zn), characterizing 12 alluvial aquifers from a protected
area (Ronisoara Forest). HEI and HPI scores indicated three levels of
pollution. The majority of samples were characterized by a low pollution
level, one sample with medium pollution level and five out of the twelve
samples were characterized by a high level of pollution.
The Water Quality Index (WQI) used in the study was based on 12
physico-chemical indicators. The results indicated three quality statuses,
generally excellent and two with poor and good quality levels. Ac­
cording to the correlation matrix, the WQI scores were positively
2-
correlated to the NH+ 4 , TDS, total hardness, EC and SO4 amount.
Protection policies must be outlined and enclosed in order to protect
the natural environments, as part of protected areas.
CRediT authorship contribution statement
Thomas Dippong: Conceptualization, Methodology, Investigation,
Formal analysis, Writing – original draft, Writing – review & editing.
Maria-Alexandra Hoaghia: Formal analysis, Methodology, Writing –
original draft, Writing – review & editing. Marin Senila: Formal
analysis.

10
T. Dippong et al. Ecological Indicators 143 (2022) 109347

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the work reported in this paper. M., Noor, A., Umaru, I., Almahbashi, N.M.Y., 2020. Water quality hazard assessment
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Khadija, D., Hicham, A., Rida, A., Hicham, E., Nordine, N., Najlaa, F., 2021. Surface
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