http://www.revistadechimie.ro REV.CHIM.(Bucharest) ♦67♦No. 9 ♦2016 1728Researches on Heavy Metals Determination from Water and Soil in Galati County,… [625440]

http://www.revistadechimie.ro REV.CHIM.(Bucharest) ♦67♦No. 9 ♦2016 1728Researches on Heavy Metals Determination from Water
and Soil in Galati County, Romania
CARMEN PENELOPI PAPADATU1, MARIAN BORDEI1, GHEORGHE ROMANESCU2,3, ION SANDU2,4*
1 Dunarea de Jos University of Galati, Faculty of Engineering, 111 Domneasca Str.,800008, Galati, Romania
2 Alexandru Ioan Cuza University of Iasi, ARHEOINVEST Interdisciplynary Platform, 22 Carol I Blvd., Corp G, 700506, Iasi,
Romania
3 Alexandru Ioan Cuza University of Iasi, Faculty of Geography and Geology, 22 Carol I Blvd., Corp G, 700506, Iasi, Romania
4 Romanian Inventors Forum, 3 Sf. Petru Movila St., Bl. L11, Sc. A., III/3, 700089, Iasi, Romania
This work presents a monitoring study accomplished on water and some soil samples collected from some
points of Danube River and from other two locations situated in Galati County, from Romania. Water samples
were collected from four points in Danube River, one point in Prut River (Oancea city) and from one point in
Vadeni village (water from fountain). The heavy metals concentrations were determined using the Atomic
Absorbtion Spectroscopy (AAS) Technique, together with some physical parameters. The soil samples
were studied using two complementary techniques: X-Ray Fluorescence (XRF) and Scanning Electron
Microscopy (SEM). It explores the possibility of the existence of a correlation between the concentration of
heavy metals from surface waters and the concentration of heavy metals in soil in order to assess the
contamination as a result of anthropogenic activities.
Keywords: heavy metal determination; water and soil monitoring; anthropogenic contamination; AAS,
SEM-EDX and XRF techniques
The total complex of ecosystem is known as the
biosphere, because it comprises the surface layer of theplanet capable of supporting life. People must take in
consideration the rules which govern the health and
functioning of the biosphere because, if these rules are notrespected, the life must disappear.
The plants and animals able to exist in any area will
form a biotic community. Essentially, an ecosystem is abiotic community in interaction with its physical
environment of sunlight, atmosphere, water and soil or
rock. In this ecosystem for each species exists as apopulation, the growth or it decline which are affected by
the capacity of the system to provide the requirements of
life [1].
W ater is an obvious limiting factor for plants and animals.
The plants are classified in relation to their tolerance for
dry, medium or wet conditions as:
xerophytes, mesophytes
and hydrophytes . Most land plants are in the intermediate,
mesophytic range; desert plants are usually xerophytes;
hydrophytes grow in water or require an abundance of
water in the soil. All plants require water to support their
active growth and metabolism [2].
Exposure to environmental toxicants can have profound
effects on normal growth and development. Many
environmental toxicants as the heavy metals from soil and
water can alter the reproductive function and they can haveeffects on the central nervous system and behaviour. The
link between these reproductive and neurologic
phenomena has not been systematically investigated yetbut we know that the heavy metals existents in water and
soil have bad consequences on human body, plants and
animals. The neuro-endocrine (hypothalamic-pituitary-gonadal) system, which integrates inputs and outputs from
the nervous and reproductive systems, is functionally and
anatomically situated to mediate the effects ofenvironmental toxicants, particularly those that are
endocrine-disrupting chemicals (EDCs), in case of
developmental processes [1].
* email: ion.sandu@uaic.roOver 90% of Cd, Pb, Mn, Ni, Cu and Zn contents present
in freshwater and sediments originates from humanactivities [3], associate with suspended particulate matter
which settle and are accumulated in the bottom sediment.
In literature was shown that heavy metals concentrationsin aqueous phase decreased while they increased in the
solid phase (as material in suspension and/or sediment)
and in biota, conclusion which is useful in performing ofassessment of water quality and the heavy metals pollution
impact on coastal ecosystems [4-6].
In this paper it is presented a study accomplished on
water and soil samples. This work analyzed the
concentration of heavy metals from surface waters and
concentration of heavy metals (Cu, Zn) in soil in order toassess the contamination as a result of anthropogenic
activities. Main sources of pollution affecting the complex
come from industrial area (mainly Metallurgical industry)of the Galati city, from the core Port and from the Danube
(practically is the end area after 9 countries and many
industrial and agricultural pollution sources) [3].The watersamples were collected from three points in Danube River,
one point in Prut River (Oancea city) and from one point in
Vadeni village (water from fountain). The hydrographical
basin of the Prut River is located in the north – east of the
Danube basin with a catchment area of 27500 km2 being
developed on the territory of the following three countries:Ukraine, Romania and Moldavia.
In Romania, the area of the Prut River basin has 10967
km
2. There are many sources of water along the Prut River
and Danube River [7-10]. In figure 1 was presented a map
of the hydrographic basin of the Prut River and partially, we
can observe the Danube River corresponding to Galati area[11].
Beside the water analysis, it was accomplished a
chemical and structural analysis of soil. The soil sampleswere collected from different depths for analyses using X-
Ray Fluorescence (XFR) and Scanning Electron Microscopy
(SEM) Technique In table 1 were presented some

REV.CHIM.(Bucharest) ♦67♦No. 9 ♦2016 http://www.revistadechimie.ro 1729permissible values for heavy metals in water and indicators
[12-15]. This study was realized during the followingperiod: 04.01.2014 – 07.01.2014.
Experimental part
Materials and methods
For the water samples we considered for this study
sampling sites (stations) such as: ( S1) – Prut (Oancea
45°00' N and 28°07' E) and the measures were done in two
days: in 04.18.2014 and in 05.21.2014; ( S2) – the mouth
spill of Siret River in Danube (the Bridge Galati-Braila) andthe measures were done in two different days: 05.20.2014
and 06.30.2014; (
S3) – Danube River (Braila Cliff) and the
measures were done in the days: 05.20.2014 and06.30.2014; (
S4) – Danube River (Galati Cliff, near the ore
carrier Port) and the measures were done in the days:
05.20.2014 and 06.30.2014; ( S5) – V adeni Village in Galati
County (water fountain) and the measures were done in
04.20.2014 – before the floods.
Galati is the county seat. Oancea village is documented
in 1521 during the rule of Stefan Voda. It is situated in the
Eastern part of Romania, on the right bank of the Prut River,
at 57 Km north of Galati town and 7 Km West of the towncalled Cahul in Moldavia Republic.
Methods used for water analysis
The monitoring process of water quality was made in
accordance to the National Integrate System of Monitoring
of Romanian Waters. The samples procedure is accordingto APHA. At each sampling time, the following chemical
and physical parameters were analyzed: water debit,temperature,
pH, Cu2+, Zn2+ etc. The physical values were
obtained on situ by means of a multiparameter type WTW
Multi350i. The concentrations of the heavy metals (forexample, Cu
2+, Zn2+) were determined using the AAS
(Atomic Absorption Spectroscopy) method. The analyses
were carried out at the laboratory of the Materials andEnvironment Quality Centre from Dunarea de Jos University
– Faculty of Engineering.
Methods used for soil analysis .
The soil samples were studied using two techniques: X-
Ray Fluorescence (XRF) and Scanning Electron Microscopy(SEM). The collected soil samples were dried and all the
roots and rocks were removed. For the SEM analysis the
samples were sieved and pressed to a carbon tape.
Results and discussions
Experimental results have enabled a short monitoring.
Seasonal averages of physical parameters for Prut River
point (
S1) ranged the records between 90.18 and 351.5
m3/s for flow water; 5.55 and 21.18oC for temperature and
7.8-8.1 for pH value. The water debit in the studied zone for
S1 had an average value approximately 100 m3/s. The debit
was relatively constant. The seasonal variation of thetemperature was within the normal range.
In figures 2 and 3 were presented some heavy Metals
(Cu
2+, Zn2+) concentrations from water, for zone S1 (Prut
River – Oancea zone). For this zone, in May, the
concentration of Cu2+ was higher than the value from April.
The value was 0.22 mg/L in April and it was 0.27 mg/L inMay. The concentration of Zn
2+ from water was 0.21 mg/L
in April and it was 0.22 mg/L in May, after floods. In this
case, in summer period was observed that Zn2+
concentration decreased.
Fig. 1. The hydrographic basin of Prut River and Danube River
Table 1
PERMISSIBLE
VALUES FOR
HEAVY METALS IN
WATER AND
INDICATORS
Fig. 2. Cu2+ mean concentration from the water in S1 zone: M1
represents the measured value at 04.18.2014; M2 represents the
measured value at 05.21.2014

http://www.revistadechimie.ro REV.CHIM.(Bucharest) ♦67♦No. 9 ♦2016 1730For this zone ( S1), at analyzing the samples dated
04.18.2014, besides the heavy metals, were more
determined the following optional: nitrites (0.0082 mg/L),nitrates (9.40 mg/L), phenols (3.60 mg/L), sulfates (211
mg/L). At analyzing the samples dated 05.21.2014, besides
the heavy metals, were more determined the followingoptional: nitrites (0.124 mg/L), nitrates (9.51 mg/L),
phenols (3.86 mg/L), sulfates (235 mg/L). The last results
were obtained after spring floods.
Taking account the
S2 zone, it was made the pH
determination dated 06.30.2014. The value measured in
this case, was 7.17. For the sample dated 05.20.2014, the
pH value was 8.33. The concentration of Cu2+ and Zn2+
from water, in S2 zone, were presented in figures 4 and 5.
For this zone ( S2), at analyzing the samples dated
05.20.2014, besides the heavy metals, were more
determined the following optional: nitrites (0.17 mg/L),
nitrates (13.1 mg/L). At analyzing the samples dated06.30.2014, besides the heavy metals, were more
determined the following optional: nitrites (0.16 mg/L),nitrates (13 mg/L). The concentrations correspond to
normal limits. In this case, in summer period was observed
a decreasing of heavy metals concentrations, most likely
caused by the fixation of pollutants in sediment andvegetation, followed by a higher increasing tendency on
Danube River, possibly caused by the input of industrial
water. The results obtained for
S3 zone are presented in
figure 6 and 7.
For this zone ( S3), at analyzing the samples of water
from the River (on the coast) dated 05.20.2014, besidesthe heavy metals, were more determined the following
optional: nitrites (0.14 mg/L), nitrates (9.10 mg/L), phenols
(3.7 mg/L). At analyzing the samples dated 06.30.2014,besides the heavy metals, was more determined the
following optional: (0.15 mg/L) and nitrates (9 mg/L). The
pH value was 8.03, in normal limits. Cooper registeredvariations between 0.1 mg/L and 0.15 mg/L. In this case, it
is observed that the maximum experimental value is
almost to alert threshold value. The results obtained for
S4
zone are presented in figures 8 and 9.
For S4 zone, at analyzing the samples collected near the
ore carrier Port dated 05.20.2014, besides the heavy metals,were more determined the following optional: nitrites
(0.150 mg/L), nitrates (9.20 mg/L). The
pH value was 6.87.
For the samples dated 06.30.2014 the pH values was 8.07
(after floods). The samples were collected directly from
the coast of the River, near the ore carrier Port, without
Fig. 3. Zn 2+ mean concentration from the water in S1 zone: M1
represents the measuring values at 04.18.2014; M2 represents the
measuring values at 05.21.2014, after floods
Fig. 4. Cu2+ and Zn2+ concentrations from the water in S2 zone
(samples dated 05.20.2014)
Fig. 5. Cu2+ and Zn2+ concentrations from the water in S2 zone
(samples dated 06.30.2014)
Fig. 6. Cu2+ and Zn2+ concentrations from the water in S3 zone
(samples dated 05.20.2014)
Fig. 7. Cu2+ and Zn2+ concentrations from the water in S3 zone
(samples dated 06.30.2014)
Fig. 8. Cu2+ and Zn2+ concentrations from water in S4 zone
(samples dated 05.20.2014)

REV.CHIM.(Bucharest) ♦67♦No. 9 ♦2016 http://www.revistadechimie.ro 1731chemical processing. It can be observed that the
concentration of Cu2+ from the water is higher, especially
after floods. In figure 10 were presented the concentrations
of Cu2+ and Zn2+ from fountain water (V adeni Village)
corresponding to the samples dated 04.18.2014. Copper
registered variations between 0.005 mg/L and 0.150 mg/
L. In this case, it is observed that the maximumexperimental value is close to alert threshold value.
Besides the heavy metals, were more determined the
following optional: nitrites (0.07 mg/L), nitrates (27.50 mg/
L). High concentrations of copper were found in water
because Cooper registered almost 0.18 mg/L. In this case,
it is observed that the maximum experimental valuecorresponds to alert threshold (Quality Class IV-polluted).
The concentration of Zinc from the fountain water was
included in normal limits.
There are differences between the concentrations of
heavy metals (Cu
2+ and Zn2+) from fountain water and the
concentrations of these heavy metals from river(Groundwater v.s. surface water). These differences can
be explained taking into account the human activities
which determine the air pollution, for example. The qualityclasses of the drinking water [34-37] and the limit values
for heavy metals were presented in table 2.
Copper is the most important mineral involved in the
process of photosynthesis and nitrogen assimilation in
Fig. 9. Cu2+ and Zn2+ concentrations from water in S4 zone
(samples dated 06.30.2014, after floods)
Fig.10. Heavy metals concentrations obtained from
fountain (draw well) water sample ( S5 zone)
Table 2
THE QUALITY CLASSES FOR WATER ACCORDING TO [38]plants affect, in the composition of protein complexes, such
as hemocyanin, cytochrome oxidase and lactasetyrosinase [34, 35]. In literature, in unpolluted freshwater
the normal copper content in solution is 0.5 to 2 mg/L and
very polluted is 500-2000 mg/L [34-36]. For Copper indrinking water, we can accept the value of 2 mg/L, if the
distribution pipes are from Copper. In table 3 were presented
the admissible limits according to Ord.756/1997 [33] forless sensitive soil. The results obtained for the soil samples
from Prut (Oancea) zone were presented in table 4. The
samples were collected from different depths.
In figures 11, 12, 13 and 14 were presented the variation
of the heavy metals concentration in soil, depending by
the depth.
Chromium (Cr) element has all the concentrations over
the legal normal threshold and under the legal alert
threshold. The Cr sources are the pigment industry, stainlesssteel and other alloys [35]. This element in soil can be
Cr(III) which is a stabile element and Cr(IV) which is very
toxic for living organisms.
The normal concentration in soil for copper – Cu(II) – is
15 mg/kg. But Cooper registered variations between 19.24
mm/kg (1/5 sample) and 24.54 mg/kg (2/10 sample).Inthis case, it is observed that the maximum experimental
value is over the legal normal thresholds but is under the
legal alert threshold. Zn(II) registered variations between51.08 mg/kg (3/15 sample) and 72.56 mg/kg (2/10
Table 3
ADMISSIBLE LIMITS ACCORDING TO [33] FOR LESS SENSITIVE SOIL
Table 4
ELEMENTS CONCENTRATIONS FOR SOIL SAMPLES (EXPERIMENTAL)

http://www.revistadechimie.ro REV.CHIM.(Bucharest) ♦67♦No. 9 ♦2016 1732sample). In this case, it is observed that the measured
values are smaller than the maximum permissible value
of 100 mg/kg corresponding for legal normal level, as in
literature [35, 39, 40]. In soil, Cu(II), Cr(III) and Ni(II)registered higher concentrations. In both cases (river water
and soil), copper has concentrations over the legal normal
thresholds. Compared with the concentrations from riverwater, appeared differences between the experimental
values. These differences can be explained due to the
existence of the anthropogenic activities such as: industrialwater spilled partial treated, corrosive gas and acid rain,
determined by human activities. In figure 15 was presented
a SEM image where we can identify a soil structure basedon clays and less quart.
There can be observed large particles (5-15 µm) and
discrete particles (0.5 – 2 µm). These particles have
different morphology, such as platy, nodular and spherical.
The dimension of the aggregate is uniform and suggests a
covering with a humic material because there are notevident pores.
Fig. 11. Ni(II) concentration in soil, depending by depth
Fig. 12. Cr(III) concentration in soil, depending by depth
Fig. 13. Cu(II) concentration in soil, depending by depth
Fig. 15. SEM image soil
(sample 1/5, 1000X)
Fig. 14. Zn(II) concentration in soil, depending by depth
Conclusions
There are differences between the concentration of
heavy metals in the waters of the rivers, the concentration
of the heavy metals from soil and from fountain water
because the anthropogenic activity (acid rain, industrialoverflows) existence. Taking into account the admissible
limits for heavy metals in water, the analysed samples
proved that the water is in weighted average polluted (III –rd class of pollution). During the considered period, the
degree of pollution ranges from class II to class IV
(polluted). The pollution intensity is maximum in thesummer period (Class III-IV), in the case of Cu
2+ in water.
The quality of the water of Danube River situated at the
confluence with Prut River corresponds to the Third (III)Class of pollution. This water quality corresponds to the
weighted average polluted limits.
It is important to accomplish a study which reunites
results for water and soil to understand the environmental
pollution in the Galati County region. The heavy metals
concentrations were found in normal values in springperiod, before the floods, in soil and for Zinc (Zn
2+) in water.
The constant monitoring of the Danube River, Prut River
and other water sources is necessary because the wateris an environment that sustains an ecosystem which
depends on the quality of the water and soil. Composition
of river water differs from the composition of water fromthe aquifer since intervenes the air pollution. The study
revealed that the Cu
2+ content in water and sediment
samples from the two studied rivers (except Zn2+ in water
samples) exceeded the maximum permissible
concentration for quality class II (regulated by WFD and
transposed into Romanian legislation by Order No. 161/2006), and it was especially high, this water being affected
by anthropogenic load and the metallurgical industry. It is
also important to take into account the important influenceof the Danube River concentrations on heavy metals
(loaded with pollutants from 9 countries situated
upstream) and the necessity to have global measures inorder to avoid at least the increase of the Danube pollution
in the future.
Acknowledgement: The study on heavy metals determination from
the water was realized in Laboratory from Dunarea de Jos University
of Galati, Romania.
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Manuscript received: 11.04.2016