Articulo sobre la distribución de metales pesados

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Marine Pollution Bulletin
journal homepage: www.elsevier.com/locate/marpolbul
Spatial distribution and environmental geochemistry of zinc metal in water
and surficial bottom sediments of Lagoon Burullus, Egypt
Abd El-Monsef Ahmed El-Badrya,⁎
, Ahmad Mohamed El-Kammarb
a
National Institute of Oceanography and Fisheries, Aswan Research Station, Egypt
b
Department of Geology, Faculty of Science, Cairo University, Egypt
A R T I C L E I N F O
Keywords:
Lagoon Burullus
Bottom sediments
Pollution
Zinc fractionations
Egypt
A B S T R A C T
Lagoon Burullus is located in the North West quadrant of the Nile Delta. It receives drainage water through
several drains around the lagoon. Understanding the mobility and bioavailability of zinc metal in bottom se-
diments of Lagoon Burullus is essential for the design of remediation processes and the institution of environ-
mental recommendation for zinc pollution.
Single extractions used to fractionate zinc into five fractions. The chemical analyses preceded using atomic
absorption spectrometry after using the digestion technique. Zinc concentrates in the residual fraction
(167.5 μg/g) followed by the organic (14.6 μg/g), exchangeable (3.2 μg/g), carbonate (2.4 μg/g) and then the
Fe-Mn hydroxides (1 μg/g) fractions. The average content of zinc (189 μg/g) is about three fold the average
earth's crust.
Ecological pollution index show that the metal has a low-risk assessment to surrounding ecosystem. The
anthropogenic activities considered as the main source of pollution.
1. Introduction
Zinc is an essential element, which is important for plants, animals,
and humans for physiological and reproductive functions. The max-
imum allowable limit (MAL) of Zn for worldwide soils is 300 ppm
(Kabata-Pendias, 1995). Applications of Zn fertilizers can temporarily
help offset plant Zn deficiency symptoms. Hence, it is important to have
a better understanding of the transformation of soil zinc fractions. This
helps in understanding the zinc species and its availability to plants.
Zinc metal can be drained to an aquatic ecosystem by human ac-
tivities. Several drains around the Lagoon Burullus throw agricultural
and industrial wastewaters. Furthermore, Brimbal Canal, situated at the
western side of the lagoon, throw fresh water into the lagoon. However,
during the last few decades, the environment of the lagoon changed
seriously due to the contribution of several new drains which dug to
relocate agricultural and industrial wastes to the lagoon.
Many authors, e.g., Harter (1983), Calmano et al. (1993), Dho and
Lee (2003), Chakraborty et al. (2014), Wojtkowska et al. (2016), and
Lin et al. (2016), studied the role of pH, Eh, bioturbation or resuspen-
sion, grain size, organic matter content among other factors on the
accumulation of heavy metals in bottom sediments. According to
Bastami et al. (2017) monitoring of heavy metals deposition in sedi-
ments provides a continuous surveillance of pollution in the aquatic
system and for advisable controlling on pollution.
Lagoon Burullus (UNESCO-protected area), like other
Mediterranean lakes of Egypt, suffer from growing deterioration due to
the unsupervised actions, especially during the last few decades. El-
Asmar et al. (2013) reported that during the 1970s, the lagoon body
was quite far from human intervention and the lake was one of the least
polluted coastal lagoons in Egypt. The building of the high dam in the
1960s, affected the irrigation regime in the Nile Delta and necessitated
large irrigation and drainage network. The expanded reclamation ac-
tivities, especially in the southern and southwestern fringes and the
landward movement of sand dunes, caused a drop in the open water
surface area.
El-Sheikh et al. (2012) studied the crucial parameters controlling
the plant resettlement on soil dredged from the outlet of Lagoon Bur-
ullus to the Mediterranean Sea and deposited nearby, forming by this
way new land that underwent a primary plant succession. Hossen and
Negm (2016) reported changes in the water body of Lagoon Burullus
due to the severe anthropogenic activities. The agriculture area in-
creased by 45.52% (10,529.02 ha), while the sand bar and urban area
decreased mostly by the same amount during the period from 1984 to
2015. Khalil and El-Gharabawy (2016) added that lately, the lagoon
becomes a sediment sink, which led to shrinking in its area and depth
accompanying with increasing contaminant levels, especially by heavy
http://dx.doi.org/10.1016/j.marpolbul.2017.10.002
Received 6 August 2017; Received in revised form 2 October 2017; Accepted 3 October 2017
⁎
Corresponding author.
E-mail address: amkammar@hotmail.com (A.E.-M.A. El-Badry).
Marine Pollution Bulletin xxx (xxxx) xxx–xxx
0025-326X/ © 2017 Published by Elsevier Ltd.
Please cite this article as: El-Badry, A.E.A., Marine Pollution Bulletin (2017), http://dx.doi.org/10.1016/j.marpolbul.2017.10.002

2. metals. Recently, El-Zeiny and El-Kafrawy (2017) applied remote sen-
sing and GIS to assess water pollution in Lagoon Burullus. Total ni-
trogen (TN), total phosphorus (TP) and the biochemical oxygen demand
(BOD) selected to evaluate water pollution and levels of water dete-
rioration in the lagoon. They concluded that the eastern and southern
parts of the lake are the most polluted due to the excessive human
activities, particularly from agricultural and domestic sources.
Shokr et al. (2016) confirm that the sediment adjacent to lagoon
represent a hazard to human life in the area, where inc content greatly
exceeded permissible limits (377.6 mg/kg). This could be caused by
infiltration of irrigation water through the studied area. Zn contents are
higher than the 52 mg/kg average of the upper lithosphere (Wedepohl,
1995) and lower than the maximum permissible value of 200 mg/kg
(CSQG, 2007).
El-Amier et al. (2017) stated that the lagoon sediments work as
important sources of different toxic pollutants such as heavy metals,
which in turn accumulate in aquatic organisms through food chains.
The main aim and objectives of this manuscript is to map water and
bottom sediment pollution for zinc metal and its fractionation in the
lagoon using original chemical analysis data.
2. Materials and methods
Fourteen sites, covering the Lagoon Burullus body, considered for
sampling during summer 2014. Table 1 shows the details of longitude
and latitude of the sampling locations, each site represents bottom se-
diment and surface water samples. In addition, seven bottom sediment
samples collected near from the agricultural drains (Fig. 1). The bottom
sediments were collected from the lagoon using a grab sampler (Ekman
type), which was immersed to a depth ranging between 60 cm and
450 cm. The preparation of sediment for total zinc content analysis was
done where the surface bottom sediment samples were air-dried, grind
and preserved for chemical analyses.
The chemical analyses for the zinc performed for whole sediment
and the five sequential extraction fractions by atomic absorption
spectrometry (Perkin-Elmer 3110, USA) with graphite atomizer HGA-
600, after using the digestion technique according to the standard
APHA (1998).
2.1. Sequential fractionation methods
The sequential extraction procedure described by Tessier et al.
(1979) and modified by Rao et al. (2008) adopted in the present study
(Table 2).
The exchangeable extracted with 8 ml of 1 M 2MgCl2 at neutral pH
for 1 h. The carbonate-bound fraction (F2) extracted with 8 ml of 1 M
sodium acetate adjusted to pH 5.0 with acetic acid (for 5 h). The Fe-Mn
oxyhydroxides bound fraction (F3) extracted with 0.04 M hydro-
xylamine hydrochloride in 25% Acetic acid (v/v) at 96 °C with occa-
sional stirring for 6 h. The organic-bound fraction (F4) extracted with
3 ml of 30% hydrogen peroxide in 0.02 M nitric acid (adjusted to pH 2
with HNO3). The mixture then heated to 85 °C for 2 h with occasional
stirring. The crystalline residual/lithogenic fraction (F5) obtained by
complete digestion of the residue with aqua-regia in a digestion bomb.
Table 1
Longitude and latitude of the sampling locations.
Station Latitude Longitude Station Latitude Longitude
1 31°32′28.3″N 31°03′42.4″E 12 31°24′54.5″N 30°41′56.6″E
2 31°33′31.0″N 31°01′03.0″E 13 31°28′09.0″N 30°56′07.6″E
3 31°34′02.5″N 30°59′22.4″E 14 31°28′52.3″N 30°58′53.2″E
4 31°33′30.5″N 30°56′53.7″ E 15 31°24′52.9″N 30°36′28.5″E
5 31°32′47.2″N 30°54′41.1″E 16 31°24′02.3″N 30°36′50.7″E
6 31°31′46.8″N 30°51′47.5″E 17 31°24′57.4″N 30°39′32.0″E
7 31°30′21.5″N 30°48′54.5″E 18 31°26′13.1″N 30°46′58.8″E
8 31°29′08.8″N 30°46′11.3″E 19 31°26′33.4″N 30°49′24.7″E
9 31°28′00.3″N 30°42′58.5″E 20 31°29′14.3″N 30°52′42.7″E
10 31°27′37.4″N 30°42′56.6″E 21 31°26′34.2″N 30°53′39.3″E
11 31°26′59.5″N 30°43′33.6″E
Fig. 1. Location map of the sampling sites.
Table 2
Summary of the sequential extraction steps of Zn fractionation.
Step Fraction Reagent Experiment conditions
F1 Exchangeable 8 ml of 1 M 2MgCl Shake for 1 h at neutral pH
F2 Carbonate-bound 8 ml of 1 M sodium
acetate
Shake for 5 h at pH 5.0
F3 Fe-Mn 0.04 M NH2OH·HCl,
CH3COOH
Shake for 6 h at pH 2
(96 °C)
F4 Organic-bound 3 ml of H2O2 in 0.02 M
HNO3
Shake for 2 h at pH 2
(85 °C)
F5 Residual Mixture of 3 HF-HCI/
HNO3
16 h at 80 °C in a digestion
bomb
A.E.-M.A. El-Badry, A.M. El-Kammar Marine Pollution Bulletin xxx (xxxx) xxx–xxx
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3. 3. Results and discussions
3.1. Zinc metal in lagoon water
Zinc metal content of the investigated lagoon water ranged from
0.7 μg/L to 3.6 μg/L, with an averaging 2 μg/L (Fig. 2A, Table 3). In
general, the content increases toward the northeastern direction pos-
sibly due to flocculation processes near to the lagoon inlet.
3.2. Geochemical backgrounds
The average of Zn content for surfacial bottom sediments of the
present work (189 μg/g) is about three fold the average earth's crust
(70 μg/g) as quoted by McLennan and Taylor (1999).
The metal content of the investigated sediments fluctuates between
95 μg/g and 758 μg/g averaging 188 μg/g. The frequency distribution
of the Zn is unimodal having a maximum at about 150–200 μg/g
(Table 4 and Fig. 2B). The highest concentration of Zn represents more
than two-fold and half-fold the MPL (300 μg/g) of soil as quoted by
Kabata-Pendias (1995).
Discharging from El-Gharbia drain can explain the increase of Zn in
the lagoon's water. This drain discharges industrial and agricultural
wastewater directly into the lagoon. The industrial wastes mostly de-
rived from El-Mahalla El-Kobra factories. The distribution of zinc in
bottom sediments shows an increase toward the north and northeastern
sides of the lagoon, forming two high concentrated spots (Fig. 2C).
3.2.1. Fractionation of zinc metal in the studied lagoon
The geochemical phases at each extraction phase are largely oper-
ationally defined and indicate relative rather than absolute chemical
speciation. The solubility of metals is the main interpretations of the
fractionation approach. According to Rieuwerts et al. (1998), the
bioavailability of metal in sediments depends on their distribution be-
tween the solid and solution phases. This distribution is due to the soil
processes of cation exchange, specific adsorption, precipitation and
complexation and pH value. The mobility and bioavailability of metals
decrease approximately in the order of extraction sequence and hence
the strength of the chemical reagents used in extraction increases with
the sequence. The obtained geochemical maps of the sequential ex-
traction results illustrate that different anthropogenic activities affect
the zinc speciation pattern.
3.2.2. Dissolved or exchangeable fraction
Zinc metal in the exchangeable fraction held by electrostatic ad-
sorption represent the most mobile and readily available for biological
uptake in the environment thus this fraction considered as a pollution
indicator (Zakir, 2008).
The concentration of metals in this phase indicates the environ-
mental impact. In the sediments of Lagoon Burullus, Zn associated with
the exchangeable fraction ranges between 1.4 μg/g and 7.9 μg/g,
averaging 3.2 μg/g. This concludes that the exchangeable (bioavail-
able) fraction of Zn is insignificant suggesting low health risk. El-
Gharbia and the eastern Burullus drains continuously discharge was-
tewater that supply the bioavailable zinc to the lagoon (Fig. 3A).
3.2.3. Carbonate-bound fraction (acid soluble)
It has been reported by Gleyzes et al. (2002) that trace metals ex-
tracted from soil and sediments with sodium acetate (1 M) adjusted to
pH 5 may have also been specifically sorbed to low energy sites on the
surfaces of clay minerals, organic matter, and oxide minerals. There-
fore, heavy metals recovered within this fraction are not strongly bound
and can be released in acidic conditions (pH < 5). In the present
study, the carbonate fraction accounts for a relatively less quotient than
the exchangeable fraction, where the content fluctuatesbetween0.5 and
6.8 μg/g with an average 2.4 μg/g (1.27% of the total metal con-
centration). The speciation pattern of the carbonate in this fraction
suggests lower environmental risk. The distribution of the carbonate-
bound Zn in the studied sediment increases toward the eastern,
southeastern and extreme western sides of the lagoon, where agri-
cultural and human activities dominate (Fig. 3B).
3.2.4. Fe-Mn oxy-hydroxidesfraction (reducible)
In comparison with carbonate minerals, Fe-Mn oxide minerals have
relatively large area and surface site density (Forstner and Wittmann,
1983). The Fe-Mn oxide, the reducible phase of the soil under oxidizing
conditions is a significant sink for the heavy metals. However, the
speciation results of the present work documents in significant con-
tamination risks of zinc associated with Fe-Mn oxy-hydroxides fraction.
Zinc associating the Fe-Mn oxy-hydroxides fractions preads over most
of the lagoon area but at low content, averaging 1 μg/g (Table 3 and
Fig. 3C).
3.2.5. Organic fraction (oxidizable fraction)
The organic matter plays an important role in the distribution and
dispersion of metals by mechanisms of chelating and cation exchange.
In this phase, a reaction between a metal ion and an organic ligand
Fig. 2. Spatial distribution map of zinc by μg/L in the studied water lagoon (A), frequency
distribution of zinc in the studied lagoon sediment (B) and geochemical map of zinc by
μg/g in the studied lagoon sediment (C).
A.E.-M.A. El-Badry, A.M. El-Kammar Marine Pollution Bulletin xxx (xxxx) xxx–xxx
3

4. leads to a species, which either can precipitate directly or adsorbed on
soil materials. The organic-bound Zn represents 7.98% of the total
metal budget. Organic fraction decreases toward the middle portion of
the lagoon, suggesting that the main part of zinc is possibly anthro-
pogenic derived from agricultural drains (Fig. 3D).
3.2.6. Residual fraction
The residual fraction is concerned with the most stable and least
bioavailable of all the chemical fractions of the sediments. In this
fraction, metals are confined within the crystal lattice of silicates and
well-crystallized oxide minerals. The residual fraction is a major carrier
of metals in most environmental systems. The percent of this fraction
can be taken as a guide to the degree of non-availability of metals to
biota or diagenetic processes except over long time scales (Tessier et al.,
1979). Zinc content shows an increase toward the outlet of the lagoon
toward the north and northeastern sides (Fig. 3E), reflecting their li-
thogenic natural association in the crystalline silicate mineral sand the
most inactive.
The maximum content of zinc concentrates in the insoluble fraction,
which represents an average about 88.7% of the total zinc. The organic
fraction accumulates important quotient of zinc in lagoon sediments,
averaging 7.7%, whereas the exchangeable and carbonate fractions
represent only about 3% of the total zinc. The Fe-Mn oxyhydroxides
fraction represents the least contribution of about 0.5% of the total zinc
content, in average. The average data of zinc speciation in Lagoon
Burullus sediments suggest the following order of abundance: residual
fraction > organic fraction > exchangeable fraction > carbonate
fraction > Fe-Mn oxy-hydroxides fraction.
It is noticeable that there is a similar between the concentration of
zinc in the residual phase (167.5 μg/g) and the source rocks of the
adjunct wild mass, according to Rifaat (2005), the concentration of zinc
in the adjacent deposits ranges between 11 μg/g and 221 μg/g.
In average, the exchangeable, carbonate, organic and Fe-Mn oxy-
hydroxides fractions collectively represent 11.3% of the total zinc,
whereas the non-available residual fraction represents 88.7% of the
total zinc. The above date suggests that the metal has low contamina-
tion risk in lagoon environment.
3.2.7. The regional pollution index (RPI)
The degree of pollution of the Lagoon Burullus bottom sediments
can be calculated by normalizing the metals concentration to their
Maximum Permissible Limits (MPL) used for the worldwide soil. In the
given equation of the pollution index, the MPL of an element is con-
sidered as the “pollution standard level or goal”. The following equa-
tion calculates regional pollution index (RPI):
= ×RPI Pollution concentration 50/Pollutant standard level or goal
For each region, the highest calculated index is used as the RPI for
that region. An RPI of 50 corresponds to the relevant standard/goal.
The RPI is categorized as low, medium or high, as follows: low pollution
index from 0 to 24, medium pollution index from 25 to 49, and high
pollution index 50 or higher.
In the present work, the bottom sediments have RPI of medium
pollution level by the total zinc content.
3.3. Enrichment factor (EF)
Enrichment Factor is considered as an effective tool to evaluate the
magnitude of contaminants in the environment. Iron (Fe) was chosen as
the controlling element. The enrichment factor for zinc metal was cal-
culated from the formula quoted by Rule (1986) and Rubio et al.
(2000):
=Enrichment Factor (EF) (M/Fe) /(M/Fe)sample background
Table 3
Concentrations of zinc in water μg/L, bottom sediments μg/g and five steps of zinc fractionations data of bottom Burullus Lagoon sediments μg/g.
Stations Total zinc content Zinc fractionations in sediments μg/g
In water
μ g/L
In sediments
μg/g
(EXC)
Exchangeable
(CA)
Carbonate bond
(FM)
Fe-Mn hydroxide bond
(OM)
Organic bond
(RES)
Insoluble
1 2.600 178.0 3.700 5.400 0.100 12.40 156.5
2 3.200 192.0 7.900 0.700 0.800 31.20 151.4
3 3.400 183.0 6.200 6.800 1.500 14.50 154.0
4 3.600 758.0 2.500 3.200 1.400 0.500 750.4
5 2.000 126.0 1.800 1.200 0.100 13.70 109.3
6 1.200 218.0 2.700 1.000 0.100 17.80 196.5
7 0.700 162.0 1.400 2.400 0.300 0.100 157.8
8 1.600 221.0 2.400 1.400 8.400 18.40 190.4
9 1.000 112.0 3.100 1.400 0.500 8.800 98.20
10 1.000 128.0 1.900 2.200 0.100 19.10 104.8
11 2.300 199.0 4.200 1.500 0.100 12.20 181.1
12 1.500 147.0 2.000 0.500 1.400 0.100 143.1
13 1.600 111.0 2.300 0.700 0.100 14.00 94.00
14 2.100 129.0 2.500 3.200 0.100 13.60 109.7
15 2.000 111.0 1.800 0.900 1.000 15.70 91.60
16 1.900 158.0 2.000 1.600 0.100 9.800 144.6
17 1.900 95.00 2.600 1.100 2.900 16.60 71.80
18 1.700 183.0 3.200 4.300 0.100 14.70 160.8
19 1.600 193.0 5.000 4.500 0.100 14.60 168.9
20 1.600 166.0 4.700 5.700 2.300 2.000 151.3
21 1.600 194.0 2.600 1.400 0.400 57.50 132.1
Average 1.700 188.8 3.200 2.400 1.000 14.60 167.5
Max 3.600 758.0 7.900 6.800 8.400 57.50 750.4
Min 0.700 95.00 1.400 0.500 0.100 0.100 71.80
Standard deviation ± 0.800 ± 135.7 ± 1.600 ± 1.900 ± 1.900 ± 12.30 ± 137.9
Table 4
Frequency & distribution data for Zn μg/g for 21 bottom lagoon sediments.
Bin Lower Upper Count Percent Total Percent
1 95 100 1 4.8 1 4.8
2 100 150 7 33.3 8 38.1
3 150 200 10 47.6 18 85.7
4 200 250 2 9.5 20 95.2
5 250 758 1 4.8 21 100
A.E.-M.A. El-Badry, A.M. El-Kammar Marine Pollution Bulletin xxx (xxxx) xxx–xxx
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5. where M is the concentration of metal. The background value is that of
average shale, obtained by McLennan and Taylor (1999).The EF va-
lues: < 2 indicate that the metal is entirely from crustal materials or
natural processes, > 2 suggest that the sources are more likely to be
anthropogenic, 2–5 moderate enrichment, 5–20 significant enrich-
ment,20–40 very high enrichment, and > 40 extremely high enrich-
ment.
The enrichment factors (Ef) of total zinc content, is moderate.
3.4. Geoaccumulation index (Igeo)
The geoaccumulation index (Igeo) as defined by Müller (1969); en-
ables an assessment of the enrichment degree by considering the an-
thropogenic pollution, the geochemical background values, and the
effect of natural diagenesis. The Igeo was computed using the following
equation:
= ×I log2 (C /1.5 B )geo n n
where, Cn measures the concentration of an element n in sediments,
and Bn is the geochemical background value of the element n according
to McLennan and Taylor (1999).A constant of 1.5 is used due to a given
metal fluctuations in the soils as well as some very small anthropogenic
influences (Loska et al., 1997). The geo-accumulation index consists of
seven classes or grades. The Igeo values: < 0 indicate that the metal is
Uncontaminated, From 0 to 1 suggest that Uncontaminated to moderate
contaminated, From 1 to 2 Moderate contaminated, From 2 to 3
Moderate to heavily contaminated, From 3 to 4 Heavily contaminated,
From 4 to 5 Heavily to extremely contaminated, > 5 Extremely con-
taminated. The highest class (six) reflects a 100-fold enrichment above
the background values (Förstner et al., 1990).
The calculated geoaccumulation index (Igeo) indicates an un-
contaminated state of the studied bottom sediments by zinc metal.
4. Conclusions
Lagoon Brullus is one of four shallow northern coastal lakes of
Egypt. It receives a huge quantity of agricultural, industrial, municipal
and domestic wastewater, in addition to navigation and fishing activ-
ities. The analyzed Zn element in water has distribution increase toward
a northeastern direction due to flocculation processes close to her la-
goon inlet. Also, the content of Zn in the lagoon water have con-
centrations higher than those in Mediterranean Sea water, which in-
dicate the influence of the dumping wastewater of different sources into
the lagoon.
Based on chemical analysis data and the calculated geoaccumula-
tion index, enrichment factor and the regional pollution index, the
bottom sediments of the Lagoon Burullus have markedly low to mod-
erate degree of pollution. The spatial distribution of zinc metal in the
Lagoon Burullus reveals that the agricultural wastewater supplied by
El-Maksaba and Mastarouh villages, and the industrial wastewater
brought by El-Gharbia drain are the main contributors of pollution. The
speciation of Zn suggests that the residual fraction is the main carrier of
zinc (88.7% of total content). A significant percentage of the metal
occurs in the organic matter fraction (7.73% of total content).The
speciation and bioavailability of zinc follow the order;
RES > OM > EXC > CA > Fe-Mn at concentrations; 167.5, 14.6,
3.2, 2.4, 1 μg/g in average, respectively.
Acknowledgment
The authors are grateful to the team of Baltim research station for
Fig. 3. Geochemical map of exchangeable zinc fraction (A), carbonate fraction (B), Fe-Mn
oxy-hydroxides fraction (C), organic fraction (D) and residual zinc fraction (E) in the
studied lagoon sediment.
A.E.-M.A. El-Badry, A.M. El-Kammar Marine Pollution Bulletin xxx (xxxx) xxx–xxx
5

6. facilities provided in sampling collections.
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