distribution of uranium and thorium radioelements in...
TRANSCRIPT
JAKU: Earth Sci., Vol. 23, No. 2, pp: 149-168 (2012 A.D. / 1433 A.H.)
DOI: 10.4197 / Ear. 23-2.8
149
Distribution of Uranium and Thorium Radioelements in
Subsurface Pleistocene-Holocene Sediments of the Nile
Delta, Egypt
Yehia H. Dawood and Hamdy Hamed Abd El-Naby
Faculty of Earth Sciences, King Abdulaziz Univ., Jeddah, KSA
Received: 12/12/2011 Accepted: 24/6/2012
Abstract. Collaborative techniques were used to investigate the textural and mineralogical characteristics as well as uranium and thorium contents of the Pleistocene-Holocene subsurface sediments of the onshore area of northern Nile Delta. Fluctuation of water flow during the formation of these sediments resulted in particle sizes variability over time. Approximately 25% of the samples are classified into sand, 20% clayey silt, 18% silty sand, 15% sandy silt and 15% sand-silt-clay. The average uranium content of these sediments is 3.7 ppm and that of thorium is 7.83 ppm. The ranges of Th/U ratio (1.03-4.74) possibly reflect vertical variability based on changes in textures, mineralogical composition and organic matter contents. This variation points to interactions between fluvial, brackish and freshwater regimes, which would be expected to typify a delta setting. Geochemical behaviour of both uranium and thorium is regarded as the essential factor controlling the distribution of the two elements. Zircon, monazite and apatite are the main accessory minerals hosting uranium and thorium. However sorptive uptake of uranium by sediments of relatively high organic matter contents have also played a significant role in uranium adsorption to the sediments.
Keywords: Nile Delta; Uranium; Thorium; Heavy minerals; Subsurface sediments.
Introduction
The naturally occurring radioelements are present in different
concentrations in sedimentary rocks. The fate and transport properties of
150 Y. H. Dawood, H. H. Abd El-Naby
contaminant metals such as uranium and thorium in soils and sediments
are crucial for monitoring and mitigate the dispersion effects of these
elements deep in the subsurface. Different factors affect the distribution
of uranium and thorium in the subsurface sediments including source of
clastic supply to the sedimentary basin, groundwater chemistry,
microbial activity that can affect uranium mobility through direct or
indirect redox changes (Wilkins et al., 2006). In oxic environments,
uranium is typically present as UVI
, in the form of uranyl with two tightly
bound oxygen atoms (UO22+
) that are often relatively mobile. In contrast,
under anoxic conditions uranium is generally present as UIV
, in the form
of hardly soluble mineral phases such as uraninite (UO2), and is,
therefore, considered to be relatively immobile (Langmuir, 1978).
Conversely, thorium is unaffected by redox conditions and remains
insoluble as Th+4
. Understanding uranium speciation in groundwater and
uranium adsorption, precipitation and coprecipitation with soils,
sediments, organic matter such as humic substances, and microorganisms
are all key aspects towards understanding the transport properties of
uranium within the subsurface. Several studies were concerned with the
mineralogy of subsurface sediments of the Nile Delta (e.g. Amer, 1974;
Zaghloul et al., 1980; and El Sisi et al., 1996). Zaghloul et al. (1980)
concluded that the older sediments of Sidi Salem and Abu Madi
Formations are relatively rich in stable minerals compared to the younger
sediments of Kafr El Sheikh and younger formations. The Late
Quaternary subsurface stratigraphy of the northern delta consists of the
older alluvial sand and stiff mud unconformably overlain by shallow
marine to coastal transgressive sand which, in turn, is unconformably
overlain by a variable sequence of Holocene deltaic sand, silt, and mud
(Stanley and Warne, 1993).
The main aim of the present study is to recognize the relation
between distribution of uranium and thorium radioelements in the
Pleistocene-Holocene subsurface sediments of northern Nile Delta and
their mineralogical composition.
Geologic Setting of the Nile Delta
The Nile Delta covers nearly 60,000 sq kms of the northern part of
Egypt. It has, in general, a featureless surface with a northward slope,
except for some limited topographic features such as the Khatatba
Distribution of Uranium and Thorium Radioelements in … 151
positive structural and topographic features, and the westward Wadi El-
Natrun negative element. Generally, no outcrops occur on the Delta
surface, being mainly covered with recent mud and alluvial deposits
(Fig. 1), and also with some sand accumulations known as the Turtle-
backs. At least seven distributaries flowed across the Nile Delta and
discharged into the Mediterranean at various times during the Middle to
Late Holocene (Toussoun, 1922; Stanley and Warne, 1993). Five of these
distributaries became no longer active, leaving only Damietta and
Rosetta branches. The structural setting of the Nile Delta occupies a key
position within the plate tectonic development of the eastern
Mediterranean and the Levant. It lies on the northern margin of the
African plate, which extends from the subduction zone adjacent to the
Cretan and Cyprus arcs, to the Red Sea where it is drifted apart from the
Arabian plate.
Fig. 1. Location map of the study area.
152 Y. H. Dawood, H. H. Abd El-Naby
The subsurface stratigraphic column of the Nile Delta region, after
Ismail et al. (2010), is given in Table 1. The Nile Delta basin contains a
thick sequence of Neogene-Quaternary clastics. According to Stanley and
Warne (1993), the Late Quaternary subsurface stratigraphy of the
northern delta consists of, from bottom to top: alluvial sand and stiff mud
(older than ~12 ka) unconformably (separated by a hiatus) overlain by
shallow marine to coastal transgressive sand (~ 12 to 8 ka). This sand is,
in turn, unconformably overlain by a variable sequence of Holocene
deltaic sand, silt, and mud as old as ~7.5 ka. The overall architecture and
specific environments of deposition within these three sequences record
the interplay of factors that controlled the evolution of the Nile delta.
These factors include sea-level changes, subsidence, climate oscillations,
and sedimentary processes.
The Pleistocene-Holocene subsurface sequence of the Nile Delta is
composed of three main formations namely; Baltim, Mit Ghamr and
Bilqas. Baltim Formation of Early Pleistocene overlies El Wastani
Formation (Late Pliocene) and underlies Mit Ghamr Formation
(Pleistocene). Baltim Formation is composed of intercalations of clay,
sand, shale, with thin bioclastic limestones with numerous Planktonic
foraminiferal species and several benthic species (Ismail et al., 2010).
Based on palaeontological studies, this formation has been dated as Early
Pleistocene (Deibis et al., 1986) and from Pleistocene to Recent (Ismail
et al., 2010).
Table 1. The subsurface stratigraphic column of the Nile Delta (after Ismail et al., 2010).
Age
Formation
Description
Holocene
Bilqas Sand and clays interbeds
Pleistocene Mit Ghamr Clay, sand and silt intercalations
Baltim Clay with sand and argillaceous limestone intrebeds, locally lignitic and silty
Late Pliocene El Wastani Intercalations of sand, shale, clay, with some dolomite and limestone
Middle Pliocene Kafr El Sheikh shale-clay intercalations with some minor occurrences of sands, siltstones, argillaceous limestones, and dolomites
Early Pliocene Abu Madi Intercalations of sand, clay, and shale
Late Miocene
Rosetta Sand with occurrences of anhydrite and clay
Qawaseem sand to sandstone
With a few interbeds of clay.
Sidi Salem intercalations of shale, sand, clay, with rare occurrences of white, bioclastic limestone.
Distribution of Uranium and Thorium Radioelements in … 153
Mit Ghamr Formation overlies Baltim Formation and underlies
Bilqas Formation. The thickness of this formation decreases northward
(Ismail et al., 2010). This formation is composed of intercalations of
clay, sand, and silt, with some limestone. Ismail (1984) dated this
formation as Late Pliocene to Quaternary, while Azzam (1994) ascribed
it to the Pleistocene age. Moreover, Badran (1996) dated it as Late
Pliocene to Pleistocene in age, and it was later dated as Pleistocene to
Recent (Ismail et al., 2010). This formation grades into the overlying
Bilqas Formation by the increase of interbedded clays with sands, rich in
peat, with a coastal or lagoonal fauna (Ismail et al., 2010). Bilqas
Formation constitutes the top basin fill with coastal sands and deposits
from the Nile floods. This formation covers the whole Delta region.
However, it is difficult to differentiate it from the underlying Mit Ghamr
Formation (Ismail et al., 2010).This formation is composed of sand
interbedded with clay rich in molluscan fragments. The clays contain
plant remains and carbonaceous matter. It is dated as Holocene by
Badran (1996). Azzam (1994) mentioned that during the Holocene, a
marine transgression covered most of the Northern Delta area and gave
rise to a few metres of marine sediments capped by agricultural soil. Abu
El Enein (1990) ascribed this formation to the same age. Based on the
faunal association, this formation is dated as being Pleistocene to Recent
in age (Ismail et al., 2010). The Holocene rocks are represented by the
intermittent marine transgressions that give rise to a few metres of marine
sediments.
The source rocks which provide sediments to the Nile River and
Delta are characterized by markedly different geological terranes. An
average of 84% of the flow in the main Nile is derived from Ethiopia
during summer floods and 16% is introduced from the central Africa
Lake Plateau (Said, 1981; Stanley et al., 1988). The dominant influence
of the Ethiopian Plateau terrains is recorded in heavy mineral data from
Pleistocene and Holocene core sections in the promontories of the Nile
Delta (Stanley et al., 1988) and in offshore deposits on the Egyptian shelf
(Stanley et al., 1979). Furthermore, heavy mineral suites in modern
coastal sands along the delta margin are characterized by Ethiopian
components (El Fishawi and Molnar, 1985).
154 Y. H. Dawood, H. H. Abd El-Naby
Sampling and Analytical Procedures
Forty ditch cutting samples were collected from one borehole,
located at 20 Km SE of the Burullus Lake of northern Nile Delta area
(Fig. 1). Depth interval from surface ranges between 1-40 m. The color
of these sediments is variable depending on the mineralogical
composition and organic matter contents. The color ranges from light
gray, brown to black. The sample analyses were performed using
different analytical procedures available at the laboratories of Geology
Department of Ain Shams University, Faculty of Earth Sciences of King
Abdul Aziz University and the laboratories of XRAL, USA. The
collected samples were dried at 100 °C in an oven for 3 days and then
split into three parts for laboratory investigations. The investigations
include determination of organic matters, carbonates, heavy minerals,
uranium and thorium contents for the whole sample.
The first portion of the sample was weighed and then treated by
warm 0.2 N HCl in order to calculate the carbonate percentage. The
insoluble residue was wet sieved in order to separate sand size fractions
for the purpose of heavy minerals separation. After dryness, the
percentage of the sand fractions was calculated. The heavy minerals were
separated using bromoform. Microscopic investigation, Back Scattered
Electron imaging (BSE) and Energy Dispersive X-ray Spectrometry for
some separated heavy mineral grains were performed using JEOL JXA-
8200 Electron Probe Micro Analyzer. The clay deflocculation in the
separated -63µm size fraction was obtained through repeated
centrifugation. After transferring the suspended sediments to a graduated
glass cylinder and vigorously shaking, the silt and clay percentages were
determined using the pipette method.
The second portion of the sample was used to measure the
percentage of organic matter contents. A clean and desiccated crucible
was weighed before putting in a few grams of dried samples. The
combined mass was measured and the crucible was then put in a muffle
furnace at temperature of 450oC for 8 hrs. The crucible was removed and
allowed to dry in desiccator. The crucible is then re-weighed and the
organic matter content is calculated.
The third portion of each sample was crushed in a jaw crusher and
powdered to 200-mesh size by ball milling. Uranium and thorium
contents were measured by Instrumental Neutron Activation Analysis
Distribution of Uranium and Thorium Radioelements in … 155
(INAA). The irradiated samples are allowed to decay for approximately 7
days, and are counted on a high-resolution coaxial germanium detector
for up to 2000 s. All spectra are collected on a Canberra Series 90 multi-
channel analyzer. Reference materials were analyzed in each batch of
samples to monitor analytical accuracy. Precision was also determined by
analysis of sample duplicates. Both precision and accuracy were
generally within 10%.
Results
Composition of Pleistocene-Holocene Subsurface Sediments
The percentages of organic matters, carbonates, sand, silt and clay
size fractions in the borehole sediments are shown in Table 2. The
organic matter contents range between 3.28 and 15% with an average of
8.77%. The carbonate fraction is represented mainly by molluscan
fragments of different sizes. It constitutes a significant proportion of the
light minerals in the sediments with an average content of about 4.92%.
The sand size fractions of the borehole sediments constitute about
39.51%, in average. Conversely, the averages of silt and clay size
fractions are 32.2 and 14.6%, respectively (Table 2). The sand-silt-clay
ternary diagram of Krumbein and Sloss (1963) shows wide distribution
of samples in seven different fields. This plot classifies around 25% of
the samples into sand, 20% clayey silt, 18% silty sand, 15% sandy silt
and 15% sand-silt-clay (Fig. 2).
The mineralogical composition of the clay fraction in the subsurface
sediments of the Nile Delta were previously identified as
montmorillonite, chlorite, mixed-layer illite-montmorillonite, illite and
kaolinite (Fayed and Hassan, 1970) and as smectite, kaolinite and illite
(Stanley et al., 1998). Conversely, the separated clay fraction of the Nile
River streambed sediments is dominated by kaolinite, illite and
montmorillonite (Dawood, 2010).
The microscopic investigation of the heavy mineral fractions
showed the presence of the characteristic River Nile assemblage
including amphiboles, pyroxenes, biotite, muscovite, iron oxides,
tourmaline, zircon, monazite, apatite, titanite, kyanite, sillimanite,
andalusite, staurolite and garnet (Shukri, 1950). The percentage of heavy
fractions range between 0.01 and 7.52 % with an average of 2.43%
(Table 2).
156 Y. H. Dawood, H. H. Abd El-Naby
Table 2. Sedimentological data of the borehole sediments of the Nile Delta.
S. N.
Sand
Total Light
minerals %Heavy
minerals %Total
Sand% Silt % Clay %
Organic matters % Carbonates %
1 65.76 3.31 69.07 23.66 2.21 4.15 0.91 100 2 72.51 7.52 80.03 1.71 7.05 8.05 3.15 99.99 3 74.27 7.14 81.42 1.32 6.60 9.72 0.94 100 4 59.73 3.97 63.70 19.26 6.08 7.36 3.58 99.98 5 47.47 1.87 49.34 0.88 30.14 9.32 10.32 100 6 33.76 2.82 36.57 27.31 20.16 11.8 4.16 100 7 39.73 3.65 43.38 28.86 13.23 11.74 2.79 100 8 28.14 0.01 28.15 39.65 20.55 8.2 3.45 100 9 40.73 1.68 42.41 22.25 20.37 14.08 0.89 100 10 6.34 0.08 6.42 59.12 10.46 7.59 16.4 99.99 11 17.75 0.40 18.15 48.49 17.59 8.48 7.28 99.99 12 2.58 0.01 2.59 61.92 15.46 9.09 10.93 99.99 13 1.78 0.03 1.81 58.66 22.93 10.7 5.9 100 14 65.22 2.67 67.88 10.29 9.06 9.35 3.42 100 15 58.45 3.94 62.39 21.11 8.47 3.56 4.47 100 16 68.54 2.65 71.19 5.15 8.05 5.09 10.52 100 17 70.16 7.90 78.05 3.51 5.06 10.93 2.43 99.98 18 75.32 2.33 77.65 10.45 5.17 5.78 0.94 99.99 19 72.10 4.25 76.35 13.21 3.90 5.6 0.92 99.98 20 60.79 0.09 60.88 0.47 22.01 11.63 4.98 99.97 21 52.93 3.92 56.85 15.68 5.24 10.08 12.13 99.98 22 54.16 3.69 57.86 21.34 14.70 5 1.08 99.98 23 45.77 5.12 50.89 16.06 15.30 13.29 4.44 99.98 24 60.68 5.19 65.87 0.43 13.00 6.01 14.69 100 25 75.68 3.27 78.95 4.98 7.57 6.23 2.26 99.99 26 8.71 0.06 8.77 65.28 14.38 8.99 2.58 100 27 33.40 0.28 33.68 27.12 26.21 11.22 1.77 100 28 7.57 0.06 7.63 49.07 28.29 13.9 1.11 99.99 29 5.59 0.05 5.64 46.51 31.26 10.86 5.7 99.97 30 19.18 2.75 21.93 44.07 14.12 7.75 12.12 99.99 31 5.68 1.02 6.70 71.82 14.28 3.28 3.9 99.98 32 0.47 0.02 0.49 58.60 20.01 14.58 6.32 100 33 0.39 2.01 2.40 66.62 18.97 8.94 3.04 99.97 34 13.06 1.16 14.22 61.07 12.94 10.56 1.21 100 35 0.19 4.31 4.50 55.06 25.47 12.45 2.51 99.99 36 25.67 1.51 27.17 55.81 12.15 3.4 1.47 100 37 29.96 1.65 31.60 51.05 7.90 4.23 5.2 99.98 38 28.18 2.22 30.40 47.03 8.23 7.13 7.18 99.97 39 20.67 1.57 22.24 30.79 23.94 15 8.02 99.99 40 34.16 0.85 35.01 42.15 15.64 5.55 1.65 100
Ave. 37.08 2.43 39.51 32.20 14.60 8.77 4.92 99.99
Distribution of Uranium and Thorium Radioelements in … 157
Fig. 2. Triangular plot of the Nile Delta subsurface sediments (after Krumbein and Sloss,
1963) .
U-Th Contents of the of Pleistocene-Holocene Subsurface Sediments
The concentrations of uranium and thorium in the Pleistocene-
Holocene subsurface sediments are given in Table 3, The measured
values are on a dry weight basis. The uranium contents of these
sediments range between 1 and 5.4 ppm with an average of 3.7 ppm and
that of thorium is in the range of 2.8-16.1 ppm with an average of 7.83
ppm. The Th/U ratio ranges between 1.03 and 4.74 with an average value
of 2.19.
Accessory minerals hosting uranium and thorium are common in the
studied sediments and represented mainly by zircon, monazite and
apatite. The percentages of these minerals were determined by counting
about 400 grains per slide. The zircon percentages range between 1.96
and 8.67 with an average of 5.42, monazite ranges between 0.44 and 1.97
with an average of 1.12 and apatite ranges between 0.1 and 0.41 with an
average of 0.23. Back Scattered Electron Image (BSI) of separated zircon
and apatite grains from the studied sediments at 1.5 non-magnetic
158 Y. H. Dawood, H. H. Abd El-Naby
fraction is shown in Fig. 3a, while Fig. 3b shows a BSI of a fractured
monazite grain separated at 1.5 magnetic fraction.
Table 3. U and Th contents of the borehole sediments of the Nile Delta.
S. N. U (ppm) Th (ppm) Th/U S. N. U (ppm) Th (ppm) Th/U 1 4.9 13 2.65 21 4.8 7.4 1.54 2 5.4 13.3 2.46 22 3.5 8.8 2.51 3 4.3 15 3.49 23 5 15.7 3.14 4 5.2 15.2 2.92 24 3.4 16.1 4.74 5 2.5 6.1 2.44 25 2.5 6.3 2.52 6 4.2 5.3 1.26 26 3.8 3.9 1.03 7 5.2 15.2 2.92 27 4.2 4.4 1.05 8 3.2 5.4 1.69 28 4.7 5 1.06 9 3.3 13.3 4.03 29 2.1 5.6 2.67 10 2.7 3.1 1.15 30 4 5.4 1.35 11 3.7 4.5 1.22 31 1 4.3 4.30 12 2.1 6 2.86 32 4 8.4 2.10 13 3.9 5.2 1.33 33 5 6.6 1.32 14 4.2 4.7 1.12 34 5.2 7.7 1.48 15 2.9 7.6 2.62 35 4.6 9.5 2.07 16 2.3 3.5 1.52 36 2.1 3.7 1.76 17 5 12.8 2.56 37 1 3.2 3.20 18 3.5 4.6 1.31 38 4.4 12.7 2.89 19 3.4 10.4 3.06 39 5.2 7.4 1.42 20 3.8 4.1 1.08 40 1.7 2.8 1.65 Ave. 3.7 7.83 2.19
Ave.: average of 40 samples.
Fig. 3. Back Scattered Electron Images (BSI) a) separated zircon grains (dark grey) and
well rounded apatite grains (white). b) separated fractured monazite grain.
Discussion
The composition of the Pleistocene-Holocene subsurface sediments
of the northern Nile Delta is dominated by sand size fraction followed by
silt and clay sizes, respectively (Table 2 and Fig. 2). Data of the grain
Distribution of Uranium and Thorium Radioelements in … 159
size analysis of the studied sediments indicates that the grain sizes are
most likely changed over time. Fluctuation of water flow is the main
cause for such changes. For example, an increase in silt at about 26-40m
is followed by an increase in sand at about 14-25m. This shift in
composition may reflect input of finer sediments in the deeper part
during large flood period (Fig. 4).
Fig.4. Vertical distribution of particle sizes in the studied sediments.
The contents of organic matter and clay fraction in these sediments
are remarkably higher than the corresponding constituents in the Nile
River streambed sediments (Dawood, 2010). Figure 5 shows a significant
160 Y. H. Dawood, H. H. Abd El-Naby
positive correlation between organic matters and clay fractions in the
investigated sediments. On the other hand, carbonates, composed
predominantly of shell fragments of different sizes, are lower in the
subsurface sediments compared to the streambed sediments (Dawood,
2010).
Fig. 5. Bivariant plot between clay fraction and organic matter contents.
The heavy mineral varieties of these sediments reflect basically the
composition of the rocks in the drainage basin. Amphiboles, pyroxenes,
kyanite, sillimanite, andalusite and ilmenite seem to be derived from the
Ethiopian and Central African Highlands (Foucault and Stanley, 1989).
Monazite, zircon and apatite are most probably of local sources, i.e. the
Red Sea Hills and Aswan granites (Dawood and Abd El Naby, 2007).
Detrital zircon, apatite and monazite are considered as the major uranium
and thorium bearing minerals in these sediments. Uranium is associated
with zirconium and hafnium in zircon and sometimes with thorium and
cerium in monazite. In addition, uranium in the form of uranyl ion
(UO2)2+
commonly replaces Ca in the structure of apatite (Abd El Naby
and Dawood, 2008). Thorium is a main constituent in monazite, Th-rich
monazite and thorite. Thorite inclusions in monazite were reported by
Dawood and Abd El-Naby (2007) in the Mediterranean beach sediments
derived by the River Nile. Based on the microscopic investigation of
different magnetic fractions, zircon is more abundant than both monazite
and apatite (Fig. 3a, b).
Distribution of Uranium and Thorium Radioelements in … 161
While thorium is not soluble in near surface environments, dissolved
uranium is found in most natural water at very low concentration, where
the estimated worldwide average for dissolved uranium in rivers ranges
between 0.3 and 0.6 ppb (Scott, 1982). This value increases significantly
to be abnormally high in some cases due to chemical weathering of
uraniferous rocks such as in Platte River of the North American High
Plains Region where uranium content reaches up to 31.7 ppb (Snow and
Spalding, 1994). The main factors controlling uranium concentration in
river water are the prevailing Eh–pH condition (Scott, 1982) and
availability of HCO3− complex, where uranyl-carbonate plays a crucial
role in uranium migration (Langmuir, 1978; Mangini et al., 1979; and
Gorman-Lewis et al., 2008). Conversely, the uranium and thorium
contents of the Delta sediments depend, in general, on the mineralogical
forms of these two elements in the catchment area. River runoff delivers
uranium to the coastal zone and delta areas where interactions between
dissolved and particulate phases can act to remove from, or add to,
dissolved uranium in the water (e.g. Barnes and Cochran, 1993). The
average values of uranium and thorium in the subsurface sediments of the
northern Nile Delta are 3.7 and 7.83 ppm, respectively (Table 3), which
are comparable with the corresponding values in the majority of the
World Rivers. For example, the average uranium in the streambed
sediments of the River Nile is 2.06 ppm and that of thorium 6.58 ppm,
whereas uranium and thorium averages in the sediments of the rivers
draining into Gulf of Mexico are 2.48 and 9.2 ppm, respectively (Scott,
1982, Dawood, 2010).
Uranium and thorium in these sediments are most likely found
incorporated into minerals of detrital origin. In addition, uranium could
be adsorbed directly from river water onto clay minerals or organic
debris, removed from river water to sediments directly if the reducing
condition exists (Durrance, 1986). The interrelationships between
different components of the investigated sediments and both uranium and
thorium is shown in the correlation matrix (Table 4).
Thorium concentrations are strongly correlated with heavy mineral
contents (R=0.71) (Table 4, Fig. 6a). This correlation is obvious in the
vertical distribution of both variables (Fig. 7). The shaded rectangles in
Fig. 7 demonstrate the intervals of high correlation between thorium and
heavy mineral contents (2-26m and 34-40m). At the depth of 32m,
thorium shows a remarkable increase with increasing organic matter
162 Y. H. Dawood, H. H. Abd El-Naby
contents reflecting a local thorium biosorption in the studied column.
Picardo et al. (2009) observed an increase in thorium biosorption with
increasing bed depth. Conversely, uranium while being less significantly
correlated with heavy minerals content (R=0.4), it shows a higher
positive correlation with organic matter contents (R=0.55) (Table 4, Fig.
6a, b). The (8-27m) depth interval marks this positive correlation (Fig. 7).
Samples of relatively low uranium, low organic contents and high heavy
minerals (e.g. sample 30) were microscopically investigated in detail.
These samples showed predominance of heavy mineral varieties of low
uranium contents such as amphiboles, pyroxenes and garnet. Based on
grain counting process, the ratios of (Am+Grt+Px)/(Zrn+Mnz+Ap) in
these samples are high, ranging from 5.2 to 7.3. Despite that, clays are
considered as a potential sorbent of uranium and the ability of
montmorillonite to sorb uranyl ions affects the fate and transport of
uranium (Chisholm-Brause et al., 2001; and Drot et al., 2007). Clays do
not show any particular correlation with uranium or thorium in the Nile
Delta subsurface sediments indicating minor role for radioelements
adsorption by clays (Table 4).
Based on analyses of numerous rock samples, Adams and Weaver
(1958) demonstrated the usefulness of the Th/U ratios as an indicator of
relatively oxidizing or reducing conditions. Thorium is unaffected by
redox conditions and remains insoluble as Th+4
. Uranium, however,
exists as insoluble U+4
under highly reducing conditions, which leads to
Table 4. Correlation matrix between different components of the subsurface sediments
and both uranium and thorium.
lights heaviesTotal Sands
Silt Clay Organics Carbonates U Th
lights 1.00
heavies 0.67 1.00
Total Sands 1.00 0.71 1.00
Silt -0.92 -0.64 -0.92 1.00
Clay -0.61 -0.55 -0.62 0.31 1.00
Organics -0.32 -0.11 -0.31 0.03 0.60 1.00
Carbonates -0.19 -0.14 -0.19 0.03 0.05 -0.02 1.00
U 0.13 0.40 0.15 -0.21 -0.06 0.55 -0.19 1.00
Th 0.40 0.71 0.43 -0.42 -0.31 0.18 -0.13 0.55 1.00
Value more than ± 0.55 is significant
Distribution of Uranium and Thorium Radioelements in … 163
uranium enrichment in sediments, whereas it exists as soluble U+6
under
oxidizing conditions, leading to uranium loss from sediments. Thus,
Th/U ratios could be used as a proxy for redox conditions of the
depositional environment varying from 0 to 2 in anoxic environments to
7 in strongly oxidizing environments. Lower ratios would indicate
reducing environmental conditions, most commonly marine (Carvalho et
al., 2011), while higher values would be associated with uranium
mobilization through weathering and/or leaching, and would therefore
indicate an oxidizing, possibly terrestrial environment. According to the
diagnostic values suggested by Adams and Weaver (1958), the ranges of
b
Fig. 6. Bivariant plots of: a) U, Th and heavy minerals content, b) organic matters vs. uranium
content in the subsurface sediments of northern Nile Delta.
164 Y. H. Dawood, H. H. Abd El-Naby
Th/U ratio (1.03-4.74) of the subsurface sediments of northern Nile Delta
most likely reflect vertical variability based on changes in textures,
mineralogical composition and organic matter contents. A case
demonstrating exchange between fluvial, brackish and freshwater
regimes, which would be expected in delta areas.
Fig. 7. Vertical distributions of uranium (ppm), thorium (ppm), heavy minerals (%) and
organic matters (%) in the in the Pleistocene-Holocene subsurface sediments of the
Nile Delta in Egypt.
Distribution of Uranium and Thorium Radioelements in … 165
Conclusions
Particle size analyses, heavy minerals separation, microscopic
investigation, Back Scattered Electron imaging and Instrumental Neutron
Activation Analysis (INAA) were used to investigate the
sedimentological, mineralogical and uranium-thorium distribution of the
Pleistocene-Holocene subsurface sediments of northern Nile Delta. These
sediments are composed of three main formations namely; Baltim, Mit
Ghamr and Bilqas. The sand size fractions of these subsurface sediments
constitute about 39.51%, in average. Whereas, the averages of silt and
clay size fractions are 32.2 and 14.6%, respectively. About 25% of the
samples are classified into sand, 20% clayey silt, 18% silty sand, 15%
sandy silt and 15% sand-silt-clay. The organic matter contents range
between 3.28 to 15% with an average of 8.77%. The average content of
carbonates is 4.92%. The particle sizes variability of the studied
sediments indicates variation over time based on the fluctuation in water
flow. The average uranium content of these sediments is 3.7 ppm and
that of thorium is 7.83 ppm. The variation in Th/U ratios indicates
vertical inconsistency based on changes in textures, mineralogical
composition and organic matter contents of the subsurface sediments.
Correlation matrix between different components of studied sediments
showed significant positive correlations between organic matters and
clay fractions; thorium and heavy minerals contents and uranium and
organic matter contents. Geochemical behaviour of both uranium and
thorium, frequency of accessory minerals, particularly zircon, monazite
and apatite as well as sorptive uptake of uranium by organic matters are
the essential factors controlling the distributions of the two elements.
Acknowledgment
Laboratory facilities were kindly offered by the Faculty of Science
of Ain Shams University and Faculty of Earth Sciences of King
Abdulaziz University. Uranium and thorium contents were measured by
Instrumental Neutron Activation Analysis (INAA) at XRAL laboratories,
USA.
References
Abd-El Naby, H.H. and Dawood, Y.H. (2008) Natural attenuation of uranium and formation of autunite at the expense of apatite within an oxidizing environment, south Eastern Desert of Egypt. Applied Geochemistry, 23: 3741–3755.
166 Y. H. Dawood, H. H. Abd El-Naby
Abu El Enein, M.A. (1990) Contribution to the Miocene stratigraphy of the Nile Delta. Unpublished PH.D. Thesis, Geology Department, Faculty of Science, Ain Shams University, Cairo, Egypt, 186 p.
Adams, J.A.S. and Weaver, C.E. (1958) Thorium to uranium ratios as indications of sedimentary processes: example of concept of geochemical facies. American Association of
Petroleum Geologists Bulletin, 42: 387-430. Amer, Kh.M. (1974) Geological and mineralogical studies on the sedimentary succession of the
continental shelf of the Nile Delta, Ph.D. Thesis, Faculty of Sciences, Mansoura University, 124p.
Azzam, A.S. (1994) An integrated seismo-facies and seismo-tectonic Study of the Nile Delta of Egypt, utilizing common-depth seismic reflection data. PH.D. Thesis, Geology Department, Faculty of Science, Ain Shams University, Cairo, Egypt, 240 p.
Badran, A.M. (1996) The contribution of logging analysis and seismic Stratigraphy in the reservoir valuation and Lithology Determination of the north western Delta Abu Qir Offshore Egypt. Ms.C. Thesis, Geophysics Department, Faculty of Science, Ain Shams University, Cairo, Egypt, 112 p.
Barnes, C.E. and Cochran, J.K. (1993) Uranium geochemistry in estuarine sediments: controls on removal and release processes. Geochimica et Cosmochimica Acta, 57: 555– 569.
Carvalho, C., Anjos, R.M., Veiga, R., Macario K. (2001) Application of radiometric analysis in the study of provenance and transport processes of Brazilian coastal sediments. Journal
of Environmental Radioactivity, 102: 185-192. Chisholm-Brause, C.J., Berg J.M., Matzner R.A. and Morris, D.E. (2001) Uranium (VI)
Sorption Complexes on montmorillonite as a Function of Solution Chemistry, Journal of
Colloid and Interface Science, 233: 38–49. Dawood, Y.H. (2010) Factors controlling uranium and thorium isotopic composition of the
streambed sediments of the River Nile, Egypt. Journal of Earth Sciences, KAU, 21 (2):77-103.
Dawood, Y.H. and Abd-El Naby H.H. (2007) Mineral Chemistry of Monazite from the black sand deposits, northern Sinai, Egypt: a Provenance Perspective. Mineralogical Magazine, 71 (4): 441–458.
Deibis, S., Futyan, A.R.T., Ince, D.M., Morley, R.J., Seymour, W.P. and Thmpson, S. (1986) The stratigraphy framework of The Nile Delta and its implications with respect to the region’s hydrocarbon Potential. EGPC, Eighth Exploration Conference Centenary of first
oil well, Nov. 7-23, 15 p. Drot, R., Roques, J. and Simoni, E. (2007) Molecular approach of the uranyl/mineral interfacial
phenomena, Comptes Rendus Chimie, 10: 1078-1091. Durrance, E.M. (1986) Radioactivity in Geology: Principles and Applications. Ellis Horwood
Limited, Chichester, UK.: 441p. El Fishawi, N.M. and Molnár, B. (1985). Mineralogical relationships between the Nile Delta
coastal sands. Acta Mineralogica Petrographica, Szeged. 27: 89–100. El Sisi, Z.A., Sharaf, L.M., Dawood, Y.H. and Hassouba, A.B. (1996): Source of clastic supply
to Sidi Salem and Abu Madi Reservoirs of the Nile Delta: A Provenance Study. Proceedings of the EGPC 13th Exploration and Production Conference, Egypt, 1:291-296.
Fayed, L.A. and Hassan, M.I. (1970) Identification and distribution of clay minerals in some sediments of the Nile Delta, U.A.R. International Journal of Rock Mechanics and Mining
Sciences & Geomechanics Abstracts. 7, 6: 605-610. Foucault, A. and Stanley, D. J. (1989) Late Quaternary paleoclimatic oscillations in East Africa
recorded by heavy minerals in the Nile Delta, Nature, 339: 44-46. Gorman-Lewis D., Burns, P.C. and Fein J.B. (2008) Review of uranyl mineral solubility
measurements, Journal of Chemical Thermodynamics, 40: 335-352.
Distribution of Uranium and Thorium Radioelements in … 167
Ismail, A.I., Boukhary, M. and Abdel Naby, A.I. (2010) Subsurface stratigraphy and micropaleontology of the Neogene rocks, Nile Delta, Egypt, Geologia Croatica, 63(1): doi: 104154/gc.2010.01
Ismail, A.A. (1984) Quantitative well logging analysis on some subsurface Successions in the Nile Delta area. Ms.C. Thesis, Geology Department, Faculty of Science, Ain Shams University, Cairo, Egypt, 214 p.
Krumbein, W.C. and Sloss, L.L. (1963) Stratigraphy and Sedimentation: 2nd ed., W. H. Freeman
and Company, San Francisco: 660p. Langmuir, D. (1978) Uranium solution–mineral equilibria at low temperatures with applications
to sedimentary ore deposits. Geochimica et Cosmochimica Acta, 42: 547–569. Mangini, A., Sonntag, C., Bertsch, G. and Muller, E. (1979) Evidence for a higher natural
uranium content in world rivers, Nature, 278: 337-339. Picardo, M. C., Ferreira, A.C.M. and da Costa, A.C.A. (2009) Continuous thorium biosorption
– Dynamic study for critical bed depth determination in a fixed-bed reactor. Bioresource
Technology, 100: 208–210. Said, R. (1981) The geological evolution of the River Nile: New York, Springer-Verlag: 151p. Scott, M.R. (1982) The chemistry of U- and Th- series nuclides in rivers In: M. Ivanovich and R.
S.Harmon (Eds.) "Uranium series disequilibrium: Applications to environmental problems, Clarendon Press, Oxford: 181-201.
Shukri, N.M. (1950) The mineralogy of some Nile sediments, Geological Society of London
Quarterly Journal, 105: 511-534. Snow, D.D. and Spalding, R.F. (1994) Uranium isotopes in the Platte River drainage basin of the
north American High Plains Region, Applied Geochemistry, 9: 271-278. Stanley, D.J., Nir, Y. and Galilitt, E. (1998) Clay Mineral Distributions to Interpret Nile Cell Provenance and Dispersal: III. Offshore Margin between Nile Delta and Northern Israel. Journal
of Coastal Research, 14, (1): 196-217 Stanley, D.J. and Warne, D.J. (1993) Nile Delta: Recent geological evolution and human
impact. Science, 260: 628-634. Stanley, D.J., Sheng, H. and Kholief, M.M. (1979) Sand on the southern Mediterranean Ridge:
proximal basement and distal African Nile provenance. Nature, 279: 594–598. Stanley, D.J., Sheng, H. and Pan, Y. (1988) Heavy minerals and provenance of Late Quaternary
sands, Eastern Nile Delta, Journal of African Earth Science, 7: 735-741. Toussoun, O. (1922) Mémoires sur les anciennes branches du Nil Époque Ancienne. Mémoire de
l'Institut d'Egypte, 4: 212p. Wilkins, M.J., Livens, F.R., Vaughan, D.J. and Lloyd, J.R. (2006) The impact of Fe(III)-
reducing bacteria on uranium mobility. Biogeochemistry, 78: 125–150. Zaghloul, Z.M., El Shahat, A., Hegab, O. and Kora, M.A.M. (1980) Mineralogy of the
Tertiary-Quaternary subsurface sediments, West Nile Delta. Egyptian Journal of Geology, 24:177-188.
168 Y. H. Dawood, H. H. Abd El-Naby
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