Journal of Environmental Management 299 (2021) 113652

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Journal of Environmental Management

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

Effective and sustainable adsorbent materials for oil spill cleanup based on
a multistage desalination process
Ameera F. Mohammad a, b, Aya A-H.I. Mourad a, c, Emmanuel Galiwango a, Essa G. Lwisa a,
Ali H. Al-Marzouqi a, *, Muftah H. El-Naas d, **, Bart Van der Bruggen b,
Mohamed H. Al-Marzouqi a
a
Chemical and Petroleum Engineering Department, UAE University, Al Ain, United Arab Emirates
b
Chemical Engineering Department, KU Leuven, Leuven, Belgium
c
Academic Support Department, Abu Dhabi Polytechnic, Institute of Applied Technology, Abu Dhabi, United Arab Emirates
d
Gas Processing Center, College of Engineering, Qatar University, Doha, Qatar

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

Keywords: Oil spills, which are often caused by crude oil transportation accidents, contaminate coastal waters and land and
Oil spill can harm aquatic life, seabirds, humans, and the entire ecosystem. Ocean currents and wind complicate oil spill
Adsorbent material cleanup and extend the oil spill area. This study proposes a new approach to control oil spills using solids
Multistage desalination
recovered from the treatment of reject brine through a novel multistage desalination process. The aim is to
Oil recovery
Electrocoagulation treatment
produce applicable adsorbent for oil spill cleanup especially in the final cleaning stages. The multistage desa­
lination process is based on the electrochemical treatment of high-salinity reject brine and Solvay and modified
Solvay liquid effluents in a closed Plexiglas electrocoagulation cell. After the electrochemical treatment, the
collected solids were dried and ground for utilization as adsorbents in oil spill cleanup. Results were promising
for the adsorbent produced from the electrochemical treatment of the modified Solvay effluent. A maximum
adsorption capacity of 2.8 g oil/g adsorbent was achieved, with an oil recovery of 98%. In addition, the re­
generated solids after toluene extraction process were recycled and achieved an adsorption capacity of 2.1 g oil/g
adsorbent in the second oil spill clean-up cycle. The structural and chemical characteristics of the adsorbents
produced from the multistage desalination process were investigated using X-ray powder diffraction, Fourier
transform infrared spectroscopy, and scanning electron microscopy. Results support the adoption of the collected
solids as effective oil-adsorbent materials.

1. Introduction In 1994, the largest recorded oil spill of 16,000 tons occurred in the
United Arab Emirates (UAE). This oil spill resulted in a disaster to the
The release of liquid petroleum oil into marine ecosystems or eastern coast of the UAE and adversely impacted the fishing industry
freshwater environments is an important problem that causes many (Issa, 2010). Effective oil spill-control measures are therefore necessary.
environmental hazards. Recently, the world has experienced severe and Consequently, governments worldwide have imposed strict regulations
irrecoverable damage from several marine oil spill accidents. These regarding chemical spills (Carmody et al., 2008). The UAE government
accidents are particularly harmful to aquatic life (Schwacke et al., 2014; is currently implementing a codified National Oil Spill Contingency
Saadoun, 2015; Maki, 1991). Oil spills result in huge losses of heavy oil Plan, which details specific procedures for responding to an oil spill.
and substantial damage to wildlife and fishing activities (Jafarinejad, Many technologies and chemicals have been implemented for oil spill
2016; Jernelöv, 2010; Onyena and Sam, 2020). Tanker-cleaning oper­ recovery, including biological, chemical precipitates, membrane filtra­
ations discharge up to 45% of the oil spill. In contrast, ship and oil tion, physiochemical, ion exchangers, sorbents, and gelatinization
platform accidents discharge only 5% and 2% of the oil spill, respec­ methods (Hoang et al., 2018; Sueiro et al., 2011; Tamis et al., 2012).
tively (Issa, 2010). However, high spill intensity and site topography may limit oil-cleaning

* Corresponding author. P.O. Box: 15551, Al Ain, United Arab Emirates.

** Corresponding author. P.O. Box: 2713, Doha, Qatar.
E-mail addresses: [email protected] (A.H. Al-Marzouqi), [email protected] (M.H. El-Naas).

https://doi.org/10.1016/j.jenvman.2021.113652
Received 28 April 2021; Received in revised form 7 August 2021; Accepted 27 August 2021
Available online 2 September 2021
0301-4797/© 2021 Elsevier Ltd. All rights reserved.
A.F. Mohammad et al. Journal of Environmental Management 299 (2021) 113652

methods. The optimal oil-cleaning methods require improvements to developed sorbent is a better alternative to the widely used commercial
manage oil spills more economically (Hoang et al., 2018). For example, polypropylene (PP) sorbent by about 5–9 times. Wu et al. (2014)
surfactants were not effective when applied to oil dispersion. This developed an oil spill sorbent by treating polyurethane sponges with
ineffectiveness is caused by the rapid dilution of surfactants in seawater. silica sol and gasoline. High recyclability and high motor oil sorption
However, sorbents may have potential for oil spill cleanup operations capacity (∼ 103 ± 3 g/g) were reported. It was also reported that the
especially for the final cleaning stages. There are two types of sorbents, developed sorbent is a good alternative of the commercial poly­
used for either adsorption and absorption. Oil is attracted to the surface propylene sorbent which has less oil sorption capacities of 15–25 g/g.
of the sorbent in adsorption, whereas oil is internally incorporated into A literature review revealed the complex nature of oil spills. Some oil
the sorbent pores in absorption (Ifelebuegu and Johnson, 2017). The spill components bind to sorbents, while others are highly unreactive
heavy weight of some sorbents may cause them to sink and be retained (Teas et al., 2001). Most organic and inorganic approaches face signif­
at the bottom of the seawater. Moreover, some sorbent materials are icant challenges, including hydrophilicity (i.e., materials having a strong
toxic to aquatic life (Sayed and Zayed, 2006). Adsorption is a more affinity for water), high density causing sinking of the oil-rich adsorbent,
applicable, effective, and economical technique for oil spill recovery requirement of mixing with additives, increased toxicity, and low
than absorption (Abdelwahab et al., 2017). sorption capacity. Therefore, more efficient, cost-effective, and
In their work, Karakasi et al. (Karakasi and Moutsatsou, 2010) environment-friendly sorbent materials are required for oil spill
studied the oil sorption performance of high calcium fly ash (HCFA) by cleanup.
utilizing artificial ocean water. It was concluded that, the oil sorption Reject brine is a high-salinity by-product of the liquid stream pro­
capacity of HCFA recorded up to 0.7–0.9 g oil/g HCFA. In addition, the duced in large quantities in desalination plants. An equivalent amount of
hydrothermal treatment of HCFA with sodium oleate has not produced saline waste or reject brine is produced for every m3 of potable water
significant rise in oil sorption capacity, due to the insufficient increase in generated by a desalination unit (Mustafa et al., 2020). Reject brine
porosity. Magnetite nanoparticles (MNP) were evaluated by Debs et al. waste is commonly reinjected into surface water. However, this practice
(2019) for the removal of a new motor oil (NMO) and Petroleum 28◦ API has a negative impact on the environment (El-Naas, 2011). Reject brine
(P28API) from water. They have followed the ASTM F726–12 technique comprises many components in high concentration, including sodium
modified by inclusion of a lyophilization step to ensure the accuracy of (Na+), magnesium (Mg2+), calcium (Ca2+), potassium (K+ ), chloride
the outcomes. It has been observed that, the removal of 3522 ± 118 g/kg (Cl− ), and sulfate (SO2−
4 ). These components can be converted into many
(NMO) using MNP and 2157 ± 281 g/kg (P28API) employing MNP. useful products for critical industrial applications (Mustafa et al., 2020;
Lin et al. (2012) prepared a nanoporous polystyrene fibers with a Mohammad et al., 2019). The Solvay and modified Solvay processes are
high porous structures utilizing electrospinning. The developed sorbents very promising methods for treating reject brine and capturing CO2 gas
have great potential in wastewater treatment, oil accident remediation to produce water with reduced salinity, clean CO2 gas, and other useful
and environmental protection. It demonstrated a motor oil sorption solids (Mohammad et al., 2016; El-Naas et al., 2017a; El-Naas, 2018).
capacity of 113.87 g/g. Yuan et al. (Yuan and Chung, 2012) proposed a These processes employ a combined reaction, where CO2 reacts with
polyolefin polymer as an oil absorbent with aliphatic and aromatic side ammonia and brine in the Solvay process and with calcium hydroxide
chains. This polymer has the same solubility parameters as the hydro­ and brine in the modified Solvay process (El-Naas et al., 2017a). Based
carbons in crude oil. The developed polyolefin polymer is amorphous on these processes, a treatment is proposed using the electrochemical
and possesses a light cross-linked structure. The oil-absorption capacity concept for the reject brine and Solvay and modified Solvay liquid ef­
of the polyolefin polymer can reach 45 times its weight. fluents to collect more solids for use as possible adsorbents in oil spill
Sayed and Zayed used a calcium aluminum silicate sludge that was cleanup.
treated with dodecyl benzene sulphonic acid, onion, and garlic for oil The objective of this study was to produce potential adsorbents from
spill cleanup and determined that the adsorption capacity reached up to waste brine, which is available in large quantities in the UAE. These
2 g oil/g sludge, 0.455 g oil/g onion, and 0.385 g oil/g garlic (Sayed and adsorbents can be used to recover oil from different water surfaces.
Zayed, 2006). Bryk and Yakovenko investigated a clay material These types of adsorbents are eco-friendly and sustainable. The pro­
composed of a large quantity of iron oxides as the sorbent. The posed approach is based on utilizing the solids recovered from a novel
adsorption capacity of this clay material reached up to 4 g oil/g solid multistage desalination process. The target adsorbent should have a high
(Bryk and Yakovenko, 1987). Likon et al. (2013) investigated poplar oil uptake capacity along with selectivity, reusability, cost-effectiveness,
seed hair fibers as potential oil sorbents and determined that the poplar and nontoxic properties.
seed hair fibers had an absorption capacity of 182–211 g heavy motor
oil/g fiber. Raj and Joy (2015) developed a new adsorbent using coconut 2. Materials and methods
shells. This fabricated adsorbent was based on activated carbon and iron
oxide (FeO) nanoparticles. The magnetic property of this solid enhanced This study proposes a novel multistage desalination process based on
the adsorption capacity of the spilled oil from 3.01 g premium oil/g the electrochemical treatment of high-salinity reject brine and Solvay
adsorbent to 12.93 g premium oil/g adsorbent. Hoang and Pham (2018) and modified Solvay liquid effluents. These liquids were treated in a
evaluated an absorbent made from polyurethane and 25% rice straw closed Plexiglas electrocoagulation cell. The following subsections
with a 0.5-mm size. The polyurethane and rice straw absorbent showed discuss the brine and crude samples, the experimental procedure for the
an absorption capacity of 14.921 g crude oil/g absorbent. electrochemical treatment, and the oil spill cleanup process.
The artificial sorbents made of polypropylene or polyurethane are
the most commonly used commercial sorbents (Wu et al., 2014; Teas
et al., 2001). They possess good hydrophobic and oleophilic character­ 2.1. Brine samples
istics, high oil/water selectivity, low density, and abundantly available
in large-scale. But, the oil sorption capacities of these sorbents are only A brine sample with a mean salinity (based on sodium chloride
tens gram of oil per gram of sorbent. If the capacity of synthetic sorbent content) of 73,540 mg/L and a pH value of 8.36 was collected from a
could be improved, then it would be very beneficial for the oil spill multistage flash desalination unit in a local desalination plant located in
cleanup (Ceylan et al., 2009; Lim and Huang, 2007; Choi and Moreau, Abu Dhabi, UAE. The brine ion content was measured using inductively
1993). Zhu et al. (2011) fabricated a novel oil sorbent which consists of coupled plasma spectrometry (Varian 710-ES ICP optical emission
polyvinyl chloride (PVC)/polystyrene (PS) fiber by an electrospinning spectrometer). The ions with the highest concentrations in the brine
process. The results demonstrated that, the sorption capacities of the samples were sodium (Na+), magnesium (Mg2+), calcium (Ca2+), po­
PVC/PS sorbent for motor oil was 146 g/g. It was also concluded that the tassium (K+ ), chloride (Cl− ), and sulfate (SO2− 4 ). Preliminary results

2
A.F. Mohammad et al. Journal of Environmental Management 299 (2021) 113652

revealed their average concentrations with calculated error deviations stirrer trapped within a Plexiglas ring (inner diameter of 50 mm and H of
as 24,280 ± 9 ppm (Na+), 2856 ± 6 ppm (Mg2+), 1482 ± 4 ppm (Ca2+), 10 mm) and with a velocity of 2 RVS was placed in the center of the cell
905 ± 3 ppm (K+ ), 37,582 ± 6 ppm (Cl− ), and 6051 ± 5 ppm (SO2− 4 ).
to enhance the mixing inside the reactor, thus eliminating bulk circu­
The treated brine in the Solvay and modified Solvay process had 35%– lation and improving the mixing. Rectangular aluminum plates with a
40% less salinity compared with the feed brine (Mohammad et al., 2016; width of 55 mm, length of 135 mm, and thickness of 2.0 mm were used
El-Naas et al., 2017a). The treated brine is considered to be within the as electrodes in the electrocoagulation reactor. These aluminum plates
salinity range of 40,000–45,000 ppm. In the traditional Solvay process, were inserted into the top base of the inner cylinder. The space between
ammonia and CO2 react with the feed brine, and the main products are the electrodes was 50 mm. The two electrodes were connected to a
sodium bicarbonate and ammonium chloride. In the modified Solvay power supply that delivered the required current density of 5–15
process, calcium oxide and CO2 react with the feed brine and produce mA/cm2 by applying a voltage of 1–4 V. Two tubes were inserted into
sodium bicarbonate and calcium chloride (Mohammad et al., 2016; the middle of the inner cylinder cover. The first tube extended to the
El-Naas et al., 2016, 2017a, 2017b). In both processes, the liquid ef­ bottom of the reactor to provide an air jet. The second tube extended to a
fluents were electrochemically treated in a second desalination stage level over the treated mixture to vent the accumulated gases out of the
using electrocoagulation. The second desalination stage further reduces reactor. This procedure prevented liquid from leaving the reactor. The
salinity and recovers additional valuable solids. The recovered solids are reactor was filled with a total volume of 0.25 L of the treated mixture for
evaluated for oil spill cleanup and oil recovery. all the experiments. The applied current and voltage were maintained at
a fixed level for each experiment. The temperature was set to a specific
2.2. Oil samples value for each run. After each run, the treated brine samples were
collected and filtrated using a Buchner funnel filtrating kit to separate
Actual crude oil samples (three replicates) were used to evaluate the the solid coagulants. The solids were dried at 120 ◦ C for 48 h and then
oil spill cleanup potential. These samples were collected from the Bu ground using an electric grinding mill to obtain a fine powder.
Hassa field in Abu Dhabi, UAE. The crude oil samples were light grade. Electrocoagulation is an effective process for the treatment of
The average API gravity and density of the Bu Hassa light grade (BHLG) contaminated water and involves the passing of an electric current
oil samples were measured using PVT cell under ambient conditions and through the wastewater to destabilize and separate the contaminants.
recorded to be 35.7◦ ± 0.1 and 0.855 × 10− 3 gm/L ± 0.002, respectively The current is often passed through iron or aluminum electrodes and
(Lwisa and Abdulkhalek, 2021). The compositional analysis of the crude generates the following four chemical reactions for the aluminum
oil samples were carried out through Gas-Liquid Chromatography and electrode (Hakizimana et al., 2017):
the results are tabulated in Table 1 (Lwisa and Abdulkhalek, 2021). The anode dissolution, which results in aluminum ions as shown in
Reaction (1):
2.3. Experimental procedure and setup for solid adsorbent preparation Al(s) → Al+3(aq) + 3e− (1)

Electrochemical treatment was employed for the untreated feed Water electrolysis, which results in hydrogen gas and hydroxide ions
brine as a reference sample and Solvay and modified Solvay effluents as as shown in Reaction (2):
targeted solutions to be tested. The Solvay effluent contained sodium
2H2O(aq) + 2e− → H2(g) + 2OH− (2)
bicarbonate, magnesium hydroxide, and ammonium chloride (Moham­
mad et al., 2016). The modified Solvay effluent contained calcium The first step of the coagulant formation in its initial form as shown
chloride, magnesium carbonate, calcium carbonate, potassium carbon­ in Reaction (3):
ate, and sodium bicarbonate (El-Naas et al., 2017a). The novel multi­
stage desalination process was based on the integration of Al3+(aq) + OH− (aq) →Al(OH)2(s) (3)
electrocoagulation and chemical precipitation into a single simulta­ The last reaction is the complex reaction through chemical precipi­
neous process at moderate-to-high pH values. The electrocoagulation tation by combining the aluminum hydroxide with other soluble ions as
process was applied to each solution mixture (i.e., feed brine, Solvay following:
effluent, and modified Solvay effluent) for 4–6 h using aluminum elec­
trodes with a current density of 5–10 mA/cm2 and a temperature range Cations (aq) + anions (aq) + XAl(OH)3 + X(H2O) (aq) = complex. XAl(OH)3X
of 25 ◦ C–35 ◦ C. Electrons were generated at the anode with a (H2O) (4)
moderate-to-high pH level and sufficient anodic potential. At the cath­
For the electrochemical treatment for the brine and effluents of the
ode, hydrogen gas and hydroxyl ion generation improved the dissocia­
Solvay and Modified Solvay process, there is a high possibility to form
tion of the dissolved components and precipitated new solid
several components as illustrated in Reaction (4). In addition, there are
components. The closed electrocoagulation cell is illustrated in Fig. 1. It
side reactions that may occur based on the solid products which are
comprises two vertical Plexiglas cylinders with a total height of 135 mm
already present in these effluents such as magnesium hydroxide, sodium
and an inner cylinder with an internal diameter of 145 mm. The fresh
bicarbonate, ammonium chloride and potassium carbonate in the case of
brine, Solvay and modified Solvay effluents were treated separately in
the Solvay process, and sodium bicarbonate, calcium chloride, magne­
the inner cylinder. Circulating water flowed into the outer cylinder to
sium hydroxide and potassium carbonate as the case in the modified
control the reaction temperature. Thus, the outer cylinder served as a
Solvay process (Mohammad et al., 2016; El-Naas et al., 2017a). After the
jacket for the inner cylinder. The total working volume of the inner
electrocoagulation process, the recovered solid structure and composi­
cylinder was 1 L. An air jet with a flow rate of 0.1–0.3 L/min was
tion are investigated and tested for oil wettability and adsorption ca­
introduced through a tube extended to the bottom of the cell to ensure a
pacity, and utilized as a possible solid oil adsorbent material to control
uniform liquid velocity distribution between the electrodes. A magnetic

Table 1
Compositional analysis of the BHLG Oil samples (Lim and Huang, 2007).
Component H2 H2S CO2 N2 C1 C2 C3 iC4 nC4 C5 iC5 nC5 C6 C7 C8 C9 C10+

Mole% 0.0 0.0 2.59 0.12 34.16 6.72 6.36 1.54 4.05 0.01 1.99 2.66 4.78 3.82 6.11 2.58 22.51
± ± ± 0.03 ± ± ± ± ± ± ± ± ± ± ± ±
0.02 0.007 0.01 0.006 0.02 0.003 0.01 0.001 0.004 0.002 0.004 0.002 0.008 0.002

3
A.F. Mohammad et al. Journal of Environmental Management 299 (2021) 113652

Fig. 1. Schematic of the combined (electrochemical) treatment process.

oil spills. cycle and oil adsorption capacity was calculated for the recovered solid.
The second half of the recovered solid material was regenerated using
the toluene Soxhlet extraction method and the mass of solid recovered
2.4. Experimental procedure for the oil spill cleanup was calculated according to Equation (9). The regenerated recovered
solid material was also used for the second cycle of the oil spill cleanup.
Actual seawater samples from the beach in Abu Dhabi, UAE, were
used for the oil spill cleanup experiments. A common dynamic sorption Orecovery% = (Orecovered (g)/ Oad (g)) x 100% (8)
method was implemented to determine the oil adsorption capacity of the
Srecovery% = (Srecovered (g)/ Sm (g)) x 100% (9)
tested solids material (Bayat et al., 2005; Wei et al., 2003; Islam, 2007).
Approximately 1 L of seawater was added to a glass beaker for each Where, O recovery% is oil recovered percentage, O recovered is the mass of
experimental run. A crude oil sample of 0.05 L was added to the top of oil recovered in (g), S recovery% is solid recovery percentage and S recovered
the seawater, and a shaking apparatus was used to simulate the motion is the mass of solid recovered in (g).
of sea waves. The solid samples were tested separately by spreading 10 g
of each sample onto the oil spill surface. This mixture was shaken for 15 3. Results and discussion
min at 50 cycles/min. The floating oil–solid structure was then sepa­
rated from the top of the seawater using a fine polyester mesh and 3.1. Characterization of the adsorbent materials
weighed after complete drainage. The oil–solid structure was then
heated for 4 h at 120 ◦ C to evaporate the water content. The oil–solid After the electrochemical treatment, the coagulant and treated brine
structure was reweighed to calculate the percentage of the adsorbed oil. were filtrated. The recovered solid was dried and divided into three
The mass of water (Wm) and adsorbed oil (Oad) were calculated based on samples. Subsequently, the dried solid samples were individually tested
the following formulas: for solubility in seawater at room temperature. For each solubility test,
1 g of the solid sample was added to 0.05 L of seawater. This mixture was
Wm(g) = OSWm – OSDm (5)
shaken for 4 h at 25 cycles/min at room temperature. The three solid
Oad (g) = OSDm - Sm (6) samples showed a low solubility in seawater. The average solubility of
the solid samples ranged from 0.014 to 0.023 g/L of seawater. The three
Where, Wm is the water mass in (g), OSWm is the oil-solid wet solid samples showed high resistance to mixing with water and formed a
structure mass in (g), OSDm is the oil-solid dry structure mass in (g), Oad strong layer on the water surface. This layer on the water surface did not
is the adsorbed oil mass in (g), and Sm is the initial solid mass in (g). mix or settle without a vigorous mixing process.
Oil adsorption capacity OCad (g of oil/g of solid) is calculated by The densities of the solid samples measured using a Pycnometer
Equation (7): ranged from 1.962 to 2.057 g/cm3. Sieve analyses were performed on
OCad = Oad (g) / Sm (g) (7) the three solid samples. The solids collected from the treated modified
Solvay effluent showed the finest particle size of less than 74 μm with a
It is worth mentioning that the volatile content of the crude oil was mass percentage of 10.5% compared to the solids collected from the
measured at the same heating conditions (120 ◦ C and 4 h) for an oil-solid treated Solvay effluent and treated brine of mass percentage of 7.7% and
structure in a separate blank test (0.05 L of oil and 10 g of solid without 7.1%, respectively. On the other hand, maximum particles size more
seawater) and found to be around 0.046 g/g oil, which is considered to than 210 μm were found with a mass percentage of 11.8% in the solids
be low and neglected as compared to the adsorbed oil mass. Based on collected from treated brine compared to 8.1% mass percentage for the
these results an error value in the range of ±0.05 g oil/g solid material is solids collected from the treated modified Solvay effluent. Results of the
expected in oil adsorption capacity. sieve analyses are given in Table 2. The surface areas of the solid samples
A mechanical extraction process (i.e., a centrifuge system) was were measured based on the adsorption of nitrogen gas using a surface
employed to recover the oil from the adsorbent material and the per­ area analyzer (Micrometrics model Gemini 2375 porosity analyzer) at
centage of oil recovered was calculated according to Equation (8). Half 77.05 K. In the first stage, all solid samples were degassed at 150 ◦ C
of the recovered solid material was reused in a second oil adsorption under vacuum for 24 h. Then, the saturation state was realized by

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A.F. Mohammad et al. Journal of Environmental Management 299 (2021) 113652

Table 2 Table 4
Sieve analysis of the solid samples. X-ray diffraction analysis for the solids main composition produced from TB, SE,
Mass Fraction (Averaged of three samples)
and MSE.
Symbol on XRD chart Name Composition
Particle Size (μm) Solids collected Solids collected Solids collected
(Averaged of three from the treated from the treated from the treated A Kulkeite Mg8Al(AlSi7O20) (OH)10
samples) fresh brine Solvay effluent modified Solvay B Fersilicite FeSi
effluent C Ferri-Ottoliniite (Na,Li) (Mg3Fe2+++)Si8O22(OH)2
D Donbassite (Na,Li) (Mg3Fe2+++)Si8O22(OH)2
x > 210 11.8 10.3 8.1
E Killalaite (2Ca3Si2O7•(H2O)
177 < x < 210 7.5 8.6 5.4
F Sergeevite Ca2Mg11(CO3)9(HCO3)4(OH)4•6(H2O)
149 < x < 177 17.3 13.4 10.6
G Hatrurite Ca3SiO5
125 < x < 149 20.1 17.5 18.8
H Zemkorite (Na,K)2Ca(CO3)2
105 < x < 125 18.2 10.4 12.5
I Marokite (CaMn2+++O4)
88 < x < 105 7.7 13.6 16.2
74 < x < 88 10.3 18.5 17.9
X < 74 7.1 7.7 10.5
Total 100 100 100 Maximum hydrophobicity properties were observed for the solids
recovered from the treated Modified Solvay effluent and thus maximum
oil adsorption capacity is expected. Further confirmation for the low
increasing the applied pressure to fill the fine pores with liquid nitrogen. water adsorption value (~0.05 g water/g solid material) which is
In the final stage, the applied pressure was gradually reduced to evap­ related to the low contact angle analysis results.
orate the condensed gas from the analyzing system. The collected data
were used to quantify the effect of the gas adsorption and desorption 3.1.2. XRD analysis of the collected solids
models as functions of the applied pressure at a constant temperature. XRD was performed on each solid sample. The analysis was con­
The surface area was measured based on the Brunauer–Emmett–Teller ducted for a 2Ɵ range of 5◦ –80◦ for each sample. The XRD analysis re­
(BET) method, and the pore size distribution was calculated based on the sults for the solid products are shown in Fig. 3(a–c). A systematic
Barnett–Joyner–Halenda (BJH) method (XavIer and BandA, 2016). The analysis procedure that defined the d-spacing in terms of their intensity
BET surface area of the solids collected from the treated modified Solvay was used. This procedure started with the three most intense peaks for
effluent was found to be 77.128 m2/g. This is comparable to the surface each identified crystal structure (Kontoyannis and Vagenas, 2000). The
area of the fabricated magnetic activated carbon for oil spills separation electrochemical treatment for the brine and the Solvay and modified
which is reported to be 66.3 m2/g (Shokry et al., 2020). Table 3 shows Solvay effluents produced solids with several crystal structures as ex­
the surface area and pores measurements for the three tested solid pected. Table (4) and Figure (3) show the main components in these
samples. The properties of the solid samples were low solubility in solids. Previous studies indicated that the crystalline solids stricter are
seawater, low density and particle size distribution, and high surface generally supposed to adsorb material rather than absorb due to the
area and pore volume. These properties of the solid samples support minimal pathways for adsorbent to penetrate the particle bulk. This can
their applicability to oil spill cleanup (Zhao et al., 2013; Yu et al., 2015). be confirmed by the adsorbent extraction process after the adsorption,
The main composition for the collected solid samples was identified where high adsorbent recovery through mechanical extraction propose
using X-ray powder diffraction (XRD). Further, scanning electron mi­ the adsorption phenomena.
croscopy (SEM) and Fourier transform infrared (FTIR) spectroscopy
were employed to determine the surface morphology, texture, and shape 3.1.3. FTIR spectroscopy
of the produced solids. An IRTrace-100 FTIR spectrophotometer (Shimadzu, Kyoto, Japan)
was used to investigate the difference in functional groups between the
3.1.1. Contact angle analysis three solid samples. The FTIR employed a 4 cm− 1 spectral resolution and
Fig. 2(a–c) shows the droplets of freshwater, seawater and crude oil 34 scans. The spectral wavelength results ranged from 500 to 4000
on the surface of the solids recovered from the treated brine (TB), Solvay cm− 1. Fig. 4 displays the major absorption bands and the differences
effluent (SE) and modified Solvay effluent (MSE), respectively. The low among the samples. These differences were resulted from the different
contact angle of all solids in oil compared to the contact angle in treatment conditions. The solid samples showed different band absorp­
freshwater and seawater is a clear indication of the hydrophobic prop­ tion bands (Fig. 4(a–c)). For example, the solids show bands at
erties of the solids and low water wettability (Mahmoud, 2020). 3293–3410 cm− 1 resulting from the O–H bond stretching (Kontoyannis
and Vagenas, 2000; Lamadrid et al., 2014). Such bond stretching is
characteristic of Ferri-Ottoliniite and Kulkeite crystals. The solid sam­
Table 3
ples also had absorption bands between 1648 and 1765 cm− 1. These
Surface area and pores analysis of the solid samples.
absorption bands correspond to a C– – O vibration mode. The absorption
Parameter Solids from the Solids from the Solids from bands are attributed to a bicarbonate bond produced during the CO2
treated fresh brine treated Solvay the treated
capturing process for both the Solvay and modified Solvay processes,
effluent modified
Solvay such as Sergeevite crystals. The bands between 943 and 1060 cm− 1
effluent indicated C–O bond stretching. The bands indicate typical absorption of
Single-point SA 32.457 45.651 76.355 a carbonate group by the brine salts through Solvay and modified Solvay
(m2/g) processes. The presence of the C– – O and C–O bonds indicated hydro­
BET SA (m2/g) 32.337 46.782 77.128 phobic behavior by the solids. The hydrophobic behavior supports the
Langmuir SA 99.248 141.041 221.697 potential use of these solids for high oil wettability in the oil spill
(m2/g)
cleanup process (Tunnicliff and Jones, 1962). In addition, the variability
Micropore area 21.5661 27.7113 24.589
(m2/g) of the peak intensity from the FTIR analysis confirms that the recovered
External surface 30.8712 34.7626 32.875 solids from the treated MSE have more hydrophobic properties than TB
area (m2/g) and SE solids (Matějková and Šimon, 2012).
Micropore 0.0132868 0.0140506 0.019947
volume (cm3/
g) 3.1.4. SEM analysis
Pore radius (nm) 2.81961 2.80759 2.08408 The structural morphologies of the collected solids were analyzed

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A.F. Mohammad et al. Journal of Environmental Management 299 (2021) 113652

Fig. 2. Contact angle analysis of the solids collected from (a) MSE (b) SE, and (c) TB.

Fig. 3. X-ray diffraction patterns for the solids collected from (a) TB, (b) SE, and (c) MSE.

using a scanning electron microscope (JEOL Neoscope JCM-5000, show a more porous structure than the fresh brine solids and have
Tokyo, Japan). The samples were coated with gold via vacuum spat­ needle-like 2-μm crystals. Fig. 5 (c) shows a micrograph of the solids
tering while being clamped to a sample holder. The images were from the treated modified Solvay effluent. The solids from the treated
captured on a spot size of 40 using 10 kV. Fig. 5 (a) shows a micrograph modified Solvay effluent had the maximum observed pores distribution
of the solids collected from the electrochemical treatment of the fresh in the structure among the three solid samples and had a homogeneous
brine; the solids show an irregular rounded surface texture and a specific surface. Additionally, cracks and shell-like surfaces were observed in the
pore size distribution within the mineral structures. Fig. 5 (b) shows a micrographs of the three samples. The cracks/shell-like surfaces indi­
micrograph of the solids from the treated Solvay effluent; these solids cated a high-exchange exposed surface area. A study reported that low

6
A.F. Mohammad et al. Journal of Environmental Management 299 (2021) 113652

collected samples from the seawater.

The solid adsorbent produced from the treated modified Solvay
effluent achieved a maximum adsorption capacity of 2.1–2.8 g oil/g
adsorbent. The ranges of the oil adsorption capacity for the Solvay
effluent and fresh reject brine were 1.6–1.8 g oil/g adsorbent and
1.1–1.5 g oil/g adsorbent, respectively. A mechanical extraction process
was employed to recover the oil from the adsorbent materials. The
percentage of oil extracted from the treated brine and Solvay and
modified Solvay effluents were ≥74%, ≥94%, and ≥98%, respectively.
The high oil recovered percentages from the oil-solid structure based on
the mechanical extraction process propose that adsorption is the domi­
nant phenomena in extracting oil from water body. The solid masses
were completely recovered (100%) when the toluene Soxhlet extraction
method was applied to the solid samples. Moreover, after the mechan­
ical extraction, the recovered solids were reused for a second cycle of the
oil spill cleanup process. This second oil spill cleanup process, after the
mechanical extraction, achieved an oil adsorption capacity of ≥0.6 g
oil/g adsorbent ≥0.7 g oil/g adsorbent and ≥0.8 g oil/g adsorbent for
the solids collected from the treated fresh brine, Solvay and modified
Solvay effluent, respectively. On the other hand, after the toluene
extraction, the clean recovered solids were reused for oil spill cleanup
process and achieved more oil adsorption capacity compared to the
mechanical extraction (≥0.9 g oil/g adsorbent, ≥ 1.5 g oil/g adsorbent,
≥ 2.1 g oil/g adsorbent for the solids collected from the treated fresh
brine, Solvay and modified Solvay effluent, respectively).
Figs. 7 and 8 show the results of the average oil adsorption capacity
and oil recovery efficiency, respectively. In contrast, the regenerated
solids after the toluene Soxhlet extraction process showed a high oil
Fig. 4. FTIR analysis of the solids collected from (a) TB, (b) SE, and (c) recovery efficiency of ≥72%, ≥89%, and ≥91% from the solids collected
MSE solids. from the treated fresh brine, Solvay and modified Solvay effluent,
respectively. The obtained results confirmed that the treated solid from
agglomerate and cracks/shell-like surfaces indicate the hydrophobic MSE is the best in terms of surface area, pores measurements, hydro­
behavior of the collected solids (Cao et al., 2016). phobic properties and, oil adsorption efficiency compared with TB and
SE. On the other hand, the adsorption capacity and the oil recovery
percentage from the first and second cycle as presented in Figs. 7 and 8
3.2. Oil adsorption capacity and oil recovery efficiency for the adsorbent
are found to be statistically different. The results from the single factor
materials
ANOVA analysis (Table 5) depict that the source of variance is statisti­
cally different between the different cycles using the same tested solids
For the oil adsorption capacity and oil recovery evaluation, three
(MSE solids).
replicates for each solid sample (TB, SE and MES) were tested and error
The second cycle always shows a lower adsorption value and re­
deviation was calculated. After the solid samples were added to the oil
covery percentage, this should be related to the decrease in the available
surface, the oil droplets were attracted to the solid particles and formed
adsorption sites each cycle because of the damaging and blocking of the
an oil–solid floating structure on the top surface of the seawater. The
fine adsorption sites and accordingly holding some oil insides each
oil–solid structure demonstrated high resistance to a vertically applied
adsorption cycle. In addition, the loss of efficiency in the oil adsorption
force, which was used to sink the structure. Instead, the structure
from one cycle to another could be investigated in more details and
remained on the surface. A very strong (vigorous) mixing process was
minimized by further parametric study and statistical evaluation to
required to make all the solid–oil structures sink to the bottom of the
propose the optimum oil recovery process and conditions that have
glass beaker. These findings support the applicability of these solids to
maximum extraction efficiency for each cycle.
oil cleanup because the mixed structure can easily be collected from the
Based on the findings from both adsorption cycles, it can be
surface of a waterbody. Fig. 6 illustrates the oil adsorption by the

Fig. 5. SEM analysis of the solids collected from (a) TB, (b) SE, and (c) MSE solids.

7
A.F. Mohammad et al. Journal of Environmental Management 299 (2021) 113652

Fig. 6. Utilization of the collected solids in the BHLG Oil spill cleanup process.

Table 5
Results of single factor ANOVA analysis for the adsorption and recovery process
from the first and second cycles using the MSE solids.
ANOVA Single Factor

Source of Variation SS df MS F P-value

Between different adsorption cycles 0.54 1 0.54 54 0.001826

Within the same adsorption cycle 0.04 4 0.01
Total 0.58 5

Between different recovery cycles 0.735 1 0.735 73.5 0.001017

Within the same recovery cycle 0.04 4 0.01
Total 0.775 5

overall cleanup efficiency.

4. Adsorption kinetics

To evaluate the adsorption kinetics of crude oil uptake from oil/

seawater system onto solids collected from TB, SE, and MSE for 0.05 L
oil/L seawater at 25 ◦ C (42.75 g oil/L seawater), pseudo-first order and
Fig. 7. BHLG Oil adsorption capacity of the collected solid samples from the pseudo-second order kinetic models were investigated using a non-
first and second adsorption cycles which were regenerated by the toluene linear procedure which is the most common method to define the
Soxhlet extraction process in three replicates. adsorption kinetic parameters (Mahmoud, 2020). Each solid sample (TB,
SE, MSE) with a same adsorption time was measured three times inde­
pendently, and the average adsorption capacity and standard deviation
were calculated. The agreement of experimental results with the
adsorption models, as shown in Figure (9), was evaluated by the cor­
relation coefficient R2. The expressions of kinetic models are presented
in the following equations: Pseudo-first-order model (Tayeb et al.,
2020).

OCad = OCe (1 − e− K1 t
) (10)
Pseudo-second-order model (Piperopoulos et al., 2019):
/
OCad = K2 OCe2 t (1 + K2 OCe t) (11)

where OCe is the oil adsorption capacity (g oil/g solid) at equilibrium, K1

(L/min) and K2 (g solid/g oil. min) are the constants of pseudo-first
order and pseudo-second order kinetic models, respectively.
Table (6) listed the parameters of adsorption kinetic models, which
displays that the modeled adsorption capacity of both the pseudo-first
and second-order kinetic model are in very good agreement (R2 >
0.99) with experimental oil capacity which suggested that the process of
oil adsorption is physical as well as chemical adsorption in nature
(Mantripragada et al., 2020).
Fig. 8. BHLG Oil recovery efficiency of the oil–solid mixture from the first
adsorption cycle and the second adsorption cycle after the toluene Soxhlet 5. Adsorption isotherm
extraction process in three replicates.
Initial oil concentration (Ci) quantity from 0 to 50 g/L seawater was
concluded that these adsorbents are very promising materials for use in used to study the effect of initial oil concentration on the oil adsorption
oil spill cleanup. Furthermore, the recovered solid after each regenera­ capacity using 1.0 g of the solids collected from the treated modified
tion process was found to be approximately 98%–100%, which indicates Solvay effluent (MSE) at temperature of 25 ◦ C and for 24 h of fixed
the sustainability of the proposed materials. However, a methodology mixing conditions. The equilibrium oil concentration (Ce), which is the
for further optimizing the collected solids is required to improve the difference between the initial oil concentration (Ci) and the final oil
concentration (Cf) was calculated and plotted with oil uptake value as

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A.F. Mohammad et al. Journal of Environmental Management 299 (2021) 113652

Table 6
Results of oil adsorption kinetic models of oil on solids collected from TB, SE and MSE for 0.05 L oil/1 L seawater at 25 ◦ C.
Adsorption kinetic models Fitting constants TB 95% confidence deviation SE 95% confidence deviation MSE 95% confidence deviation

Pseudo-first-order model OCe 1.418381 0.0065792 1.74 0.0033738 2.723668 0.0061215

K1 2.213887 0.095385 3.45 0.0882937 2.374375 0.0519596
R2 0.987985 – 0.9918 – 0.996724 –

Pseudo-second-order model OCe 1.419163 0.0032786 1.74 0.0018025 2.721911 9.56x10− 07

K2 2.21004 0.0640328 3.44 0.0629231 2.379142 1.10x10− 05

R2 0.998748 – 0.9997 – 0.999686 –

illustrated in Table (7) to define the equilibrium oil uptake value on the
MSE sample by nonlinear models (Zhu et al., 2009; Soliman et al., 2013).
QL KL Ce
OCad = (12)
1 + KL Ce

where QL (g oil/g solid) and KL (L/g solid) are Langmuir constants,

respectively.
1
OCad = KF Cen (13)

where KF (g oil/g solid) is constant and n is the intensity of oil adsorption

for Freundlich model.
KRP Ce
OCad = (14)
1 + ACeB

where KRP (L/g soil) and A (L/g solid) are constants, and B is the
exponent of adsorption energy for the Redlich-Peterson model.
The isotherm evaluation can provide a useful information on the
adsorption mechanism. The fitted constants for each model indicate that
Fig. 9. Adsorption kinetics of BHLG Oil onto collected solids from treated brine the Redlich-Peterson model isotherm reaches the best fitting model for
(TB), Solvay effluent (SE) and modified Solvay effluents (MSE) for 0.05 L oil/1 L oil adsorption onto MSE with highest correlation coefficient R2 of
seawater at 25 ◦ C in three replicates.
0.9107 compared to other isotherms models. This three-parameter
empirical adsorption model is integrating elements from both the
shown in Figure (10). The experimental procedures for the same equi­ Langmuir and Freundlich isotherms and does not follow ideal monolayer
librium oil concentration were repeated three times and the average adsorption characteristics and hence a multilayer oil adsorption is
adsorption capacity and standard deviation were calculated. It was clear dominant (Wu et al., 2010). In addition, Redlich-Peterson isotherm
that the oil removal is remarkably increased with increasing the equi­ model has a linear dependence on adsorbate concentration in the
librium oil concentration, where the oil adsorption capacity increased numerator and an exponential function in the denominator, which
from 0.41 to 2.72 g oil/g solid for changing the equilibrium oil con­ represent the adsorption equilibrium over a wide range of adsorbate
centration from 0.09 to 1.28 g oil/1 L seawater. Based on these exper­ concentration. Hence, it can be applied in the homogenous and het­
imental results, isotherm models of Langmuir, Freundlich and Redlich- erogeneous systems. As noted from the data listed in Table 7, the value
Peterson (R–P), Equations (12)–(14), respectively, were assessed as of B is not equal to one, which indicates deviation from Langmuir
isotherm. In addition, the value of KRP/A indicates the theoretical
adsorption capacity that is evaluated based on the listed data and found
to be 3.0831 g oil/g solid, which can be considered very close to the
experimental value (2.8 g oil/g solid). The deviation error for the listed
constants for the R–P isotherm model was in the range of
0.00621–0.13808, compared to Langmuir model which has a very close

Table 7
Results of oil adsorption isotherm models of oil on solids collected from MSE
equilibrium concentration from 0.09 to 37.28 g oil/L seawater at 25 ◦ C.
Adsorption isotherm Fitting 95% confidence MSE
models constants deviation

Langmuir model QL 0.1749374 2.81

KL 0.1597285 4.56
R2 – 0.9065

Freundlich model KF 6.43x10− 05 1.86

N 0.0003485 6.92
R2 – 0.7781

Redlich-Peterson model KRP 0.1380876 11.13

Fig. 10. Adsorption isotherm of BHLG Oil onto collected solids from MSE at A 0.0157916 3.61
B 0.00621396 1.04
equilibrium concentration from 0.09 to 37.28 g oil/1 L seawater at 25 ◦ C in
R2 – 0.9107
three replicates.

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A.F. Mohammad et al. Journal of Environmental Management 299 (2021) 113652

Table 8
Examples of various oil spill adsorbent/absorbent materials with their properties.
Reference Sorbent Material Adsorbed Substance Adsorption BET surface Density (g/ Advantages
capacity (g/g area (m2/g) cm3)
sorbent)

Sidik et al. ( Lauric acid treated oil palm leaves Crude oil adsorption 1.2 ± 0.12 – – - Waste material extracted
Sidik et al., from oil-palm leaves
2012) - Economic
Radetić et al. ( Recycled wool-based nonwoven Crude oil adsorption 11.50 – – - Waste material
Radetić et al., material - High biodegradability
2003)
Vlaev et al. ( Black rice husk ash Crude oil adsorption 6.22 228 1.8 - Good adsorption capacity
Vlaev et al., - Low cost
2011)
Wang et al. ( Hydrophobic aerogel Oil adsorption 2.80 660–671 – - High porosity
Wang et al., - high hydrophobicity
2010)
Banerjee et al. ( Oleic acid-grafted sawdust Crude oil adsorption 6.00 3.0 – - Waste material from timber
Banerjee industry
et al., 2006) - Biodegradable material
Hao et al. (Hao Super-hydrophobic rock wool Absorption of high-viscosity 6–13 – 0.1 - Industries produce large
et al., 2019) modified by PDMS/SiO2 oils (e.g. diesel oil, engine oil) quantities from waste rock
wool
- Low cost
- Environmentally friendly
- Degradable naturally
Liu et al. (Liu microcrystalline cellulose and Absorption of different type of 3–14 – – - Biodegradable and
et al., 2017) methyl cellulose Silica sponge oils and organics (e.g. toluene, Biocompatible polymer
diesel oil, gasoline) - Good elasticity and
mechanical properties
Wang et al. ( Ultrathin Al2O3/silane polyurethane Absorption of silicon oil/ 80–150 – – - Outstanding water-
Wang et al., foam engine oil/cyclohexane/ repelling ability and oil-
2014) chloroform affinity
- excellent recyclability
- quit low
Choi et al. (Choi sugar-templated Absorption of silicon oil/ 5.0–11 – 0.18 to 0.75 - Elastically deformed into
et al., 2011) polydimethylsiloxane sponge engine oil/toluene/ any shape
chloroform - compressed repeatedly in
air or liquids without
collapsing
- low cost
Wang et al. ( polycarbonate porous monoliths Adsorption of CH3OH/ 4.96–9.23 146.8 – - Z8/PC is highly selective
Wang et al., modified with metal organic Cyclohexane/Kerosene/CCl4/ - renewable.
2020) framework (Z8/PC) diesel oil/Cetane - fast kinetics
Current Study Solids collected from treated Crude oil adsorption 2.80 33–77 1.962–2.057 - Regenerated adsorbent
modified Solvay effluent (MSE)’ - Waste material
- Average to high surface
area
- Fast Kinetics
- Low density and solubility
in water

R2 value of 0.9065 and constant deviation errors in the range of areas, and main advantages for some adapted oil spill adsorbent
0.15972–0.174937. The R–P isotherm model was selected as the best-fit materials.
model with maximum R2 value and minimum constant deviation error
values. However, the R–P model is a three-parameter model, and it is 7. Conclusions
expected to give better fit than the other two-parameter models.
This study proposes new oil-adsorbent solids that can be produced
6. Limitations of the proposed adsorption material from treated reject brine. These adsorbents have low solubility and
hence low negative impact on environmental systems. The low density
Current oil spill adsorption methods that use similar materials face of these solid materials decreases the operational cost of spreading fresh
the challenge of discharge to the site owing to their low density, since sorbent over the oil spill areas. Additionally, the oil–solid structure re­
the low density of these materials can be aggravated by bad weather on mains light with less density than seawater. Thus, a collection of oil­
water bodies with an oil spill. The adsorbents collected from the treated –solid structures can be employed for oil spill cleanup with reduced
brine and Solvay/modified Solvay effluents are no exceptions to this operational costs. Mechanical extraction and toluene Soxhlet extraction
reality. Furthermore, a wide range of crude oil/petroleum product were used to recover and regenerate the solids for a second oil spill
compositions, leakage quantities, sensitivity of the location, and toxicity cleanup process. A maximum adsorption capacity of 2.8 g oil/g adsor­
of the chemicals exists. Developing an adsorbent that successfully bent material was achieved using the solids collected from the electro­
overcomes these obstacles remains a challenging task. The proposed chemical treatment of the modified Solvay effluent. Finally, a high oil
adsorbent solids were tested in a simulated crude oil spill environment. recovery of up to 98% was obtained using the proposed solid materials
The results of this experiment indicate promising adsorption and oil during the first cleanup process cycle. Further investigations in terms of
recovery efficiency, which warrants further investigation and optimi­ the parametric analysis are required to optimize the process parameters
zation. Table (8) the demonstrates oil adsorption capacities, BET surface for the purpose of improving and maximizing the overall cleanup

10
A.F. Mohammad et al. Journal of Environmental Management 299 (2021) 113652

efficiency using the collected solids from the treated modified Solvay Ifelebuegu, A.O., Johnson, A., 2017. Nonconventional low-cost cellulose-and keratin-
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Islam, S., 2007. Investigation of Oil Adsorption Capacity of Granular Organoclay Media
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draft preparation. Aya A-H. I. Mourad: Methodology, investigation, Heinemann.
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writing- original draft preparation. Emmanuel Galiwango: Visualiza­ 353–366.
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Al-Marzouqi: Conceptualization, reviewing and editing. Muftah H. El- application in oil spill clean up. Fuel 89, 3966–3970.
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Conceptualization, reviewing and editing. Mohamed H. Al-Marzouqi: Lamadrid, H.M., Lamb, W.M., Santosh, M., Bodnar, R.J., 2014. Raman spectroscopic
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Declaration of competing interest
Lim, T.-T., Huang, X., 2007. Evaluation of kapok (Ceiba pentandra (L.) Gaertn.) as a
natural hollow hydrophobic–oleophilic fibrous sorbent for oil spill cleanup.
The authors declare that they have no known competing financial Chemosphere 66, 955–963.
interests or personal relationships that could have appeared to influence Lin, J., Shang, Y., Ding, B., Yang, J., Yu, J., Al-Deyab, S.S., 2012. Nanoporous polystyrene
fibers for oil spill cleanup. Mar. Pollut. Bull. 64, 347–352.
the work reported in this paper. Liu, B., Zhang, L., Wang, H., Bian, Z., 2017. Preparation of MCC/MC silica sponge and its
oil/water separation apparatus application. Ind. Eng. Chem. Res. 56, 5795–5801.
Lwisa, E.G., Abdulkhalek, A.R., 2021. An experimental approach to enhanced oil
Acknowledgments
recovery by nitrogen and carbon dioxide injection followed by low salinity water
flooding for tight carbonate reservoir. Advanced Aspects of Engineering Research 2,
The authors wish to thank Dr. Hussain Awad from the Chemical and 143–151.
Mahmoud, M.A., 2020. Oil spill cleanup by raw flax fiber: modification effect, sorption
Petroleum Engineering Department at UAE University for his help.
isotherm, kinetics and thermodynamics. Arabian Journal of Chemistry 13,
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