553

Decontamination of water polluted with oil

through the use of tanned solid wastes
Amal Gammoun, Soufiane Tahiri, Abderrahman Albizane, Mohammed Azzi, and
Miguel de la Guardia

Abstract: Sorption by natural organic substrates, inorganic materials or synthetic fibers is one of the most popular meth-
ods used for the separation of oily wastes from contaminated water. In this work, the ability of chrome shavings (CS) and
of buffing dusts of crust leather (BDCL) to remove motor oils and oily wastes from demineralised water and natural sea-
water has been studied. Tannery solid wastes are formed mainly by proteins and have a highly organized structure in the
form of fibers (F: 100 nm). These wastes have a high oil sorption capacity. Tanned solid wastes are capable of absorbing
many times their weight in oil (6.5–7.6 and 12.8–14.5 g/g dry substrate, respectively, for ground CS and BDCL). The
sorption capacity depends strongly of sorbent nature. The removal of oils from the water surface is a quasi-instantaneous
process. After use, the saturated waste floats and can be removed in an efficient and easy manner. The results look fairly
promising as to possibilities of using tanned wastes to remove oils from industrial effluents and from contaminated coastal
areas.
Key words: tannery, solid wastes, chrome shavings, buffing dusts, oils, sorption.
Résumé : L’absorption par des substrats organiques naturels, des matériaux inorganiques ou des fibres synthétiques est
l’une des méthodes les plus employées pour la séparation des déchets huileux de l’eau contaminée. Dans ce travail, la ca-
pacité des dérayures de cuir chromé et des poussières de ponçage du cuir en stain, issues de la tannerie, à enlever des huiles
pour moteurs et des déchets huileux de l’eau déminéralisée et de l’eau de mer naturelle a été étudiée. Les déchets solides
de tannerie sont constitués essentiellement de protéines et ils ont une structure fibreuse très organisée (K : 100 nm). Ces
déchets ont une grande capacité d’absorption des huiles. Les déchets solides de peau tannée peuvent absorber plusieurs
fois leur poids en huile (6,5 – 7,6 et 12,8 – 14,5 g/g de substrat sec respectivement pour les dérayures broyées de
cuir chromé et les poussières de ponçage). La capacité d’absorption dépend fortement de la nature de l’absorbant.
L’élimination des huiles de la surface de l’eau est un processus quasi-instantané. Après utilisation, les déchets saturés
flottent et peuvent être facilement collectés. Les résultats permettront d’envisager la possibilité d’employer les déchets
de peau tannée pour enlever les huiles des effluents industriels et des zones côtières contaminées.
Mots-clés : tannerie, déchets solides, dérayures de cuir chromé, poussières de ponçage, huiles, absorption.
[Traduit par la Rédaction]

Introduction
Used or spent oils are toxic for the microflora used in the
biological degradation of organic substances contained in ef-
fluents. This can be explained by the formation of a layer on
the water surface limiting energy, heat, moisture, and oxy-
gen exchange between the water reservoir and the atmos-
phere (Lee et al. 1999; Pushkarev et al. 1983; Haussard et
al. 2001). Consequently, the efficiency of microorganisms
for the degradation of organic matter in wastewater treat-
ment will be decreased. The spilled oil also contributes to
an undesirable taste and odor to drinking water and causes
severe environmental damage. Contaminated water cannot
be used for municipal water supply, for industry, nor for ir-
rigation (Blumer 1969). Contamination of coastal areas due
to oil spills is a tragic event. Under favorable conditions, oil
may continue to spread over the water surface and form a
thin layer. As a result, marine life is seriously threatened,
beaches are polluted and tourism and the fishing industry
gravely suffer the effects.
Sorption by natural organic substrates (wood, cotton fi-
bers, bark, wool, milkweed, etc.) or inorganic materials (ac-
tivated carbon, charcoal, exfoliated graphite, flyash, etc.) or
synthetic fibers (acetylated cellulose, polypropylene, poly-
ethylene terephtalate, polyhexamethylene adipamide, etc.) is

Received 23 November 2005. Revision accepted 5 January 2007. Published on the NRC Research Press Web site at jees.nrc.ca on
30 August 2007.
A. Gammoun and M. Azzi. Faculté des Sciences, Université Hassan II– Aı̈n Chock, Casablanca, Maroc.
S. Tahiri.1 Faculté des Sciences El Jadida, Département de Chimie, Université Chouaib Doukkali, B.P.20, El Jadida, Maroc.
A. Albizane. Faculté des Sciences et Techniques, Université Hassan II, Mohammedia, Maroc.
M. de laGuardia. Departamento de Quimica Analitica, Edificio de Investigacion, Universidad de Valencia, Spain.
Written discussion of this article is welcomed and will be received by the Editor until 31 January 2008.
1Corresponding author (e-mail: t_soufiane@yahoo.fr).

J. Environ. Eng. Sci. 6: 553–559 (2007) doi:10.1139/S07-006 # 2007 NRC Canada

554 J. Environ. Eng. Sci. Vol. 6, 2007

Fig. 1. Molecular structure of wet blue and chrome shavings.

Table 1. Characteristics of tanned wastes. Materials and methods

Characteristics Chrome shavings Buffing dusts Sorbents
Average moisture (%) 22.33 13.23 Tanned wastes products assayed in the present study were
Ash (%)a 12.92 12.17 collected from a Moroccan tannery located in Mohammedia.
Chromium oxide Cr2O3 (%)a 4.40 4.85
Fat (%)a 2.50 7.77 Chrome shavings
Dermal substance (%)a 78.64 78.00 The small pieces of leather shaved off when the thickness
pH of soluble matters b 3.56 4.25 of wet blues is rendered uniform by a bladed cylinder. The
Bulk density (g
cm–3) 0.10 0.05 wet blue is the wet chrome tanned leather, without dressing.
Specific surface area (m2/g) 1.12 12.11 The molecular structure of wet blue and chrome shavings is
a
presented in Fig. 1.
Based on dry weight.
b
5 g of waste was stirred in 100 mL of distilled water. Buffing dusts
In our case, these wastes were generated after treating the
one of the most popular methods used for the separation of surface of crust leather (without dyes) by abrasion. The crust
oily wastes from contaminated water (Fanta et al. 1986; leather is, in general, the leather having undergone dressing
Schrader 1991; Choi and Cloud 1992; Choi et al. 1993; An- operations (wet or mechanical) but not yet finished. Wet
thony 1994; Lee et al. 1999; Mackay and Gschwend 2000; leather dressing includes neutralization, retanning and fat
Toyoda and Inagaki 2000; Haussard et al. 2001). The sorp- liquoring. These operations are carried out after tanning to
tion capacity of different materials employed is the amount give certain properties to the leather.
of oil retained by 1g of dry substrate. According to Gregg
and Sing (1967) the sorption capacity in a vast range of sol- Tested oils
ids depends on the surface area and pores. Tanned solid Three oils are used for the experiments to study their
wastes generated by the leather industry are very porous sorption on wastes. The samples used are: diesel motor oil,
and are a good candidate for sorption material. premium motor oil, and used motor oil (oily wastes or oil
The production of chromium-containing solid wastes from from draining). Oil samples have relatively similar densities:
the tanning process has been recognized as a problem for 0.885, 0.881, and 0.894, respectively. The viscosity at 20 8C
many years. Tanned solid wastes have been disposed of in is 0.337, 0.294, and 0.281 Pa
s, respectively.
landfills. Increased local restrictions on land disposal, recent
increases in the costs of land disposal and decreases in the Tanned wastes characteristics
number of disposal sites have combined to spur research Bulk density and specific surface area of chrome shavings
into alternative treatments for this material. Many scientific and buffing dusts were determined. The tested wastes were
groups have oriented their research to find a process to re- analysed for: ash, chromium oxide, fat, dermal substance,
cycle and reuse these tanned wastes (Tahiri et al. 2001a, and pH of soluble matter. The physicochemical characteris-
2001b, 2003, 2004; Cabeza et al. 1998; Taylor et al. 1998; tics of wastes were analysed using standard methods (Dutel
Brown et al. 1996; ANRED and CTC 1982). 1984).
Our research has been designed to aid the leather industry Microscopic observations of the structure and morphology
in the development of alternatives to disposal for solid tan- of the aforementioned products wastes were made using a
nery waste. The aim of this work is to study the possibility Scanning Electron Microscope (HITACHI S-4500).
of using tanned solid wastes as a sorbent in an oil spill
cleanup. Two wastes were tested as sorbents: chrome shav- Determination of the sorption capacity of tanned solid
ings and buffing dusts of crust leather, being employed syn- wastes
thetic oil–water mixtures to evaluate the efficiency of the Raw and dry tanned wastes were used for sorption of oils
tanned solids assayed. in a pure form. To obtain dry substrate, solid wastes were
# 2007 NRC Canada
Gammoun et al. 555

Fig. 2. Scanning electron micrograph of wastes. (a) chrome shavings (b) buffing dusts.

Table 2. Oils sorption capacities of tanned wastes for pure oils.

Oil/waste (g/g)
Oil type Waste type Raw waste Dry waste
Diesel motor oil Ground chrome shavings 5.74 7.00
Chrome shavings 4.06 3.73
Buffing dusts of crust leather 13.00 14.43
Premium motor oil Ground chrome shavings 6.48 6.54
Chrome shavings 2.60 3.81
Buffing dusts of crust leather 12.91 14.55
Used oil Ground chrome shavings 5.28 7.60
Chrome shavings 3.43 3.82
Buffing dusts of crust leather 12.08 12.80

dried at 100 8C for 4 h. In the case of chrome shavings, raw
material and fibers with 2–5 mm of length were used. It is
difficult to define a constant granulometry for raw chrome
shavings because these wastes have no regular fiber size. In
a 100 mL beaker, 80 mL of oil was placed and 1 g of sorb-
ent was immersed in the bath for 4 h. Material was then re-
covered and left to drip for 1 h and the amount of oil sorbed
was determined by subtracting the initial sorbent weight
from the total weight of the wetted sorbent. Tanned wastes
sorption capacity (SC, weight of pollutant picked by one
gram of sorbent) was thus quantified. All of the sorption ex-
periments were carried out at room temperature (20 ± 2 8C).
to 3 g. Tests were carried out, respectively, without and
with stirring. In the case of stirring, the beakers were placed
on a shaker, and then shaken for 10 min at 60 r/min.
At the end of the experiments, the solid–liquid phases
were separated and the sorbent was left to drip for 1 h. The
amount of residual oil in water and that retained by the
tanned wastes were determined. Residual oil in water was
extracted with petroleum ether. The solvent extractor was
evaporated and the residual oil was weighed. The amount
of oil sorbed on wastes was calculated by subtracting the
amount of residual oil in water from the initial mass of oil
added to beakers containing water.

Sorption study in a water bath

This study will examine the feasibility of using tanned
solid wastes for sorption of oils in polluted water. Deminer-
alised water and natural seawater were used. For each oil
and waste, a mass of oil (5.5 g of commercial oils and
7.5 g of oily wastes) was added to a 1000 mL beaker con-
taining 500 mL of water. To this mixture, sorbent material
was added. The effect of the sorbent mass on oil removal
efficiency was studied using different mass ranging from 1
Results and discussion
Physicochemical characters of wastes
The chrome shavings and buffing dusts, used as raw mate-
rials in this study, were analysed for pH, ash, fat, proteins and
chromium oxide and the results are presented in Table 1. As
can be seen, the analysis indicates that these wastes have an
important percentage of proteins (78.64%–78.00%). The
amount of chromium oxide is about 4.40%–4.85%. The

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556 J. Environ. Eng. Sci. Vol. 6, 2007

Table 3. Oils sorption of solid wastes in demineralised water baths containing various amounts of oil.

Oil Waste Oil in waste Water in waste

Waste type Oil type (g) (g) (%) (g/g)
Chrome shavings Diesel motor oil 5.55a 1.00 96.58 0.15
5.54b 1.07 99.53 0.18
5.59 2.01 100 1.29
5.50 2.05 100 1.24
5.57 3.03 100 1.95
5.59 3.08 100 2.09
Premium motor oil 5.58 1.02 98.62 0.54
5.63 1.08 98.49 0.34
5.54 2.06 100 1.33
5.51 2.08 100 1.48
5.58 3.10 100 2.98
5.51 3.09 100 3.14
Used oil 7.54 1.01 99.12 0.02
7.54 1.02 92.08 0.02
7.54 2.06 100 1.11
7.56 2.07 100 1.59
7.58 3.04 100 1.67
7.58 3.04 100 1.91
Buffing dusts of crust leather Diesel motor oil 15.16 1.03 98.54 0.04
15.13 1.04 99.94 0.08
15.43 2.01 100 1.01
15.21 2.04 100 1.34
15.14 3.02 100 0.87
15.00 3.08 100 0.95
Premium motor oil 15.34 1.04 98.65 0.13
15.01 1.01 99.35 0.08
15.17 2.06 100 0.56
15.03 2.04 100 0.17
15.33 3.05 100 1.19
15.02 3.02 100 1.64
Used oil 16.07 1.10 99.20 0.06
16.09 1.06 95.67 0.04
16.02 2.02 100 0.51
16.09 2.03 100 0.56
16.18 3.02 100 0.84
16.05 3.02 100 0.98
a
Without stirring.
b
With stirring 60 r/min.

buffing dusts have a significantly higher amount of fat
(7.77%) than chrome shavings (1.57%); this can be ex-
plained by the use of greases in the fat-liquoring process.
The bulk density of chrome shavings and buffing dust are
0.1 and 0.05 g
cm–3, respectively. This low density indi-
cates that these wastes occupy a large volume as compared
to other solid wastes. This causes problems in the handling
of high amounts of tanned wastes generated in the leather
industry. The specific surface area of chrome shavings and
of buffing dusts is 1.12 and 12.11 m2/g, respectively.
Scanning electron micrographs of chrome shavings and
buffing dusts
The scanning electron microscopic method is a good tech-
nique for showing structure and morphology of solids. The
resulting micrographs (Fig. 2) reveal that the studied wastes
have a highly organized structure in the form of fibers (F =
100 nm). The fibers seem to be more separated in the case
of buffing dusts. The chrome shavings fibers are more paral-
lel and very tight to each other.
Determination of oil sorption capacity
The tests were conducted on oils in their pure form. Ta-
ble 2 groups the sorption capacity (SC) of ground chrome
shavings (GCS), raw chrome shavings (RCS) and buffing
dusts of crust leather (BDCL). The sorption capacity was
calculated for raw and dry wastes. The SC of these wastes
is very strong: about 6.5–7.6, 3.7–3.8, and 12.8–14.5 g/g
dry substrate, respectively, for GCS, RCS, and BDCL. As
can be seen, sorption capacity depends strongly of the nature
of sorbent. The results indicate that the investigated oil sam-
ples showed relatively similar sorption trends since they
have relatively similar densities and similar viscosities. For
example, in the case of dry ground chrome shavings the
sorption capacity is about 7.00, 6.54, and 7.60 g/g for diesel
motor oil, premium motor oil, and used motor oil, respec-
# 2007 NRC Canada
Gammoun et al. 557

Table 4. Oils sorption of solid wastes in natural seawater baths containing various amounts of oil.

Oil Waste Oil in waste Water in waste

Waste type Oil type (g) (g) (%) (g/g)
Chrome shavings Diesel motor oil 5.58a 1.00 96.05 0.13
5.52b 1.09 98.63 1.02
5.50 2.01 100 1.98
5.51 2.03 100 1.99
5.50 3.05 100 2.55
5.66 3.03 100 1.94
Premium motor oil 5.58 1.02 96.90 0.26
5.51 1.09 98.46 1.52
5.54 2.07 100 1.17
5.54 2.13 100 1.98
5.51 3.06 100 1.99
5.51 3.04 100 2.06
Used oil 7.64 1.04 88.64 0.09
7.57 1.02 83.10 0.96
7.53 2.03 100 0.97
7.57 2.07 100 1.41
7.57 3.04 100 1.24
7.51 3.05 100 1.98
Buffing dusts of crust leather Diesel motor oil 15.26 1.06 98.50 0.16
15.07 1.08 99.30 2.53
15.15 2.05 100 0.88
15.07 2.02 100 0.98
15.13 3.05 100 0.82
15.00 3.07 100 1.43
Premium motor oil 15.24 1.08 99.14 0.15
15.08 1.06 98.96 0.17
15.07 2.03 100 0.82
15.21 2.02 100 1.35
15.10 3.05 100 0.88
15.02 3.03 100 2.03
Used oil 16.24 1.01 98.13 0.06
16.35 1.06 99.78 1.76
16.01 2.00 100 0.93
16.10 2.08 100 0.90
16.10 3.01 100 0.61
16.04 3.09 100 1.48
a
Without stirring.
b
With stirring 60 r/min.

tively. Moisture content relatively decreased the waste’s
ability to absorb oils. Buffing dust showed better sorption
properties than chrome shavings for all investigated oils.
This is due to the morphology of wastes: the fibers seem to
be more separated in the case of BDCL and consequently
allow the penetration of a greater amount of oils into the
sorbent. On the other hand, the density of BDCL
(0.05 g
cm–3) is lower than that of chrome shavings
(0.1 g
cm–3). BDCL occupy a large volume as compared to
chrome shavings and consequently a large amount of oils
could be sorbed by dusts of tanned hides.
For chrome shavings, reduction in fibre size contributed
to the change in sorption capacity. When the wastes are
ground up (2–5 mm) the retention capacity increases.
Sorption study in a water bath
Tables 3 and 4 show the variation of removal efficiency
(RE) value of the tanned solid assayed in water using 1, 2,
and 3 g of sorbent/500 mL. A study was carried out for
demineralised water and natural seawater, without stirring
and using a stirring velocity of 60 r/min. Results show that
the removal efficiency value is very significant. Tanned
solid wastes have a high selective affinity for oils in aque-
ous medium. The removal efficiency of the oils from a syn-
thetic oil–water mixture exceeds 90% (ranging from 90 to
100%). Observation shows that oils are removed only in the
zones that are in contact with the sorbent. Thus, the removal
efficiency (RE) of oil is a direct function of the surface ex-
posed to the oil–water interface. No significant difference
between the sorption in demineralised water and that in nat-
ural seawater bath was observed.
The high oil affinity of tested sorbents is mainly due to
the diffusion phenomenon. The pollutant penetrates into the
sorbent by capillary action and then fibers form aggregates
that can be removed easily from the water surface. The sorp-
tion of water is negligible and clearly lower than the oil
# 2007 NRC Canada
558
sorption. The sorption of water depends on the amount of
solid wastes on the surface. Results of experiments showed
that an excess of sorbent is not good because it can cause
the retention of water on the sites not impregnated by the
oil. To avoid this problem the oil sorption capacity values
must be taken into consideration. Only the necessary amount
of waste sorbent required to sorb the oil should be used and
dispersed on the water surface.
Tests revealed that the removal of oils from the water sur-
face is a quasi-instantaneous process. When wastes are
added to a beaker containing polluted water, oils are sorbed
immediately by the sorbent.
To show if there is any possibility of a chromium release
into the water medium, 0.5 g of waste and 100 mL of demin-
eralised water were placed in a rotatory agitator (250 r/min)
for 4 h. After this period, the solid and the liquid phases
were separated by gradual vacuum filtration and the liquid
was analysed. Results obtained revealed that chromium con-
centration in the filtrate is about 0.65 mg/L in the case of
chrome shavings. The release of chromium in the case of
buffing dusts is very low (0.06 mg/L).
The removal efficiency (RE) of oils is not affected by
stirring velocity of 60 r/min. Consequently, the tanned
wastes could be used efficiently in the field in the case of
tragic events due to the contamination of coastal areas with
oil spills.
Removal of saturated wastes from water
Observations show that saturated wastes float. The materi-
als remain on the water surface forever because the wastes
fibers become more hydrophobic than the raw wastes. The
removal of saturated wastes from water is easy and rapid. A
simple foaming with a sieve allows collection and evacua-
tion of solid waste from the water surface.
Conclusions
The results obtained prove the utility of using tanned solid
wastes for resolving an environmental problem. We have
demonstrated that oil can be efficiently removed from water
by sorption on tanned solid wastes. Extension of this work
for the treatment of an industrial effluent containing hydro-
carbons or oils will be the objective of future studies. The
use of natural waste materials for the removal of pollutants
from effluents prior to their treatment could decrease the
cost of operation and upgrade the quality of the treated ef-
fluents. The manufacture of sorption filter using wet-blue
shavings for industrial wastewater is one of the objectives
of our future studies.
Sorption of oils on wastes can increase the calorific value
of these materials. Consequently, these wastes can be easily
treated by incineration. The ashes obtained after thermal
treatment of wastes have a significant amount of chromium
oxide and could be used in several industries, for example,
the cement industry.
Acknowledgments
Authors acknowledge the financial support of the ‘‘Projet
Conjoint de Recherche PCI Maroco-Espagnole’’, Project N8
128/P/03 and 128/04/R/M.
J. Environ. Eng. Sci. Vol. 6, 2007
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