Professional Documents
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Environmental Technology
Vol. 32, No. 3, February 2011, 231249
REVIEW ARTICLE
A review of the use of red mud as adsorbent for the removal of toxic pollutants
from water and wastewater
Amit Bhatnagar*, Vtor J.P. Vilar, Cidlia M.S. Botelho and Rui A.R. Boaventura
LSRE Laboratory of Separation and Reaction Engineering, Departamento de Engenharia Qumica, Faculdade de Engenharia
da Universidade do Porto (FEUP), Rua Dr. Roberto Frias, 4200465 Porto, Portugal
(Received 5 August 2010; Accepted 2 February 2011 )
10.1080/09593330.2011.560615
Red mud (an aluminium industry waste) has received wide attention as an effective adsorbent for water pollution
control, showing significant adsorption potential for the removal of various aquatic pollutants. In this review, an
extensive list of red-mud-based adsorbents has been compiled and their adsorption capacities (maximum uptake
value of the adsorbent for the pollutant or adsorbate being removed) for various aquatic pollutants (metal ions, dyes,
phenolic compounds, inorganic anions) are presented. The review provides a summary of recent information obtained
using batch studies and deals with the adsorption mechanisms involved. It is evident from the literature survey that
red mud has been found to be efficient for the removal of various aquatic pollutants, especially arsenic and phosphate.
However, there is still a need to investigate the practical utility of these adsorbents on a commercial scale.
Keywords: water treatment; adsorption; industrial waste; red mud; adsorption capacity
1. Introduction
Increased industrial and agricultural activities have
resulted in the generation of various types of toxic
pollutants, which are the main cause of water pollution
on a global scale. The type of pollutants present in
wastewater mainly depends on the nature of the industry. However, some of the common pollutants generally
present in effluents are metal ions, dyes, phenols, insecticides, pesticides, detergents and a wide spectrum of
aromatics. Pollutants present in wastewaters can be
toxic to aquatic life and can cause natural waters to be
unfit as potable water sources. A number of processes
have been applied, with varying degree of success, to
the treatment of water and wastewater. Some of these
processes are coagulation [1], foam flotation [2], filtration [3], ion exchange [4], aerobic and anaerobic treatment [5,6], advanced oxidation processes [7], solvent
extraction [8], adsorption [9], electrolysis [10], microbial reduction [11], and activated sludge [12]. However,
these technologies have shown some significant disadvantages, which include insufficient removal of pollutants, high capital costs, high reagents and/or energy
requirements, and generation of toxic sludge or other
waste products that require further safe disposal.
Amongst several water and wastewater treatment
technologies, adsorption is considered as the most
versatile process. Activated carbon has been found to be
a very promising adsorbent and is commonly used for
232
A. Bhatnagar et al.
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uct, activated in air, showed promising adsorption characteristics. The effects of various factors (e.g. pH,
adsorbent dose, adsorbate concentration, temperature,
particle size) on the removal of these metal ions from
water were studied. The material exhibited a good
adsorption capacity and the Freundlich and Langmuir
models were able to fit the data. The adsorption
capacities of red mud were 64.79 mg/g for lead and
35.66 mg/g for chromium by batch method. The column
studies showed that the product could also be used on an
industrial scale. Metal ions adsorbed on the column of
this material could be quantitatively eluted with 1%
HNO3. The exhausted column could be chemically
regenerated by treating it with 1 M HNO3, and no
dismantling was required. Other salts present in the
effluents did not cause any disturbing effects.
Red mud was also examined for the removal of
cadmium and zinc from aqueous solutions [66]. The
crude form of red mud waste showed poor adsorption
properties; therefore, this material was first treated with
hydrogen peroxide at room temperature for 24 h to
oxidize adhering organic matter and was washed
several times with double-distilled water, followed by
drying at 100 C and cooling. The resulting material
was then activated in air in a muffle furnace at 500 C
for 3 h. The final product exhibited the best adsorption
capacity and optimum surface area. The product
obtained at temperatures higher than 500 C exhibited
poor adsorption capacity, which was due to the collapse
of surface functional groups on the adsorbent. The
removal of Cd2+ and Zn2+ was almost complete at low
concentrations, whereas it was 6065% at higher
concentrations at optimum pHs of 4.0 and 5.0, respectively, with 10 g/L of adsorbent in an 810 h equilibration time. The adsorption decreased with increase in
temperature. Chemical regeneration of the columns was
achieved with 1% HNO3. The Langmuir monolayer
capacity was found to be 1.16 104 mol/g for Cd(II)
and 2.22 104 mol/g for Zn(II) at 30 C.
Pellet-type adsorbents were made from red mud [67].
Adsorption of heavy metal ions (Pb2+, Cu2+, Cd2+) in
aqueous solutions by the pellet-type red mud adsorbents
were studied under various experimental conditions. It
was found that pellet-type red mud adsorbents made
from a mixture of 58.7 wt% red mud, 25.2 wt% kaolin,
11.7 wt% sodium silicate solution, 2.9 wt% fly ash and
1.5 wt% magnesium chloride at 600 C exhibited the
highest removal efficiency for the heavy metal ions. The
removal efficiency for Pb2+, Cu2+ and Cd2+ after 24 h of
operation was more than 95%. The Langmuir model was
able to fit with the experimental data. A continuous
adsorption experiment showed that the pellet-type red
mud adsorbents were effective in removing Pb2+.
Red mud has also been explored as a potential
sorbent for the removal of Cd, Zn, Cu and Pb from
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Table 1.
A. Bhatnagar et al.
Adsorption capacity of red mud for the removal of different metal ions from water.
Adsorbent
Red mud
Red mud
Activated red mud
Activated red mud
Seawater-neutralized red mud (Bauxsol)
Bauxsol-coated sand
Activated-Bauxsol-coated sand
FeCl3-coated sand
CO2-neutralized red mud (ANRM)
Activated red mud
Red mud
Red mud
Granular red mud
Red mud
Red mud
Red mud
Red mud
Treated red mud
Treated red mud
Treated red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Calcined red mud
Calcined red mud
Calcined red mud
Neutralized red mud
Adsorbate
Amount adsorbed
Reference
As(III)
As(V)
As(III)
As(V)
As(V)
As(V)
As(V)
As(V)
As(V)
Cr(VI)
Ni(II)
Cu(II)
Cd(II)
Cu(II)
Zn(II)
Ni(II)
Cd(II)
Cd(II)
Cu(II)
Pb(II)
Pb(II)
Cr(VI)
Cd(II)
Zn(II)
Cd(II)
Zn(II)
Copper
Zinc
Arsenic
Boron
8.86 mol/g
6.86 mol/g
11.80 mol/g
12.57 mol/g
6.0814.43 mol/g
1.643.32 mg/g
2.14 mg/g
23.268.5 mg/g
55.55 mg/g
30.74 mmol/g
13.69 mg/g
2.28 mg/g
38.252.1 mg/g
19.72 mg/g
12.59 mg/g
10.95 mg/g
10.57 mg/g
46.966.8 mg/g
35.275.2 mg/g
117.3165.8 mg/g
64.79 mg/g
35.66 mg/g
1.16 104 mol/g
2.22 104 mol/g
68 mg/g
133 mg/g
18.1865.17 mg/g
15.4599.20 mg/g
18.8327.51 mg/g
30.12 mg/g
[41]
[41]
[42]
[42]
[45]
[48]
[48]
[49]
[51]
[54]
[58]
[60]
[62]
[63]
[63]
[63]
[63]
[64]
[64]
[64]
[65]
[65]
[66]
[66]
[68]
[68]
[70]
[70]
[70]
[72]
Environmental Technology
239
Adsorption capacity of red mud for the removal of different dyes from water.
Adsorbent
Red mud
Red mud
Red mud
Red mud
Red mud
Acid-activated red mud
Adsorbate
Rhodamine B
Fast Green
Methylene Blue
Congo Red
Acid Violet
Congo Red
Amount adsorbed
5
(1.011.16) 10 mol/g
(7.259.35) 106 mol/g
(4.355.23) 105 mol/g
4.05 mg/g
1.37 mg/g
7.08 mg/g
Reference
[78]
[78]
[78]
[79]
[81]
[82]
240
A. Bhatnagar et al.
model fitted with the equilibrium sorption data. A maximum removal of 83% was observed at pH 8.0. Desorption of phenol from the spent adsorbent was only 41%
with water at pH 11.0, indicating that both physisorption
and chemisorption occurred in the adsorption process.
Red mud has also been used for the removal of
phenol, 2-chlorophenol, 4-chlorophenol, and 2,4dichlorophenol from wastewater [87]. The maximum
adsorption of phenol and 2-chlorophenol occurred at
pH 6.0, whereas the maximum adsorption of 4-chlorophenol and 2,4-dichlorophenol was achieved at pH
5.0 and 4.0, respectively. 2,4-Dichlorophenol and 4chlorophenol were sorbed by the developed adsorbent
by 9497%, while the removal of 2-chlorophenol and
phenol was 5081%. Adsorption of mixtures of phenols
was also tried by the researchers, and it was observed
that 2,4-dichlorophenol had the maximum adsorption in
comparison with the other phenols. The order of
adsorption was 2,4-dichlorophenol > 4-chlorophenol >
2-chlorophenol > phenol, and the adsorption achieved
was 97%, 93%, 80%, and 51%, respectively, with a
concentration of 2 105 M of each phenol. The authors
suggested that this sort of behaviour of red mud shows
non-specificity with respect to phenols, and thus it
could be used for the uptake of phenols individually or
in their mixtures. The removal of phenol and its derivatives was up to 98% by column experiments at a flow
rate of 0.5 mL/min. The order of removal was 2,4dichlorophenol > 4-chlorophenol > 2-chlorophenol >
phenol, and the removal took place through a particle
diffusion mechanism. The adsorption was found to be
endothermic in nature and followed both the Langmuir
and Freundlich models. Red mud was also used for the
dynamic uptake of 2,4-dinitrophenol, which was sorbed
by the developed adsorbent up to 95% [88]. The
removal of this pollutant reached 96% by column
experiments at the flow rate of 0.5 mL/min. The
adsorption process was found to be endothermic in
nature.
Tor et al. [89] conducted a study using neutralized
red mud for the removal of phenol from aqueous solution. To neutralize red mud, first the alkaline red mud
was suspended in distilled water with a liquid to solid
ratio of 2:1 on a weight basis, then stirred until the
Table 3.
Adsorption capacity of red mud for the removal of phenolic pollutants from water.
Adsorbent
Adsorbate
Amount adsorbed
Reference
Red mud
Red mud
Red mud
Red mud
Neutralized red mud
Acid-activated red mud
Phenol
2-chlorophenol
4-chlorophenol
2,4-dichlorophenol
Phenol
Phenol
0.630.74 mol/g
0.720.79 mol/g
0.780.82 mol/g
0.800.85 mol/g
4.12 mg/g
8.16 mg/g
[87]
[87]
[87]
[87]
[89]
[90]
Environmental Technology
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A. Bhatnagar et al.
Red mud as adsorbent for the removal of aquatic pollutants from water and wastewater.
Environmental Technology
Table 4.
243
Adsorption capacity of red mud for the removal of different anions from water.
Adsorbent
Adsorbate
Amount adsorbed
Reference
Phosphate
Phosphate
Phosphate
Phosphate
Fluoride
Fluoride
Fluoride
Nitrate
Nitrate
155.2 mg/g
202.9 mg/g
0.58 mg/g
0.210.48 mmol/g
13.46 mg/g
68.07 mg/g
91.28 mg/g
1.859 mmol/g
5.858 mmol/g
[92]
[92]
[93]
[99]
[102]
[102]
[102]
[103]
[103]
Figure 1.
Red mud as adsorbent for the removal of aquatic pollutants from water and wastewater.
positive enthalpy change (H) represents the endothermic nature of an adsorption. In some cases, negative
values of enthalpy change were reported indicating the
exothermic nature of the process. A positive entropy
change (S) denotes the affinity of the red mud and
increasing randomness at the solidsolution interface
during the sorption of adsorbates on active sites of the
adsorbent, whereas a negative value of entropy change
in some cases indicates that the degree of freedom
decreases at the solidliquid interface during the
adsorption.
3. Conclusions and future perspectives
In this review, the sorption properties of red mud, as an
adsorbent for the removal of diverse type of pollutants
from water and wastewater, have been reviewed based
Adsorbate
As(III)
As(III)
As(III)
As(III)
As(V)
As(V)
As(V)
As(V)
As(III)
As(III)
As(III)
As(III)
As(V)
As(V)
As(V)
As(V)
As(V)
As(V)
As(V)
As(V)
As(V)
As(V)
As(III)
As(V)
Cu(II)
Cd(II)
Cd(II)
Cd(II)
Pb(II)
Pb(II)
Pb(II)
Cr(VI)
Cr(VI)
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Activated red mud
Activated red mud
Activated red mud
Activated red mud
Activated red mud
Activated red mud
Activated red mud
Activated red mud
Bauxsol
Activated Bauxsol
Activated Bauxsol
Activated Bauxsol
Activated Bauxsol
Bauxsol
Activated Bauxsol
Modified red mud
Activated red mud
Granular red mud
Granular red mud
Granular red mud
Red mud
Red mud
Red mud
Red mud
Red mud
25
40
55
70
25
40
55
70
25
40
55
70
25
40
55
70
23
15
20
23
50
23
23
20
30
20
30
40
30
40
50
30
40
Temperature
(C)
b
8.86 mol/g
0.025 L/mol
7.93 mol/g
0.018 L/mol
7.17 mol/g
0.016 L/mol
6.18 mol/g
0.017 L/mol
6.86 mol/g
0.123 L/mol
7.73 mol/g
0.128 L/mol
9.60 mol/g
0.134 L/mol
10.80 mol/g
0.135 L/mol
11.80 mol/g
0.073 L/mol
8.85 mol/g
0.070 L/mol
7.93 mol/g
0.059 L/mol
4.49 mol/g
0.050 L/mol
12.57 mol/g
0.208 L/mol
14.99 mol/g
0.280 L/mol
17.15 mol/g
0.273 L/mol
17.71 mol/g
0.410 L/mol
6.0814.43 mol/g 0.010.76 L/mol
25.91 mmol/g
0.41 L/mol
28.90 mmol/g
0.52 L/mol
39.84 mmol/g
0.97 L/mol
40.98 mmol/g
1.01 L/mol
6.0814.43 mmol/g 0.010.76 L/mol
7.22 mmol/g
0.032 L/mol
23.268.5 mg/g
0.0900.142 L/mg
5.349 mg/g
0.2045 L/mg
qm
Langmuir constants
Adsorbent
Table 5.
5.93 L/mol
6.71 L/mol
17.08 L/mol
16.85 L/mol
1.066.70 L/mol
0.37 L/mol
6.718.2
1.4086
9.86 mg/g
10.02 mg/g
10.10 mg/g
1.45 104
2.24 104
0.31
KF
0.51 (M)/(M)n
0.59 (M)/(M)n
0.58 (M)/(M)n
0.42 (M)/(M)n
0.390.80 (M)/(M)n
0.59 (M)/(M)n
0.2790.365
2.501
0.25
0.27
0.31
0.20
1/n
Freundlich constants
(Continued)
[41]
[41]
[41]
[41]
[41]
[41]
[41]
[41]
[42]
[42]
[42]
[42]
[42]
[42]
[42]
[42]
[45]
[46]
[46]
[46]
[46]
[46]
[46]
[49]
[61]
[62]
[62]
[62]
[65]
[65]
[65]
[65]
[65]
Reference
244
A. Bhatnagar et al.
Adsorbate
Cr(VI)
Cd(II)
Cd(II)
Cd(II)
Zn(II)
Zn(II)
Zn(II)
Rhodamine B
Rhodamine B
Rhodamine B
Fast Green
Fast Green
Fast Green
Methylene Blue
Methylene Blue
Methylene Blue
Congo Red
Acid Violet
Methylene Blue
Phenol
Phenol
Phenol
2-chlorophenol
2-chlorophenol
2-chlorophenol
4-chlorophenol
4-chlorophenol
4-chlorophenol
2,4-dichlorophenol
2,4-dichlorophenol
2,4-dichlorophenol
Phenol
Phenol
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Neutralized red mud
Activated red mud
(Continued).
Adsorbent
Table 5.
30
40
50
30
40
50
30
40
50
30
40
50
50
30
40
50
30
40
50
30
40
50
30
40
50
30
40
50
Temperature
(C)
b
0.316 103 L/mol
8.55 103 L/mol
2.88 103 L/mol
1.04 103 L/mol
1.07 103 L/mol
2.75 103 L/mol
1.54 103 L/mol
14.28 103 L/mol
7.76 103 L/mol
4.08 103 L/mol
4.88 104 L/mol
1.66 104 L/mol
0.61 104 L/mol
1.79 102 L/mol
1.28 102 L/mol
0.84 102 L/mol
0.0360 L/mg
6.91 102 L/mg
8.88 104 L/mol
39.00 L/mol
49.20 L/mol
68.70 L/mol
40.00 L/mol
50.00 L/mol
71.00 L/mol
42.00 L/mol
51.80 L/mol
72.00 L/mol
44.10 L/mol
53.10 L/mol
72.21 L/mol
0.051 L/mg
0.101 L/mg
qm
4.05 104 mol/g
1.16 104 mol/g
1.06 104 mol/g
1.00 104 mol/g
2.22 104 mol/g
2.00 104 mol/g
1.81 104 mol/g
1.16 105 mol/g
1.06 105 mol/g
1.01 105 mol/g
9.35 106 mol/g
8.77 106 mol/g
7.25 106 mol/g
5.23 105 mol/g
4.81 105 mol/g
4.35 105 mol/g
4.05 mg/g
1.3724 mg/g
7.8 106 mol/g
0.63 mol/g
0.68 mol/g
0.74 mol/g
0.72 mol/g
0.75 mol/g
0.79 mol/g
0.78 mol/g
0.80 mol/g
0.82 mol/g
0.80 mol/g
0.82 mol/g
0.85 mol/g
4.127 mg/g
8.156 mg/g
Langmuir constants
0.579
3.90
4.55
4.60
4.60
4.65
4.70
4.72
2.74
4.80
4.82
4.83
4.85
0.513 mg/g
1.211 mg/g
0.51
1.785
1.333
1.282
1.754
1.369
1.333
4.166
3.703
1.754
KF
0.58
1/n
Freundlich constants
[65]
[66]
[66]
[66]
[66]
[66]
[66]
[78]
[78]
[78]
[78]
[78]
[78]
[78]
[78]
[78]
[79]
[81]
[83]
[87]
[87]
[87]
[87]
[87]
[87]
[87]
[87]
[87]
[87]
[87]
[87]
[89]
[90]
Reference
Environmental Technology
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Table 6.
A. Bhatnagar et al.
Results of thermodynamic studies of different pollutants on to red mud adsorbents.
Adsorbent
Adsorbate
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Activated red mud
Activated red mud
Activated red mud
Activated red mud
Activated red mud
Activated red mud
Activated red mud
Activated red mud
Granular red mud
Granular red mud
Granular red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
Red mud
As(III)
As(III)
As(III)
As(III)
As(V)
As(V)
As(V)
As(V)
As(III)
As(III)
As(III)
As(III)
As(V)
As(V)
As(V)
As(V)
Cd(II)
Cd(II)
Cd(II)
Pb(II)
Pb(II)
Pb(II)
Cr(VI)
Cr(VI)
Cr(VI)
Cd(II)
Cd(II)
Cd(II)
Zn(II)
Zn(II)
Zn(II)
Rhodamine B
Rhodamine B
Rhodamine B
Fast Green
Fast Green
Fast Green
Methylene Blue
Methylene Blue
Methylene Blue
2,4-dichlorophenol
2,4-dichlorophenol
2,4-dichlorophenol
Temperature
(C)
G (kJ/mol)
25
40
55
70
25
40
55
70
25
40
55
70
25
40
55
70
20
30
40
30
40
50
30
40
50
30
40
50
30
40
50
30
40
50
30
40
50
30
40
50
30
40
50
25.11
25.58
26.41
27.81
29.06
30.62
32.22
33.71
27.75
29.06
30.00
30.90
30.36
32.67
34.16
36.88
4.546
5.620
5.933
22.82
20.74
18.67
23.39
20.62
19.72
22.8
20.7
18.7
23.9
20.6
19.7
24.1
23.3
22.3
27.2
25.3
23.4
13.1
12.6
11.9
21.98
23.82
26.48
H
(kJ/mol)
12.83
1.85
6.88
7.08
15.822
S
(kJ/(molK))
0.0412
0.0407
0.0415
0.0438
0.1037
0.1034
0.1038
0.1034
0.0699
0.0708
0.0703
0.0699
0.1256
0.1269
0.1256
0.1281
0.069
85.94
0.208
78.50
0.183
85.9
0.21
78.5
0.18
67.1
140.1
84.6
189.6
31.0
59.1
46.50
0.23
Reference
[41]
[41]
[41]
[41]
[41]
[41]
[41]
[41]
[42]
[42]
[42]
[42]
[42]
[42]
[42]
[42]
[62]
[62]
[62]
[65]
[65]
[65]
[65]
[65]
[65]
[66]
[66]
[66]
[66]
[66]
[66]
[78]
[78]
[78]
[78]
[78]
[78]
[78]
[78]
[78]
[87]
[87]
[87]
Environmental Technology
[17]
Acknowledgements
Financial support for this work was in part provided by LSRE
financing by FEDER/POCI/2010. Amit Bhatnagar acknowledges his post-doctoral scholarship (DFRH-SFRH/BPD/
62889/2009) supported by the Portuguese Foundation for
Science and Technology (FCT).
[18]
[19]
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