Applied Physics A (2020) 126:38

https://doi.org/10.1007/s00339-019-3211-7

REVIEW

Utilization of carbon nanotubes in removal of heavy metals

from wastewater: a review of the CNTs’ potential and current
challenges
M. Bassyouni1,2   · A. E. Mansi1 · Alaa Elgabry1 · Basma A. Ibrahim1 · Omar A. Kassem1 · R. Alhebeshy1

Received: 31 August 2019 / Accepted: 3 December 2019 / Published online: 16 December 2019
© Springer-Verlag GmbH Germany, part of Springer Nature 2019

Abstract
Carbon nanotubes-based adsorbents have attracted substantial interest as potential adsorbents for heavy metals removal.
However many aspects such as the interaction between the modified carbon nanotubes (CNTs) and the heavy metal ions,
quantitative effect of the functional groups and regeneration of CNTs-based adsorbents are not fully understood yet. A
critical review was performed to compile an extensive profile from several studies of using pristine and modified CNTs for
heavy metals removal. CNTs demonstrated a great potential. However surface modification of CNTs is necessary as pristine
CNTs may be ineffective in arsenite [As (III)] or arsenate [As (V)] removal. Isotherms and kinetic models for the removal of
heavy metals are discussed in details. A particular focus has been placed on better understanding the mechanism of heavy
metals removal using CNTs-based adsorbents, affecting factors, maximum adsorption capacity and regeneration. The effect
of adsorbent dose, pH, initial concentration, and contact time were addressed by several researchers, which specifies the
consistency and performance of CNTs-based materials as potential adsorbents. To elucidate the mechanism of adsorption,
FT-IR, XPS, SEM, TEM and EDX results have been reviewed and discussed. It is found that Langmuir, Freundlich and sec-
ond order kinetic models are the most frequently used isotherm to describe heavy metals adsorption. CNTs-based adsorbent
can be efficiently regenerated.

1 Introduction Assessment Programme [219]/UN-Water 2018). Investiga-

The aquatic environment has reached a crucial level of
pollution; water contains plenty of toxic and even carcino-
genic compounds that affect every living thing in the globe.
Moreover, the applications of water in our life are uncount-
able. Water is used in industry, agriculture, and human needs
(Bassyouni et al. [17]. Each aspect of these has its environ-
mental impact on water like the disposal of contaminates of
irrigation, hazards from industry and domestic wastewater
[258]. Due to this large use of water, it is clear that sooner or
later shortage of water will occur as humans use about 4600
cubic km of water per year (United Nations World Water
* M. Bassyouni
migb2000@hotmail.com
1 adsorbent due to the high surface area and the adsorption
Department of Chemical Engineering, Port Said University,
Port Said 42526, Egypt
2 damage AC and result in a high cost of operation. To maxi-
Zewail University of Science and Technology, City
of Science and Technology, October Gardens, 6th of October,
Giza 12578, Egypt
tion of technologies of water treatment, such as oxidation/
reduction, coagulation/flocculation, biological treatment,
membrane separation, ion exchange, and adsorption, has
become the world preoccupation (Seef Saadi [52, 53, 62].
Water treatment by adsorption process is widely applied
due to the fact that it is applicable for different pollutants
(i.e., organics, inorganics and metals), used with high flow
rate, safety for environment, materials used can usually be
regenerated, and applicable for gaseous or aqueous media [4,
63]. Adsorption process is considered as surface treatment
process. Proper adsorbents should have high surface area
and porosity. In the last few decades, the application of the
CNTs for the removal of organic and inorganic pollutants
has been investigated which is comparable to other carbon-
based adsorbents that are used for commercial applications
[16, 125, 174]. Frequently, activated carbon (AC) is used as
capacity [24, 39]. However, the regeneration process can
mize adsorption performance, modified carbon atoms are
used to enhance their properties. Carbon nanotubes (CNTs)

13
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Page 2 of 33
were synthesized by Wiles and Abrahamson [232] and by
Iijima [88] and showed promising adsorption efficiency
and capacity because of its unique properties [197, 199].
Adsorption using CNTs can take place on individual single
wall carbon nanotube (SWCNTs) and SWCNTs bundles or
(MWCNTs) [25, 160]. The CNTs can be functionalized by
different methods to introduce different functional groups
(e.g., –COOH, –NH2···) which improve the adsorption abil-
ity and properties of the CNTs [21, 51, 238]. The distinction
between CNTs and the currently widely used adsorbent (i.e.,
activated carbon) can be observed in many previous reports
[129, 130, 169, 248]; usually the surface area of (AC) is
found to be higher than that of CNTs. However, a higher
adsorption capacity can be achieved by CNTs. The higher
adsorption ability of the CNTs is attributed to the fact that
average pore diameter and the pore volume of the CNTs are
found to be greater than those of AC [130, 135]. Moreover,
CNTs showed very promising results for the removal of vari-
ous heavy metals applied in industry [5]; Li et al. [118, 119,
213]. The research on wastewater treatment using CNTs is
of increasing importance as can be seen from the number of
yearly published papers shown in Fig. 1.
This paper reviews the ability of CNTs to adsorb vari-
ous heavy metals and highlighted the abundant and effec-
tive usages of CNTs in adsorption particularly at aqueous
media, and performs a brief comparison between CNTs and
some other nano-adsorbents; also the effect of experimental
conditions (such as contact time, pH, temperature, and initial
concentration of adsorbent and adsorbate) and several pos-
sible adsorption mechanisms, thermodynamics and kinetic
models are discussed in detail. In addition, the challenges
present in the face of applying CNTs in real life wastewater
treatment applications are addressed.
Fig. 1  Trend of CNTs’ published papers in water treatment. Obtained from ScienceDirect. Search words (CNTs adsorption for water treatment)
13
M. Bassyouni et al.
2 Morphology and purification
of carbon nanotubes and their effect
on the adsorption behavior
Carbon nanotubes (CNTs) are a kind of carbon allotropes
with an aromatic surface rolled up to form a cylindrical
structure [217]. Based on the number of cylindrical shells,
CNTs can be classified into single wall carbon nanotubes
(SWCNTs) if there is a single shell, and multi-wall carbon
nanotubes (MWCNTs) if a plurality of shells constitute
the molecule. The length of CNTs varies from 10 s of nm
to 10 s of mm [127] and the reported diameters vary from
0.7 to 2.5 nm for SWCNTs, and 4 to 150 nm for MWCNTs
[91].Carbon nanotubes have very good textural proper-
ties, i.e., large specific surface area, large pore volume
and average pore diameter, which are the main factors that
determine the adsorption capacity [73, 184]. Several stud-
ies highlight the porous nature of the CNTs [240, 242].
The nature of the pores in MWNCTs can be classified
as small diameter-inner hollow pores ranging from 3 to
6 nm (the inner diameter of the MWNCTs) and aggregated
pores ranging from 20 to 40 nm, formed by the interaction
of isolated MWCNTs [242]. The structure of CNTs and
the functional groups present on its surface allow strong
interaction with both inorganic and organic molecules
through different intermolecular forces such as van der
Waals forces, hydrogen bonding and π–π stacking (in case
of aromatic compounds) [185, 206]. This is due to the
previous reasons: carbon nanotubes have relatively higher
adsorption capability compared to the other commonly
used adsorbents which will be discussed in following sec-
tions. SWCNTs bundles are formed due to van der Waals
Utilization of carbon nanotubes in removal of heavy metals from wastewater: a review of the CNTs’…
interactions. The textural properties are mainly affected
by the diameter of the SWCNTs and the number of tubes
constituting the bundle. Different and higher number of
adsorption sites are available in the case of SWCNTs bun-
dle than those available in the case of individual nanotubes
[13, 183]. As seen in Fig. 2, the adsorption on SWCNTs
bundle can occur at four different sites [136, 183, 198]:
1. the outer surface of the nanotubes
2. the inner surface of the nanotube (in case of open ends),
3. the grooves at the area of contact between adjacent
tubes,
4. the interstitial channels formed between the tubes in
bundles.
In contrast to SWCNTs, MWCNTs do not form bundles.
The adsorption active sites available are the inner and outer
surfaces of the nanotubes plus the aggregated pores within
the adjacent tubes as shown in Fig. 3 [136, 242].
Fig. 2  Possible adsorption
sites on a bundle of SWCNTs
(a) and Transmission electron
microscope (TEM) image of a
SWCNTs bundle (b) from [136]
with permission
Fig. 3  Adsorption sites avail-
able on MWCNTs (a) and
(TEM) image of aggregated
MWCNTs (b) from [136] with
permission
Page 3 of 33  38
Carbon nanotubes may contain side products as impurity
which affect the CNTs’ adsorption ability. The main impuri-
ties are graphite sheets (wrapped up), particles and graphitic
polyhedrons, amorphous carbon, small fullerenes, substrate
materials and metal catalysts [136].The metal catalyst par-
ticles remain at the base of the nanotubes or on its tip or it is
incorporated within the nanotubes [90].
Purification techniques available for CNTs can be cat-
egorized into two groups, namely physical and chemical
purifications methods. The physical purification methods
are based on the difference in the physical properties of the
nanotubes and the present impurities. Examples of these
methods are magnetic separation, settling, physical pro-
cesses based on difference in particle size [217]. In gen-
eral, physical purification methods are used to remove small
aggregates of fullerenes, graphitic sheets or separate CNTs
having different aspect ratios [139]. These processes are
relatively mild and do not cause severe damage to the tubes,
but they are normally more complex and less effective [193].
13
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Page 4 of 33
The chemical purification methods are mainly based on
the facts that the rate of oxidation of carbonaceous impuri-
ties is higher than that of the CNTs, and that the metal-
lic impurities are dissolved by acids. Chemical oxidation
normally introduces unavoidable defects on the surface of
tubes and the pentagonal structure at the tube ends, causing
remarkable damage to the structure and morphology of the
CNTs [139]. The most commonly used chemical purification
method involves oxidation of as-synthesized CNTs in either
gas phase using O ­ 2, ­Cl2, ­H2O, etc., or liquid phase conditions
using a solution of strong acids. Oxidants commonly used
for liquid phase oxidation include acids such as H ­ NO3−, oxi-
dizing agents as H ­ 2O2 and ­KMnO4 or using a mixture of oxi-
dizers such as HCl–H2O2 and ­H2SO4–HNO3. Chemical puri-
fication introduces new functional groups to the nanotube
surface as shown in Fig. 4. As mentioned earlier, chemical
purification methods have some drawbacks; they normally
introduce unavoidable defects on the surface of tubes and
may severely damage the CNTs’ structure. However, nitric
acid is widely used in chemical purification methods, due
to its mild oxidation ability which can selectively remove
metal catalysts’ support and amorphous carbon impurities.
In addition, it is also inexpensive and abundant [139].
The purity of CNTs depends on the exposure time and
the turbulence in the medium (often induced by acid reflux-
ing). Nitric acid was tested under reflux for short duration
(30 min) by Mohanapriya and Lakshminarayanan [151],
and it was observed that the metal particles were dissolved
Fig. 4  Illustration of common
functional groups and adsorp-
tion behaviour variation [246]
13
M. Bassyouni et al.
effectively and the tube tips were opened without causing
significant structural damages to the CNTs. The removal of
most of the catalyst particles in nitric acid reflux treatment
with a prolonged duration up to 24 h at high temperature has
been studied in several researches [230]. The metal particles
as well as the carbonaceous impurities could be effectively
dissolved and removed from CNTs. However, in such harsh
conditions, some oxidative damages were induced to the
sidewalls of the nanotubes; an increase in the defects’ popu-
lation was observed in the sample. The increase of defects’
population generally increases the surface reactivity toward
the adsorption [14, 116].
The effect of the other oxidants was also tested in sev-
eral researches. Previous studies [80, 86] reported that
hydrofluoric acid is effective in removing zeolite catalyst
support without damaging the structure of the nanotubes.
Hydrogen peroxide (­ H2O2) cannot remove metal particles.
Therefore, it is usually used together with HCl [139]; the
mixture was shown to be effective in the removal of iron
particles from the CNTs surface [230]. In addition to acids,
alkali compounds may also be used. Sodium hydroxide for
example undergoes a redox reaction with carbon at the high
reactive sites of the material. Consequently, NaOH reacts
only with defective parts of the carbon nanotubes and with
disordered carbon impurities [181]. Moreover, NaOH was
reported to be effective in the removal of the catalytic sup-
port and residual metal particles without damaging the side
walls of the tubes [94]. Most of mentioned oxidants remove
Utilization of carbon nanotubes in removal of heavy metals from wastewater: a review of the CNTs’…
metals more effectively than carbonaceous impurities [139].
To solve this issue, an alkali or acidic solution in the pres-
ence of ­KMnO4 is used. The effect of the alkali solution and
­KMnO4 on the purification of SWNTs was investigated by
[251]. It was observed that alkali solution and K
­ MnO4 has a
slightly lower oxidation effect than the acidic solution, and
is therefore strong enough to attack the nanotube walls and
produce several functional groups on the surface, but can-
not open the tips effectively. The acidified K
­ MnO4 solution
showed harsher oxidation conditions which resulted in tips
opening [38].
3 Heavy metals adsorption from aqueous
solutions on carbon nanotubes
Maintaining a safe level of heavy metals in water is crucial
due to their carcinogenicity and toxicity which may cause
severe damage to various systems of the human body. Unlike
organic contaminants, heavy metals do not biodegrade over
time so they threaten the living organisms [64]. It is hard to
prevent the presence of heavy metals in wastewater as their
presence is due to many industrial activities such as smelt-
ing, surface finishing industry, mining, metallurgy. Moreo-
ver, the presence of heavy metals even at low concentrations
can cause environmental and health problems [93]. In this
section the ability of carbon nanotubes to adsorb different
heavy metals and the effect of various parameters such as
temperature, pH, adsorbent and adsorbate concentrations are
discussed.
3.1 Mercury
Mercury (II) is one of the most toxic heavy metals affect-
ing human health [163]; many adsorbents have been tested
for the removal of mercury from aqueous solutions [204,
210, 220]. However, CNTs were shown to be much more
effective than all the tested adsorbents which included the
commonly used activated carbon. A previous report for the
removal of mercury using MWCNTs produced by chemi-
cal vapor deposition (CVD) showed that the maximum
removal of mercury (II) occurs at neutral pH (6.5–7.5) and
the adsorption experimental data fitted well by Langmuir
isotherm. The thermodynamic investigation showed that
adsorption of mercury on MWCNTs is endothermic and
consequently the adsorption capacity and rate of adsorption
increased by increasing temperature. Adsorption capacity
of 93.45 mg g−1at 37 °C was achieved [200]. Moreover,
other reports confirm these results; as-produced MWCNTs
were utilized by Yaghmaeian et al. [239] to remove mer-
cury, and adsorption capacity of 25.64 mg g−1 was achieved
at 25 °C. Increasing the initial concentration of mercury
from 0.1 to 10 mg L−1 decreased the removal percentage
Page 5 of 33  38
from 70 to 45% at the given set of conditions. The work by
Chen et al. [32] showed that modifying CNTs significantly
increased the adsorption capacity. Capacities of 120.1 and
127.6 mg/g at room temperature were achieved for MWC-
NTs-OH and MWCNTs-COOH, respectively, and the rate
of adsorption was highest for MWCNTs-COOH at low con-
centration of mercury (i.e., 0.02 mg/l). A previous study
showed that the higher rate of adsorption is attributed to
the fact that the oxygen-rich functionalized MWCNTs were
more hydrophilic, which facilitated the external diffusion
of adsorbate to the adsorbent external surface [32]. Saleh
[192] performed SEM with EDX test to assert the adsorp-
tion of Hg(II) on S ­ iO2-CNT. EDX spectrum was recorded
and shown in Fig. 5a. The presence of Hg(II) can be char-
acterized by peaks at 2.195 and 9.987 keV, which indicates
the affinity of ­SiO2-CNTs toward mercury. Also, the car-
bon peaks at 0.277 keV, oxygen at 0.525 keV, and silica at
1.74 keV can be observed. A scanning electron microscope
at 20 kV (at the right of Fig. 5a) showed the morphology
of the S­ iO2-CNTs loaded with Hg(II). The uniform distri-
bution of silica nanoparticles across the nanotubes and the
presence of the mercury on the S ­ iO2-CNTs surface also
can be confirmed by EDS which appears as pink spots in
Fig. 5b. Sulfur-containing MWCNTs-S were tested by Pil-
lay et al. [170] for removing mercury and the result showed
that mercury has high affinity for sulfur. Thus, adding sulfur
to MWCNTs greatly increased the selectivity of mercury
adsorption. The removal percentage of mercury increased on
increasing sulfur content and reached almost 100% for the
maximum amount of sulfur that could be incorporated onto
the MWCNTs (3.97%). The result also showed that unlike
the normal MWCNTs, the removal percentage of mercury by
S-MWCNTs increases with increasing pH up to the value of
14, which could be attributed to the Hg(OH)n (where n = 1,
2, 3) forms of mercury,which are present at this range of
pH, are strongly attracted and adsorbed onto the more nega-
tively charged surface of MWCNTs-S than the unmodified
MWCNTs.
3.2 Zinc
Zinc is considered a hazardous heavy metal that comes from
processes such as galvanizing plants, municipal wastewater
treatments and ores [110]. The World Health Organization
(WHO [234] stated that the maximum concentration of zinc
allowed in drinking water is 5.0 mg L−1. Single and multi-
wall carbon nanotubes purified with NaOCl were utilized
in removing zinc ions from aqueous solution [128]. The
calculated maximum adsorption capacities were 43.66 and
32.68 mg g−1 for SWCNTs and MWCNTs, respectively,
and for unmodified CNTs were 10.21 and 11.23 mg g−1 for
MWCNTs and SWCNTs, respectively. Zinc removal was
observed to be higher at lower concentrations of zinc than
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Page 6 of 33
Fig. 5  a SEM image with EDX spectrum of mercury-loaded ­SiO2-CNT and b EDS mapping images mercury-loaded S
at higher concentrations. The highest removal percentage of
zinc was observed at pH 8, which is attributed to the fact that
below pH 8 the dominant zinc species is ­Zn2+ [114]. Hence,
at low pH value, H ­ + ions will compete with Z ­ n2+ ions for
the active sites on the CNTs’ surface. Moreover, at pH 8
the surface of the CNTs becomes negatively charged, which
promotes electrostatics interactions and enhances adsorp-
tion; higher than pH 11, a sharp decrease in the removal of
zinc was observed, which can be attributed to dominance
of Zn(OH)31− and Zn(OH)2− 4 ions in this pH range [114];
this created electrostatic repulsion with the negative sur-
face of the CNTs. The work by [152] showed the effective-
ness of MWCNTs for zinc adsorption, achieving a removal
efficiency of 96.65%; the optimum pH was 5, due to the
decrease in the number of ­H+ ions competing for the active
site; the experimental data were best fitted by Freundlich
isotherm. Another study by Kosa et al. [106] showed that
when MWCNTs were modified with 8-hydroxyquinoline
(8-HQ) the efficiency was increased, where equilibrium was
reached after approximately 10 min. The removal percent-
ages were 79% and 96% for MWCNTs and 8-HQ-MWCNTs,
respectively, while the adsorption of Z ­ n+2 ions increased
from 19.13 to 83.40% when the pH increased from 2 to 6.
Those results ensure that CNTs are an effective material that
can be used to adsorb ­Zn+2 ions from aqueous medium.
3.3 Chromium
Hexavalent chromium (Cr(VI)) is one of the widely used
heavy metals in industry; in contrast to trivalent chromium,
Cr(VI) has a toxic effect on the living [20, 150]. A study by
Di et al. [49] showed that acid-refluxed CNTs have a good
adsorption behavior over a wide pH range. The removal
13
M. Bassyouni et al.
­ iO2-CNT [192]
percentage of Cr(VI) was very high (more than 95%) at
acidic and neutral pH and dropped sharply at pH 8. This
can be ascribed to the point of zero charge (­ pHpzc) of the
CNTs that is found to be 7.7. Hence, below 7.7 the CNT’s
surface is positively charged, which enhances adsorption
of ­Cr2O72− and H
­ CrO4− ions present at this pH range. The
adsorption data were well expressed by Langmuir isotherm
with a maximum adsorption capacity of 26.88 mg g−1 at pH
7.5 and 25 °C. [Huang et al. [85]] showed that the applica-
tion of magnetic MWCNTs (M-MWCNTs) enhanced the
adsorption of Cr(VI) ions and facilitated the separation of
the nanotubes from the solution. The adsorption process on
M-MWCNTs was endothermic and well described by Lang-
muir isotherm. The removal of Cr(VI) was highly dependent
on pH and the adsorption capacity decreased on increasing
pH from 3 to 9. The adsorption process was well fitted by the
pseudo second-order kinetics and showed a faster reaction
rate at lower concentrations of Cr(VI). Surface morphol-
ogy of nano zero-valent iron multi-wall carbon nano tubes
(nZVI–MWCNTs) was examined by [133] using TEM and
SEM before and after adsorption of Cr(VI). TEM image of
nano zero-valent iron loaded on MWCNTs before adsorp-
tion is shown in Fig. 6a. The bright spherical spots and the
globular nodules were proved to be nZVI particles by TEM
images (at the right bottom of Fig. 6a). After adsorption of
Cr(VI), the nZVI–MWCNT nanocomposites exhibit some
polygon shapes due to the co-precipitation of chromate and
iron ions as shown in Fig. 6b. XRD patterns of bare MWC-
NTs and of nZVI–MWCNTs before and after adsorption are
shown in Fig. 6c. An XRD test showed that nZVI–MWCNT
nanocomposites still have the same structure as MWCNTs
and the framework of MWCNTs was not damaged. The pres-
ence of nZVI is observed by the presence of the apparent
Utilization of carbon nanotubes in removal of heavy metals from wastewater: a review of the CNTs’…
Fig. 6  a SEM and TEM images of nZVI supported on MWCNTs before adsorption, b SEM images of nZVI supported on MWCNTs after
adsorption of Cr(VI), and c XRD patterns of bare MWCNTs, nZVI–MWCNTs before an nZVI–MWCNTs after adsorption [133]
peak at 2θ = 44.90° which confirmed that the nZVI nanopar-
ticles might either load outside the carbon tubes or inside the
pores and cracks of the network. Peaks indicate the forma-
tion of γ-Fe2O3 (2θ = 36°) ­Fe3O4 (2θ = 36°/57°/62.5°) and
­Cr2FeO4 (2θ = 35.50°) after adsorption.
A different route of modifying CNTs can be conducted
by non-covalent wrapping. Previous research [253] applied
non-covalent wrapping to MWCNTs using polydiallyldime-
thyl ammonium chloride (PDDA). The MWNCTs-PDDA
nano composite was then tested for the adsorption of Cr(VI)
ions. The adsorption process on the MWNCTs-PDDA was
highly pH dependent, with the removal percentage increas-
ing on increasing pH from 2 to 5.1, where it reached a 100%
removal. Moreover, pristine MWCNTs achieved a removal
percentage of about 65% at the pH value of 5.1. Below pH
2, no notable adsorption occurred because Cr(VI) exists
in the neutral molecular form at this pH range [195]. The
adsorption using MWNCTs-PDDA was also tested under
flow conditions and the adsorption was favorable at lower
flow rates [253].
3.4 Arsenic
Arsenic is one of the most hazardous heavy metals for living
organisms. Arsenic produces negative effects on the human
health even if it presents at low concentration. Therefore,
a maximum concentration of 10 µg per liter of arsenic in
water was determined by WHO [235]. Arsenic is found in
two different oxidation states; arsenite or As (III), which is
a soluble, neutral, and uncharged molecule, is considered
more toxic than arsenate As (V), and is more difficult to be
removed from aqueous media [166]. Many previous studies
showed that both arsenic forms did not show any notable
adsorption on neither the surface of as-produced CNTs nor
on the oxidized CNTs [147, 161, 162]. Therefore, differ-
ent modifications were adapted to enhance the adsorption
of arsenic on CNTs. MWCNTs-zirconia nanohybrid were
Page 7 of 33  38
applied by Ntim and Mitra [162] and adsorption capaci-
ties of 2 and 5 mg g−1 were achieved for As (III) and As
(V), respectively. The adsorption process is best described
by the pseudo second order kinetics, and removal rate of
As (V) was higher than As (III). The optimum pH for As
(V) removal is found to be pH 6. This is due to the fact
that at pH 6 the dominant As (V) species is HAsO−2 4 [142]
and the point of zero charge ­(pHPZC) of MWCNTs-zirconia
nanohybrid is 6.9 [162], hence this strong attraction due to
charge difference increased adsorption for As (V). On the
other hand, As (III) maintained an almost constant removal
percentage at the range of pH studied (5–8). The work of
[Manning et al. [142]] showed that As (III) is present in
the neutral molecular form ­(H3AsO3) at pH < 8; hence con-
stant removal was shown in the studied pH range. Previ-
ous reports showed that iron oxide-modified CNTs have a
good affinity for arsenic adsorption [147, 161]. A previous
study by Veličković et al. [222] showed that iron oxide-
modified ethylenediamine MWCNTs (e-MWCNTs/Fe+2 and
e-MWCNTs/Fe+3) presented higher adsorption affinity for
As (V) than As (III). Thermodynamic study of the adsorp-
tion process showed that the adsorption is endothermic,
and spontaneous. The maximum adsorption capacities of
As(V) removal were found to be 24.69 and 14.45 mg g−1
using e-MWCNTs/Fe+2 and e-MWCNTs/Fe+3 respectively
at 45 °C. The optimum pH for As (III) adsorption was found
to be 8. At this pH value, the kinetics of adsorption of As
(V) were faster than As (III). Generally, e-MWCNTs/Fe+2
achieved higher adsorption capacities than e-MWCNTs/
Fe+3, due to the fact that at higher iron loading (the e-MWC-
NTs/Fe+2 sample), the surface potential of the adsorbent
becomes less negative [140], thus more attractive towards
the negatively charged arsenic species that were mentioned
above. FTIR analysis for e-MWCNTs/Fe+2 before and after
adsorption of 1 mg L−1 and 4 mg L−1 of As (V) is shown in
Fig. 7. It can be observed that the Fe–OHn (where n = 0, 1,
2) bands start to weaken after adsorption of As (V), peaking
13
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Page 8 of 33
Fig. 7  FTIR spectra of MWCNTs/Fe+2 a before adsorption, b after
As (V) adsorption from 1 mg L−1 aqueous solution and c after As (V)
adsorption from 4 mg L−1 solution [222]
at 974, 1043 and 1124. This provides that the adsorption
on the surface of MWCNTs/Fe+2 is mainly due to the pres-
ence of ­O−, ­OH− and ­OH2+ functional groups. Issa et al.
[89] reported that the increase in percentage removal of
As (III) at pH 8 might be attributed to the existence of As
(III) as a negative anion which promotes adsorption on the
active sites of iron oxide surface. (Presence of ­OH+2 ions
was reported at this pH value even though the surface of the
e-MWCNTs/Fe+2 itself bears a negative charge (­ pHPZC = 7.5
for e-MWCNTs/Fe+2).
Other studies [71, 252] utilized novel mixed oxides to
enhance arsenic adsorption. Chen et al. [28, 33] incorporated
Cerium-iron mixed oxide into the surface of MWCNTs with
the aid of alkylbenzene sulfonate surfactant (NASDBS); the
synthesized nanotubes (CNTs-CF) exhibited high adsorption
capability of both oxidation states of arsenic with adsorp-
tion capacities of 30.96 and 28.74 mg.g−1 for As (V) and
As (III), respectively, at 25 °C. The adsorption process was
best described by pseudo second order kinetics with As (V)
being adsorbed faster than As (III). The optimum pH for
As (III) adsorption was found to be 8, while that of As (V)
was found to be 3 in this case, and above pH 3 the removal
percentage dropped rapidly. This is due to the fact that below
pH 2.3, As (V) exists in molecular form and negative anion
is found at pH higher than 2.3 [232]. The deprotonation of
surface hydroxyl groups occurred with further increasing
pH, resulting in a negatively-charged surface which created
repulsion between the surface and As (V) negative anions.
3.5 Lead
Lead is considered one of the most hazardous heavy metals
that affects human health. It is a general enzyme inhibitor
and metabolic poison. It can accumulate in brain, kidney,
13
M. Bassyouni et al.
bones, and muscles [48]. There are various techniques
applied for the removal of lead from wastewater. However,
the adsorption process using carbon nanotubes shows excep-
tional removal efficiency of lead from wastewater. A previ-
ous study by (Li et al. [117]) for the removal of ­Pb2+ using
CNTs fabricated by catalytic pyrolysis of hydrogen–pro-
pylene mixture showed that CNTs have weak adsorption
capability of P ­ b2+ and increase with increasing pH in the
range of 3–7. The adsorption capacity increased remarkably
when CNTs were refluxed with concentrated nitric acid. The
experimental data was best expressed using Freundlich iso-
therm and a maximum adsorption capacity of 49.95 mg g−1
at pH value of 7. In addition, Atieh et al. [8] reported that
removal percentage of lead of nearly 100% is achieved using
modified CNTs at pH 7, while the percentage removal at
pH 4 and 5 was 17% and 25%, respectively. This is because
modifying the surface of CNTs can make it more negatively
charged, hydrophilic and form various functional groups
which promote adsorption. Li et al. [117] reported that pre-
cipitation of Pb(OH)2 will occur at pH > 7. Thus, adsorption
is preferred under acidic conditions; otherwise the removal
of ­Pb2+ will be due to the cooperating role of adsorption
and precipitation. Another study [247] reported that modi-
fying MWCNTs by oxidation using plasma enhanced the
adsorption capacity of lead. Oxidation of CNTs using these
techniques resulted in introducing more oxygen-containing
functional groups (e.g., COOH, OH, etc.) on the surface of
the nanotubes, increasing the specific surface area, number
of surface defects, removing some amorphous carbon and
MWCNTs caps and improving the dispersion of CNTs in
water. Xu et al. [237] also confirmed these results by apply-
ing XPS spectra for free-dried samples of Pb(II) adsorbed
on oxidized MWCNTs at pH 6.05 and 8.86 (Fig. 8). A high
resolution XPS C1s spectrum is shown in Fig. 8a. The typi-
cal graphitic carbon at 284.7 eV, which represents the C1s’
binding energy of the MWCNTs, shows that there is no dif-
ference in C1s spectra of the two samples. This is due to the
fact that the species of carbon is not influenced by pH values.
Figure 8b shows the high resolution XPS O1s spectra of the
sample around 532.5 eV. It is apparent that there is a dif-
ference between the oxygen peaks at pH 6.05 and pH 8.86.
This difference is due to the presence of oxygen-containing
functional groups on the surface of oxidized MWCNTs (e.g.,
carboxyl oxygen [–O–C=O(H), 533.6 eV] and carbonyl oxy-
gen =C=O,[530.7 eV]), which enhance the adsorption of
lead ions. The oxygen peak is shifted by 0.55 eV between pH
8.86 and 6.05 as Pb (OH)2 pellets begin to form and cover
the adsorbent surface at pH 8.86. Other works [72, 225]
showed that at pH < 7, the removal was mainly attributed to
the adsorption of P ­ b2+ and Pb(OH)+. The removal of lead
maintained a constant maximum value at pH range of 7–9.
This can be attributed to the fact that at this range of pH, the
removal of lead was achieved by simultaneous adsorption
Utilization of carbon nanotubes in removal of heavy metals from wastewater: a review of the CNTs’…
Fig. 8  XPS spectra for free-dried samples of Pb(II) adsorbed on MWCNTs. a C 1 s; b O 1 s [237]
of ­Pb2+ and Pb (OH)+ ions and precipitation of Pb (OH)2
[72, 237].
3.6 Cadmium
Listed as the 7th most hazardous substance [9], Cadmium
enters the environment through several ways including elec-
tronic waste runoff, metal refinery discharges and erosion
of natural deposits [9]; EPA [56, 57, 231]. Previous studies
confirmed that CNTs are an efficient adsorbent for cadmium
removal from aqueous solutions. A recent study by Akl and
Abou-Elanwar [3] showed that modification of CNTs by
­HNO3 increases the number of oxygen-containing groups
on the surface of CNTs with increase in surface area. The
adsorption of Cd (II) by modified CNTs was tested at pH
range (2–6.5) and the percentage removal of Cd (II) was
found to increase with increasing pH. The adsorption of
Cd (II) was previously confirmed to be higher at alkaline
range [119]. However, this range is avoided in adsorption
experiments to prevent precipitation of Cd(OH)2, so that
the removal of cadmium would be attributed to the adsorp-
tion process only. Therefore, pH range (2–6.5) is favorable
for adsorption experiments of Cd (II). The surface of CNTs
becomes more negatively charged with increasing solu-
tion pH. This is attributed to functional groups dissociation
(e.g., COOH becomes C ­ OO−) which enhances electrostatic
attractions between the positively charged Cd (II) ions and
the negatively charged surface of the nanotubes [3]. A com-
parison study by Li et al. [119] for the adsorption of Cd
(II) using oxidized CNTs with ­H2O2, ­HNO3, and ­KMnO4
showed that oxidation with nitric acid can break CNTs into
smaller chains and open the tips, which greatly increases the
Page 9 of 33  38
pore volume of CNTs. Meanwhile, weak oxidation abilities
were observed for ­H2O2 and ­KMnO4 and no increase in pore
volume was obvious. Results showed that the adsorption
capacity of the as-grown CNTs for Cd (II) is 1.1 mg g−1,
while the adsorption capacities increase for the H ­ 2O2 and
­HNO3 oxidized CNTs and reach 2.6 and 5.1 mg g−1, respec-
tively. Akl and Abou-Elanwar [3] also reported that increas-
ing the adsorbent concentration increased the removal per-
centage of Cd (II). This is expected because the higher the
dose of adsorbents in the solution, the higher the number of
active sites available for adsorption. It was also found that
the amount of Cd (II) ions adsorbed per unit mass of adsor-
bent decreases on increasing the adsorbent dose. This is due
to the fact that, increasing the adsorbent dose at constant
initial concentration of ions will at some point result in the
unsaturation of the adsorbents active sites (i.e., not all of the
available active sites were occupied [119, 203, 245].
3.7 Copper
Copper is a hazardous heavy metal at higher concentration
levels [208]; beyond permissible limits it is classified as a
carcinogenic substance, which causes learning disorders
and can accumulate in kidneys. For these reasons it must
be removed from industrial waste water [75]. A previous
study by Stafiej and Pyrzynska [211] showed that carbon
nanotubes have good adsorption properties and high capac-
ity for Cu (II) adsorption. A recent study by Sobhanardakani
et al. [208] showed that oxidized multi-walled carbon nano-
tubes (O-MWCNTs) were used as adsorbent for the removal
of copper ions from aqueous solution; their pore volume
and average pore diameter are greater than the as-produced
13
38 
Page 10 of 33
MWCNTs. Langmuir adsorption model showed agreement
with the experimental data. Results showed that the maxi-
mum adsorption capacity of copper ions was 200 mg g−1
at 25 °C, the optimum pH for this adsorption process was
found to have the value of 6 and a maximum removal per-
centage of 99.5% was achieved at the optimum pH value.
The single and competitive adsorption of Pb, Cu and Cd
by CNTs was studied by [Li et al. [118]]. The experimental
data sets showed that the adsorption affinity by MWCNTs
followed the order Pb < Cu < Cd; the as-prepared CNTs were
immersed in a mixture of HF and ­HNO3 and then reflux in
­HNO3. In between pH 1.8 and 6, the removal percentages
of Cu increased sharply and almost attained values of 100%,
the Langmuir adsorption model fitted well to the experimen-
tal data and the maximum adsorption capacity was found
to be 24.49 mg g−1 [118]. Another competitive adsorption
study with even more heavy metals using CNTs soaked and
reflux in H
­ NO3 [211] showed an adsorption affinity of the
order Cu < Pb < Co, which does not confirm the order men-
tioned above; this might be attributed to the change in the
manufacturing methodology. Freundlich adsorption model
agrees well with the experimental data and the adsorption
capacity of copper remains almost constant even in the pres-
ence of other metals.
3.8 Nickel
Nickel is regarded as one of the most harmful heavy met-
als that is characterized as a non-biodegradable toxic
heavy metal ion causing several issues to the human
Fig. 9  FTIR spectra of a raw MWCNTs, b Ni (II)-adsorbed MWCNTs by [1]
13
M. Bassyouni et al.
body [99]. Nickel is widely used in industry and is com-
monly found as an effluent; more than 40% of nickel is
used in steel production, some alloys and nickel batteries
[2]. Many separation processes have widely been applied
for nickel removal [29]. However, adsorption process is
found to be more effective for nickel removal because of
the high efficiency and low cost [40, 101]. FTIR spectra
of raw MWCNTs and Ni (II)-loaded MWCNTs (Fig. 9)
were studied by Abdel-Ghani et al. [1]. The stretching
band of C–C at 1420 cm −1 on raw MWCNTs was split
into 1419 and 1461 cm−1 after adsorption of nickel ions.
The appearances of peaks at around 400 cm −1 refer to the
strong bonding between the Ni (II) ions and the nano-
tube through oxygen-containing functional groups. These
oxygen-containing functional groups increase the adsorp-
tion capacity of nickel ions as they provide numerous
adsorption sites [214]. Acid-oxidized MWCNTs were
applied in the removal of nickel; the removal efficiency
increased from 10% to nearly 80% on increasing the pH
from 3.5 to 8. The adsorption data was well fitted using
with Langmuir isotherm with a calculated adsorption
capacity of 9.8 mg g−1 at initial pH 6.55 and 60 °C [29].
Wilson et al. [233] reported an adsorption capacity of
49.26 mg g −1 by oxidized CNTs. Moreover, in another
experiment using oxidized MWCNTs [243], adsorption
of Ni (II) increased gradually from about zero to ~ 99% at
pH 2–9. The increase in removal percentage with pH is
due to the fact that below pH 9 the dominant species of
nickel is ­Ni2+. Therefore, further increasing the pH makes
the surface of the CNTs more negative, which promotes
Utilization of carbon nanotubes in removal of heavy metals from wastewater: a review of the CNTs’…
adsorption. The MWCNTs were further decorated with
polyacrylic acid which in turn made the surface more
negative and enhanced the adsorption more than the oxi-
dation of the nanotubes alone.
3.9 Cobalt
Cobalt (Co) is an essential element to human health [132].
On the other hand, however, increasing its amount in water
can cause toxic, carcinogenic and mutagenic effects (Wang
et al. [226, 227]. Many methods, such as bio-reduction and
chemical precipitation, are used to eliminate or decrease
the concentration of Co (II) to permissible limits [11, 107].
But these methods show low removal efficiency and may
require special operating conditions (Wang et al. [226,
227]. Recent studies indicated that MWCNTs have high
adsorption capacity of Co (II) [145, 164] but are difficult
to separate from the solution. Therefore, magnetic MWC-
NTs/iron-oxide (MWCNTs/IO) composites are used to
assure separation process, although it has lower adsorption
capacity than MWCNTs (Wang et al. [226, 227]. Results
show that Co (II(removal increased slightly with increas-
ing pH within pH range of 3–6, exhibited a pronounced
rise between pH range 6–7 and reaches a percentage
removal value of 96% at pH > 10. This is because the sur-
face of MWCNTs/IO composites becomes more negative
on increasing the pH, resulting in stronger interactions
between the surface and ­Co2+ ions. Co (II) sorption is an
endothermic process fitting well using Langmuir model
with maximum adsorption capacity of 0.18 (mmol/g) at
333.15 K. Moreover, a reduction in MWCNTs/IO agglom-
eration provides more sorption sites (Wang et al. [226,
227]. Another study by Yang et  al. [244] shows that
hydrophilic group (–SO3H) incorporate onto the surface
of MWCNTs to form sulfonated magnetic multi-walled
carbon nanotubes (SM-MWCNTs) to overcome the aggre-
gation and dispersion problem of MWCNTs and increase
the sorption capacity. The adsorption with SM-MWCNTs
fitted Langmuir model with maximum adsorption capacity
of 8.42 mg g−1 at 298.15 K. Moreover, adsorption using
CNTs soaked and reflux in ­HNO3 fitted well with Freun-
dlich adsorption model.
A summary of many previous reports concerning the
adsorption of heavy metals from aqueous solutions is listed
in Table 1. For each heavy metal, different types of CNTs
(i.e., SWCNTs, MWCNTs, Functionalized CNTs) were
tested for their adsorption capacities obtained from Lang-
muir isotherm (see Sect. 5); the experimental conditions at
which these capacities were obtained, the best experimen-
tal conditions at which the highest removal percentage of
a particular metal was achieved and finally the best fitting
isotherm and kinetic model for the experimental data.
Page 11 of 33  38
4 Adsorption of heavy metals using
adsorbents other than CNTs
In the previous section, the potential of CNTs in the removal
of heavy metals from aqueous solution was discussed.
CNTs showed very promising adsorption behavior in vari-
ous experimental conditions. A wide range of adsorption
capacities and adsorption kinetics were obtained for the
as-produced CNTs and CNTs functionalized with different
methods and compounds. In this section, adsorbents other
than CNTs are reviewed. The adsorption isotherms and
kinetic models of activated carbon and many other natural
and synthetic adsorbents are listed in Table 2. For the sake
of comparison, the same data obtained for CNTs (in Table 1)
are obtained for the other adsorbents in Table 2.
5 Adsorption isotherms and kinetic models
An adsorption isotherm is a mathematical relation between
the quantity adsorbed (usually expressed as mg adsorbed per
gram of adsorbent) and the composition of the bulk phase
under equilibrium conditions and at constant temperature
[22]. Adsorption kinetics describes the change in the adsorb-
ate concentration in solution with respect to time at constant
initial concentration [189]. Moreover, the adsorption kinetic
models explain the adsorption mechanism. In this section
various isotherms and kinetic models of interest will be
discussed.
5.1 Adsorption isotherms
There are various isotherms available that describe adsorp-
tion [12]. However, the most frequently encountered iso-
therms that describe the adsorption of heavy metals from
aqueous solutions are Freundlich isotherm, Langmuir iso-
therm and Redlich–Peterson isotherm.
5.1.1 Freundlich isotherm
Freundlich adsorption isotherm is an empirical relation that
relates the concentration of a solute on the surface of an
adsorbent and the concentration of the solute in the liquid
with which it is in contact. Freundlich isotherm is the most
important isotherm dealing with multilayer sorption sites
and heterogeneousorption energies [158, 222].Freundlich
isotherm can be expressed in non-linear and linear forms
(Eq. 1):
( ) 1
1∕n
(1)
( )
q = Kf Ceq or Log(q) = log Kf + Log Ceq ,
n
13

38 

Table 1  Summary of the adsorption of heavy metals on carbon nanotubes (where m is the adsorbent dosage (mg L−1), Co is the initial concentration of adsorbate (mg L−1), PFO and PSO are
pseudo first and second order kinetic models respectively)
Adsorbate Adsorbent Calculated adsorp- Conditions Best conditions Best fitting isotherm/kinetic References

13
tion capacity (mg. model
­g−1)
Page 12 of 33

Hg(II) MWCNTs 87.72 27 °C, m range 150–1450, pH pH 6.5–7.5 Freundlich/(PSO) [200]

6.7, Co = 50
3-aminopyrazole functional- 112.360 25 °C, m = 400, pH 7.7, pH 7.7 Langmuir/(PSO) [5]
ized MWCNTs Co range 50–150
MWCNTs 25.641 25 °C, Co = (0.1, 1, 10) pH 7 Freundlich/(PSO) [239]
OH-MWCNTs 120.1 ­(Co = 4) Room temperature, m range pH 4.3, C
­ l− ions concentration Langmuir/(PSO) [32]
0.431 ­(Co = 0.02) 20–500, pH 4.3 not exceeding 0.01 M
COOH-MWCNTs 127.6 ­(Co = 4)
0.507 ­(Co = 0.02)
Sulfur functionalized 0.0728 pH 12.15, m = 5000 (varying pH 14, higher sulfur content Freundlich/(NA) [170]
MWCNT (S-MWCNTs) sulfur content), Co = 100 ppb
SWCNTs 40.16 ± 1.07 25 °C, m = 250, pH 5, Co NA Langmuir/(NA) [15]
Thiol functionalized SWCNT 131.58 ± 4.73 range 10–80 pH 9 Langmuir/(PFO)
(SWCNTs-SH)
MWCNTs 5.479 Room temperature, pH 5–8 Freundlich/(Weber–Morris) [70]
Oxidized MWCNTs 27.32 m = 1000, pH 6 pH 6–8 Freundlich/(PSO)
(O-MWCNTs) Co range 10–120
Iodide functionalized MWC- 123.45 pH 6–8 Langmuir/(PSO)-Weber–Mor-
NTs ris
S-MWCNTs 151.51 pH 6–8
MWCNTs 71.1 ± 7.3 20 °C, m = 500, pH 7, pH 4–5 Dubinin-Radushkevich/(PSO) [250]
OH-MWCNTs 78.9 ± 4.7 Co range 0.01–0.5 pH 4–6
COOH-MWCNTs 134 ± 20 pH 9
NH2-MWCNTs 205 ± 10 pH 4–9 Freundlich/(PSO)
Chitosan–COOH-MWCNTs 181.8 25 °C, m = 400, pH 4, pH 5 Frendlich/(NA) [201]
nano composite Co range 0.05–1.6
M. Bassyouni et al.
 Table 1  (continued)
Adsorbate Adsorbent Calculated adsorp- Conditions Best conditions Best fitting isotherm/kinetic References
tion capacity (mg. model
­g−1)

Zn (II) Purified SWCNTs 46.94 45 °C, m = 500, pH 7, Co NA Langmuir/(PSO) [129]

range (10-80)
Purified MWCNTs 34.36
Purified SWCNTs 43.66 25 °C, m = 500, pH 7, Co pH 8–11 Langmuir/(NA) [128]
range (10–80)
Purified MWCNTs 32.68
MWCNTs 156.25 25 °C, m range (400–20,000), pH 5 Freundlich/(NA) [152]
pH 4.5, Co = 100
MWCNTs modified with NA pH 7, m = 12,500, pH 7 (nearly 100% removal) NA [106]
8-hydroxyquinoline time = 2 h,
Co range (0.5–10) removal
(100–50.71%)
Raw CNTs 250 m = 600, pH 7, Co range NA Langmuir/(PSO) [190]
(3–250)
MWCNTs modified with 500
5,7-dinitro-8-
quinolinol
MWCNTs 90.9 m range (200–600), pH 8–12, pH 10 Langmuir/(PSO) [156]
Co = 10
oxidized CNTs 74.6268 25 °C, m = 2000, pH 7, NA Freundlich/(Weber-Morris) [218]
Co range (100–1200)
oxidized CNTs 0.0152 mmol/g 25 °C, m = 1500, pH 4.5, NA Langmuir/(NA) [65]
Co range (1–5)
Utilization of carbon nanotubes in removal of heavy metals from wastewater: a review of the CNTs’…

Functionalized CNTs 1.05 50 °C, m range (300–900), pH 10, m = 900 Freundlich/(PSO) [154]
Co = 1.1, pH 3–10
MWCNTs 10.21 25 °C, m = 500, pH 7 NA Freundlich/(PSO) [131]
Co range (10–80)
O-MWCNTs ­(HNO3 + H2SO4) 18.14 Langmuir/(PSO)
(3:1)
O-MWCNTs ­(HNO3) 27.2
O-MWCNTs ­(KMnO4) 28.01
O-MWCNTs (NaClO) 32.68

13
Page 13 of 33  38


Table 1  (continued)
38 

Adsorbate Adsorbent Calculated adsorp- Conditions Best conditions Best fitting isotherm/kinetic References
tion capacity (mg. model

13
­g−1)
Page 14 of 33

Cr(VI) Magnetic 13.158 30 °C, pH = 3, Co range pH 3 Langmuir [85]

MWCNTs (0.78–25)
superparamagnetic MWCNTs 14.28 20 °C, pH 5, Co range (5–25) pH 1 Langmuir/(PSO)- Weber– [19]
Morris
MWCNTs 2.679 20 °C, m = 1000, pH pH 2.05 Langmuir [84]
2.88 ± 0.02, Co range (NA)
nanoscale zero-valent ironpar- NA NA pH 5 (nearly 100% removal), NA/(PFO) [133]
ticles supported on MWC- ZVI:MWCNT ratio of 1:20
NTs (ZVI-MWCTs) (very fast kinetics)
functionalized 6.33 298 K, m range (20–60), pH 3 Langmuir [83]
MWCNTs pH = 3, Co = 5
magnetic CNTs 65.96 60 °C, m = 1000 pH = 6, Co pH 2 Langmuir/(PSO) (R. Chen et al. 2013)
nanoparticles range (100–800)
functionalized carbon nano- 2.517 50 °C, m = 100 mg, varying pH 9 Langmuir/(NA) [155]
tubes pH (5,7,9) Co = 1
non-functionalized carbon 2.49
nanotubes
Chitosan-coated CNTs nano- 146.5 m = 500, pH = 3, Co range NA Langmuir/(NA) [77]
composite (20–400)
As (III) 3-aminopyrazole functional- 133.33 25 °C, m = 400, pH 7.9, pH 7.88, m = 19.69 mg, Langmuir/(PSO) [5]
ized MWCNTs Co range (50–150) ­Co = 20.34
Iron oxide coated MWCNT 1.723 m range (1–10), pH 4, Co = 0.1 pH 5 Freundlich/(PSO) [161]
(Fe-MWCNTs)
Magnetite decorated MWC- 53.1525 Co range (0.2–0.4) NA Freunlich- Langmuir/Elovich [147]
NTs ­(Fe3O4-MWCNTs)
electrode
MWCNTs- zirconia nanohy- 2 m range (1000–10,000), pH 6, pH 5–8 Langmuir/(PSO) [162]
brid Co = 0.1
Surfactant assisted 28.74 25 °C, m = 200, pH 7.5, pH 8 Langmuir/(PSO) [15]
Ce–Fe mixed oxide decorated Co range (1–20)
MWCNTs
Fe- MWNCTs 4 Room temp., m = 200, pH 8, pH 8 Langmuir/(PSO) [215]
Co range (NA)
Zerovalent iron- doped 111.1 ± 4.8 m = 2500, pH 7, ­Co range pH 7 Langmuir/Weber–Morris [194]
MWCNTs in the presence of (0.1–1200)
EDTA
M. Bassyouni et al.
 Table 1  (continued)
Adsorbate Adsorbent Calculated adsorp- Conditions Best conditions Best fitting isotherm/kinetic References
tion capacity (mg. model
­g−1)

As (V) Iron oxide coated MWCNTs 0.189 m range (1–10), pH 4, pH 4 Freundlich/(PSO) [161]
(Fe-MWCNTs) Co = 0.1
Magnetite decorated MWC- 39.0868 Co range (0.2–0.4) NA Freunlich-Langmuir/Elovich [147]
NTs ­(Fe3O4-MWCNTs)
electrode
MWCNTs- zirconia nanohy- 5 m range (1000–10,000), pH 6, pH 6 Freundlich/(PSO) [162]
brid Co = 0.1
Fe2+/Fe3+ coated-ethylen- 24.69/14.45 45 °C, m = 100, pH 4, pH 3–5 Freundlich/(PSO) [222]
ediamine functionalized Co range (0.05–4)
MWCNTs
Surfactant assisted 30.96 25 °C, m = 200, pH 7.9, Co pH 3 Freundlich/(PSO) [15]
Ce–Fe mixed oxide decorated range (1–20)
MWCNTs
Zerovalent iron- doped 166.66 ± 5.8 m = 2500, pH 7, ­Co range pH 7 Langmuir/Weber–Morris [194]
MWCNTs in the presence of (0.1–1200)
EDTA
MWCNTs 32.68 Room temperature, m = 1000, pH 3 Langmuir/(PSO) [137]
Co range (10–100)
Ceria modified CNTs 78.8 m = 500, pH 3.1, ­Ca2+, ­Mg2+ pH 3 Freundlich/NA [167]
­(CeO2-CNTs) ions conc. of 10 mg.L−1, Co
range (NA)
Utilization of carbon nanotubes in removal of heavy metals from wastewater: a review of the CNTs’…

13
Page 15 of 33  38


Table 1  (continued)
38 

Adsorbate Adsorbent Calculated adsorp- Conditions Best conditions Best fitting isotherm/kinetic References
tion capacity (mg. model

13
­g−1)
Page 16 of 33

Pb(II) Nitrogen-doped multiwall 0.083 mmol/g 25 °C, m = 1000, pH 4 pH 5 Langmuir/NA [169]

carbon nanotubes Co range (0.1–0.7 mM)
Magnetic MWCNTs func- 150 m = 25 mg, pH 6.4, NA Langmuir/(PFO) [213]
tionalized with 3-choloro- Co range (0.1–25)
propyltriethoxy-silane and
8-aminoquinline
MWCNTs 97.08 Room temperature, m = 500, pH 5 Langmuir/NA [118]
Co range 10–60, pH 5
Acid-refluxed CNTs 17.44 Room temperature, m = 500, NA Langmuir/NA [117]
pH 5,
Co range (2–14)
COOH-MWCNTs 6.6 25 °C, pH 6, m range pH 7 Freundlich/(PSO) [8]
(10–160 mg),
Co = 0.01
O2-plasma oxidized MWCNTs 35.08 ± 1.69 20 °C, m = 1500, pH 5 pH 7–9 Langmuir/(PSO) [247]
O-MWCNTs 2.06 20 °C, pH 5.9 ± 0.1, m = 1000 pH 6 Freundlich/(PSO) [237]
MnO2-MWCNTs composite NA m = 10 mg, Co = 20 ppm, pH 7, flow rate 1 ml/min. NA [191]
(packed column) pH = 5.5 (95% removal efficiency)
flow rate 1–7 ml/min
NiO2–MWCNTs nano com- 24.63 m = 2000, Co range (20–100) pH 7, Co = 20 Freundlich/(PSO) [50]
posite
Tris (2-aminoethyl) amine 71 m = 1000, pH 6.7–7, pH 6.5 Freundlich/(NA) [46]
functionalized MWCNTs Co range (2–80)
diiodocarbene modified 82.73 25 °C, m = 250, pH 5, pH 5.32–5.7 Langmuir/(PSO) (Jia-Ying [241])
O-MWCNTs Co range (10–100)
O-MWCNTs 100 30 °C, m = 200, Co range pH 6 Langmuir/(PSO) [175]
(10–60)
CNTs 102.04 25 °C pH 5, m = 40 Langmuir/(PSO) [96]
M. Bassyouni et al.
 Table 1  (continued)
Adsorbate Adsorbent Calculated adsorp- Conditions Best conditions Best fitting isotherm/kinetic References
tion capacity (mg. model
­g−1)

Cd (II) Nitrogen-doped MWCNTs 8.99 25 °C, m = 1000, pH 5, pH 7 Freundlich/NA [169]

Co range (0.1–0.7) mM
Magnetic MWCNTs func- 201 m = 25 mg, pH 6.4, NA Langmuir/PSO [213]
tionalized with 3-choloro- Co range (0.1–25)
propyltriethoxy-silane and
8-aminoquinline
MWCNTs 10.86 room temperature, NA Langmuir/NA [118]
m = 500, pH 5
Co range (2–15)
Raw CNTs 11.51 30 °C, m = 1600, NA Langmuir/PSO [3]
Co (10–300)
Modified (CNTs-HNO3) 26.88
As-grown CNTs 1.1 25 °C, m = 500, pH 5.5 m = 2000 at pH 5.5 NA [119]
Co range (1.18–9.50)
H2O2 oxidized CNTs 2.6
HNO3oxidized CNTs 5.1 pH 6
KMnO4 oxidized CNTs 11 m range 300–800
Pure CNTs 14.45 30 °C, m = 500, pH 6.0 ± 0.1, NA Langmuir/PSO [212]
Co range (10–60)
Acid-oxidized MWCNTs 101 m = 500, ­Co range (NA) NA Freundlich [60]
Raw MWCNTs 1.26 ± 0.02 25 °C, m = 100, pH 8, Co (0.1, NA Langmuir/PSO [224]
0.5, 1, 3 and 5)
Oxidized -MWCNTs 22.39 ± 0.36 pH range(6–10)
Utilization of carbon nanotubes in removal of heavy metals from wastewater: a review of the CNTs’…

Ethylene diamine-functional- 21.67 ± 0.40 pH range (8–9)

ized MWCNTs
Silver-doped MWCNTs (Ag- 58.02 40 °C, m = 50 mg, pH6, pH 7.0, m = 50 mg Langmuir/PSO [177]
MWCNTs) Co range (10–100)

13
Page 17 of 33  38


Table 1  (continued)
38 

Adsorbate Adsorbent Calculated adsorp- Conditions Best conditions Best fitting isotherm/kinetic References
tion capacity (mg. model

13
­g−1)
Page 18 of 33

Cu (II) Acid-refluxed MWCNTs 28.49 Room temperature, m = 500, pH 5 Langmuir/NA [118]

pH 5,
Co range 5–30
Oxidized MWCNTs 200 m = 2000, pH 6, ­Co range pH 6 Langmuir/(PSO) (Sobhanardakaniet al. 2015)
50–400
Raw MWCNTs 142.8 m = 600, pH 7, ­Co range pH 7 Langmuir/(PSO) [190]
(3–250)
MWCNTs modified with 333.3
5,7-dinitro-8-quinolinol
Silver-doped MWCNTs (Ag- 58.02 40 °C, m = 50 mg, pH 6 pH 6 Langmuir/(PSO) [177]
MWCNT) Co range 10–100
Oxidized SWCNTs with the 166.67 25 °C, pH 5, pH 10 Freundlich,langmuir/(PSO), [18]
aid of ultrasonication (US- Co range 5–40 Elovich
SWCNTs)
US-MWCNTs 43.86 Langmuir/(PSO)
Oxidized SWCNTs with the 250 Freundlich-langmuir/(PSO)
aid of UV light (UV-SWC-
NTs)
UV-MWCNTs 142.86 Freundlich/(PSO)
S-MWCNTs 7.4 m = 5 mg, Co range 0.154– pH 9 Langmuir/(PSO) [97]
0.006
MWCNTs 12.34 20 °C, m = 800 mg/L, Co range NA Langmuir/(PSO) [149]
10–30
Iminodiacetic acid functional- 6.64 m = 400, pH 8, ­Co range NA Langmuir/(PSO) [226]
ized MWCNTs (1.2–6.0)
Chitosan-MWCNTs composite 454.55 m = 50 mg, pH 5.5, Co range NA Langmuir/(PSO) [171]
(50–250)
Purified MWCNTs 37.5 25 °C, m = 500, pH 5, pH 6 Freundlich/(NA) [66]
Co range (10–100)
Sulfonated MWCNTs 59.6
M. Bassyouni et al.
 Table 1  (continued)
Adsorbate Adsorbent Calculated adsorp- Conditions Best conditions Best fitting isotherm/kinetic References
tion capacity (mg. model
­g−1)

Ni (II) SWCNTs (NaOCl) 47.85 25 °C, m = 500, pH 7, NA Langmuir/(PSO) [130]

Co range (10-80)
MWCNTs (NaOCl) 38.46
O-MWCNTs 9.43 30 °C, m = 750, pH pH 8 Langmuir/(PSO) [29]
6.55 ± 0.02,
Co range (2–20)
O-MWCNTs 6.346*10−5 mol/g 20 ± 2 °C, m = 800, pH pH 7 Langmuir/(PSO) [243]
5.4 ± 0.1, 0.01 M NaClO4,
Co range (NA)
Polyacrylic acid functionalized 6.615*10−5 mol/g 20 ± 2 °C, m = 800, pH
O-MWCNTs 5.4 ± 0.1, 0.01 M NaClO4,
Co range (NA), C[PAA] = 10
MWCNTs 6.09 25 °C, pH 7, pH 8 Langmuir/(PSO) [1]
Co range (5–100)
O-MWCNTs 17.86 25 °C, pH 6.5 NA Langmuir/(PSO) [148]
Co = (10–30)
Oxidized CNTs 49.261 25 °C, m = 400, pH 6, Co pH 6 Freundlich/(NA) [101]
range(0–200)
Iron oxide-MWCNTs com- 9.18 25 ± 2 °C, m = 750, pH 8 Langmuir/(NA) [30]
posite pH = 6.4 ± 0.2,
Co range (NA)
O-CNTs 50.09 20 °C, m = 1000, pH 7, pH 6 Langmuir/(PSO) [178]
Utilization of carbon nanotubes in removal of heavy metals from wastewater: a review of the CNTs’…

Co range (10–80)
Magnetic MWCNTs 2.11 30 °C, Co range (0.82–4.12) pH 9.4 Langmuir/(PSO) [105]
Co (II) MWCNTs- iron oxide com- 0.15 mmol/g 20 °C, m = 500, pH = 6.4 ± 0.1, pH 10–12 Langmuir/(PSO) [227]
posite 0.01 M ­NaNO3, Co range
(NA)
Sulfonated magnetic MWC- 8.42 25 °C, m = 300, pH 6 ± 0.1, pH < 10 Langmuir/(PSO) [244]
NTs 0.01 M NaCl,
Co range 0.5–20
Poly(acrylic acid) grafted 1.49*10−4 mol/g 30 °C, m = 1000, pH 6.8 ± 0.1, pH 8.5–11 Langmuir-D–R/(PSO) [31]
MWCNTs 0.01 M ­NaClO4, Co range
(NA)
MWNCTs-hydroxyapatite 16.26 20 °C, m = 600, pH 6 ± 0.1, pH 8 Langmuir/(PSO) [126]
0.01 M NaCl, Co range (NA)

13
Page 19 of 33  38
38 
Page 20 of 33 M. Bassyouni et al.

Table 2  Adsorption of heavy metals on activated carbon and other adsorbents

Adsorbate Adsorbent Calculated adsorp- Conditions Best Conditions Best fitting isotherm/ References
tion capacity kinetic model
(mg g−1)

Hg(II) Activated carbon (AC) 25.88 30 °C, Co range pH 6 Freundlich/(PSO) [179]

prepared from Ceiba (10–140), pH 2–9
pentandra hulls
(AC) From Phaseolus 23.66 pH 7
aureus hulls
(AC) from Cicer arieti- 22.88
num waste
(AC) from mango 12.626 30 °C, m = 3000, pH 10 Freundlich/PSO [209]
kernel pH 6.5, Co range
(10–100),
(AC) 472 45 °C, m = 1000, Ph 7, NA Langmuir/(PSO) [6]
(AC) modified with 444 Co range (50–800) Freundlich/(PSO)
dimethyl disulfide (poor fitting to lang-
(AC) modified with 563 muir model)
Sulfur
(AC) modified with 496
­SO2
(AC) from Eichhornia- 28.4 30 °C, m range pH 5-10 Langmuir- Freundlich/ [98]
crassipes (200–1200), pH 5, (PFO-PSO)
Co = 20
Adulsa leaves powder 107.5 30 °C, m = 10000, pH pH 6 Langmuir/PSO [7]
6, Co range (25–100)
Cellulose modified 90.59 pH 5, Co range pH 5 Langmuir/(PSO) [138]
with dimethyl benzal (20–100)
aniline
Sheep bone charcoal 12.55 25 °C, m = 4000, pH 2, pH 3 Freundlich/(NA) [45]
Co range (NA)
Zn (II) Natural clay 80.64 23 °C, m range pH 8 Langmuir/(PSO) [221]
(0.1–0.9), pH 8,
Co = 20
Powdered Fish Bones NA T = 303 K, m range pH 5 NA/(PSO) [121]
(1–1.8),
pH 5, Co = 20
Natural bentonite 21.097 20 °C, pH 5, Co = 15 pH 5 Langmuir/(NA) [108]
Mango leaves powder NA 22 °C, m range (2–20), pH4 Langmuir, Freundli- [102]
pH 4 chand Temkin
Natural Maghnite 39.06 25 °C, pH 9 pH 9 Langmuir/(PSO) [249]
Modified by 3-Ami-
nopropyltri-ethox-
ysilane
Cr(VI) Activated carbon 3.46 pH 3, Co range (5–20) NA Langmuir/(NA) [196]
Sulfuric acid-func- 25.6 m = 250 mg, pH 1.5 pH 1.5 Langmuir/(PFO) [10]
tionalized (AC) from
olive stones
Acid treated commer- 71.4
cial (AC)
Zirconia-impregnated 0.53 mmol/g 30 °C, m = 100 mg, pH 6–9 Langmuir/(PSO) [120]
collagen fibers pH 7
Chitosan beads 76.92 m = 2000 mg, pH 3 pH 3 Langmuir/(NA) [159]

13
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Table 2  (continued)
Adsorbate Adsorbent Calculated adsorp- Conditions Best Conditions Best fitting isotherm/ References
tion capacity kinetic model
(mg g−1)

As (III) Nano zero-valent iron 18.19 25 °C, m range pH 6 Langmuir/(Boyd) [257]

supported on (AC) (500–6000)
pH 6.5, Co = 2
Magnetite 7.962 22 °C, m = 400, pH pH 2 Langmuir/(NA) [36]
6.5,
Co range (0.7–3)
Iron-modified (AC) 38.8 20 °C, m range NA Langmuir/(parabolic [34]
(100–20,000), diffusion equation)
pH 6, Co = 20–22
Cupric oxide nanopar- 26.9 Room temperature, pH 9.3 Langmuir/(NA) [143]
ticles m = 2000,
pH 8 ± 0.1, Co range
(0.1–100)
As (V) Surfactant–modified 0.0743 25 °C, m = 5000, pH 7, pH 7 Langmuir/(NA) [144]
zeolite Co range (0.02–0.4)
Nano zero-valent iron 12.02 25 °C, m range pH 3 Langmuir/(Boyd) [84]
supported on (AC) (500–6000)
pH 6.5, Co = 2
Iron-oxide-coated 0.36 25 ± 2 °C, m range NA Langmuir/(Second [141]
natural rock (1000–15000) order rate model)
pH 7.5, Co = 0.04
Magnetite 8.8 22 °C, m = 400, pH pH 2 Langmuir/(NA) [36]
6.5,
Co range (0.7–3)
Iron-modified (AC) 51.3 20 °C, m range NA Langmuir/(parabolic [34]
(100–20000), diffusion equation)
pH 6, Co = 20–22
Cupric oxide nanopar- 22.6 Room temperature, pH 6–7 Langmuir/(NA) [143]
ticles m = 2000,
pH 8 ± 0.1, Co range
(0.1–100)
Iron-impregnated 1.66 25 °C, m = 2857, pH pH 7, iron con- Langmuir/(NA) [26]
granular (AC) 6.81 ± 0.03, tent = 4.22%
iron content = 12.13%
Co range (0.05–5)
Pb(II) Activated carbon fibers 45.5 288 K, m = 7500, 308 K, pH 4 at Langmuir/(NA) [115]
pH 4, equilibrium
Co range (60–450) conc. = 50 mg/l
Activated carbon 40.984 Room temperature, NA Langmuir/(NA) [153]
from watermelon m = 1000, pH 4.5, Co
shell(GACW) range (10–500)
Activated carbon from 32.362
walnut shell (GACN)
Copper oxide oval 125 Room temperature, pH 6.5, 4 h Langmuir/(PSO) [59]
nanostructure Co range(100–300)
Activated alumina 83.33 30 °C, m = 7500, pH 5, m = 7500, pH 5 Freundlich/(PSO) [157]
Co range (3–300)
Titanate nanotubes 520.83 20 ± 0.2 °C, m = 200, pH range (5.0–6.0) Langmuir/(PSO) [236]
Co range(20–100),
Few-layered graphene 842 293 K, m = 100, pH NA Langmuir/(NA) [72]
oxide nanosheets 6.0,
Co range (NA)

13
38 
Page 22 of 33 M. Bassyouni et al.

Table 2  (continued)
Adsorbate Adsorbent Calculated adsorp- Conditions Best Conditions Best fitting isotherm/ References
tion capacity kinetic model
(mg g−1)

Cd (II) Activated alumina 35.06 30 °C, m =7500, pH 5, m = 7500, pH 5 Langmuir/(PSO) [157]

Co range (3–300)
Titanate nanotubes 238.61 20 ± 0.2 °C, m = 200, pH 5–6 Langmuir/(PSO) [236]
Co range(20–100)
Citrus maxima peel 135.185 25 °C, m = 4000, pH pH 5–6 Langmuir/(NA) [27]
5.0 ± 0.1
Passion fruit shell 23.226
Sugarcane bagasse 86.747
Activated carbon 0.079 (mmol g−1) 20 °C, m = 5000, pH 293 K, pH 6.8 ± 0.3 Freundlich/(NA) [58]
6.8 ± 0.3,
Co range (0–50)
Activated carbon from 1.851 20 °C, m range NA Langmuir/(PSO) [109]
olive stone (2500–30,000)
Activated carbon 7.47 × 10−6 mol/g 20 °C, m range m = 60,000, pH range Freundlich-Langmuir/ [216]
(12,000–40,000) (5–8) (NA)
Cu (II) Granular activated car- 7.03 30 °C, m = 100,000, pH 4.5 Langmuir/(PSO) [61]
bon in the presence pH 4.5
of competitor ions
like (Ag, Mn)
Activated carbon/chi- 74.35 20 °C, m = 0.3, pH = 7 NA Langmuir/(NA) [124]
tosan composite
Activated carbon 6.14 × 10−5 mol/g 20 °C, m = 10,000, pH 5–8 Langmuir-Freundlich/ [216]
pH 5–8 (NA)
Powdered activated 5.98 pH 6, Co range pH 6 Langmuir/(NA) [123]
carbon impregnated (988–3870)
with humic acid
Brown macroalgae 1.44 × 10−3 mol g−1 m = 50 mg, pH = 5, pH 5 Dubinin–Radushk- [37]
Co = 1.34*10−3 mol. evish/(NA)
g−1
Mesoporous anatase 12.8 ± 0.6 25 °C, m = 2500, Ph 6, pH 6 Langmuir/(PSO) [223]
nanofibers (m-TiO2- Co range (5–35)
NFs)
(TiO2-NFs) 6.9 ± 0.3
Bentonite 12.547 20 °C, pH 7, Co range NA Langmuir/(NA) [108]
(20–70)

13
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Table 2  (continued)
Adsorbate Adsorbent Calculated adsorp- Conditions Best Conditions Best fitting isotherm/ References
tion capacity kinetic model
(mg g−1)

Ni (II) Raw doum-palm seed 3.24 25 °C, pH 7, Co range pH 7, m = 10,000 Freundlich/(PSO) [54]
(10–40)
(AC) from doum palm 4.93
seed prepared by
physical activation
(AC) from doum palm 13.51
seed prepared by
physical activation
and chemical treat-
ment
(AC) treated with 28.25 25 ± 2 °C, m = 2000, pH 5, Co = 300 Langmuir/(NA) [202]
­H2SO4 Co range (25-300)
Activated carbon 69.49
treated with H
­ 2SO4
and ­HNO3
Granular (AC) 7.65697 m = 12500, Co range pH 6, Co = 10  Langmuir/(NA) [112]
(10-50) m = 25000
Bulk ­TiO2 63.82 μmol/g 25 °C, m range pH 8 Langmuir/(PSO) [55]
(10–500), pH 8,
Nano ­TiO2 114.94 μmol/g Co = 500
Activated carbon 30.769 20 °C, m = 5000, pH 5, pH 5, Co = 25  Langmuir/(NA) [78]
Co range (25–250) m = 5000
AC Treated with 37.175
­H2SO4
Commercial (AC) 0.0034 (mol/L) 25 °C, m = 1000, pH NA Langmuir/(NA) [168]
4–5, Co = (0–0.07)
Acid-precipitated basic 0.0091 (mol/L) mmol/L
lignin
Bentonite 21.39 25 °C, m = 50000, pH pH 6, m = 70000 Freundlich/(PSO) [188]
5.5,
Co range (100–2000)
ZnO-Gr 66.66 25 °C pH 8.2 Langmuir [74]
Co (II) Activated carbon 26.525 60 °C, pH 6.5, Co = 5 pH 6.5 Freundlich –Lang- [172]
muir/(PFO)
(AC) Prepared from 13.88 30 °C, m range pH 6 Langmuir/(PSO) [47]
Hazelnut Shells (1.18–3.2), Ph 6,
Co = 13.3
Nanosized TiO2 2.64 × 10−4 (mol/g) 65 °C, pH 6 pH 6 Langmuir/(PSO) [229]
powder
Bentonite 16.863 20 °C, pH 9, Co range pH 9 Langmuir/(NA) [108]
(20–70)
Mesoporous silica 35.7 25 °C, m = 1000, pH 6, pH 7 Redlich–Peterson/ [186]
(SBA-15) Co range (100–500) (NA)
Modified Mesoporous 51.6
silica (SBA-15-NH2)
(AC) from coconut 29.68
shell
Fe3O4/Bentonite 18.76 pH 8, Co = 800 pH 8 Langmuir/PSO [79]
Nanocomposite

13
38 
Page 24 of 33
where q is the amount of adsorbate adsorbed per unit mass
of the adsorbent at equilibrium (mg g−1)Ceq is the adsorb-
ate concentration at equilibrium (mg L−1)Kf is the equal to
the adsorption capacity at equilibrium concentration = 1.
Higher values of Kf indicate that a high amount of adsorb-
ate is adsorbed [222]. (1/n) is an exponent that represents
the extent of change of q with equilibrium concentration; n
should have a value ranging between 1 and 10 [176]. Lower
values of n indicate more favorable adsorption.
5.2 Langmuir isotherm
Langmuir isotherm is the most frequently used isotherm
to describe heavy metals adsorption. It describes quan-
titatively the formation of a monolayer of adsorbate on
the outer surface of an adsorbent [41]. After monolayer
formation, no further adsorption takes place. Langmuir
isotherm is based on three main assumptions:
• The adsorption active sites are identical
• The energies of adsorption on the surface are uniform
• No transmigration of adsorbate molecules occurs on
the adsorbent surface
Based on the previous assumptions, Langmuir iso-
therm is expressed in non-linear and linear forms (Eq. 2):
qm KL Ceq Ceq Ceq
1
q= or = + , (2)
1 + KL Ceq q qm KL qm
where q and Ceq have the same designations as in Freundlich
isothermqm is the maximum adsorption capacity related
to monolayer coverageKL is Langmuir isotherm constant
related to the energy of adsorption [222]. Gibbs free energy
can be calculated using the value of KL (Eq. 3):
(3)
( )
ΔG◦ = −RT ln KL ,
where R is the universal gas constant (8.314 J/mol k) and T
is the absolute temperature in Kelvin.
Another Important parameter that can be calculated
from Langmuir constant (KL) is the dimensionless separa-
tion factor RL, which defines the favorability and nature
of adsorption (Eq. 4):
1
RL = , (4)
1 + CO KL
where CO is the initial concentration of adsorbate, if RL > 1
the adsorption is unfavorable, linear if RL = 1, favorable if
0 < RL < 1 and if RL = 0 the adsorption is irreversible [82,
256].
13
M. Bassyouni et al.
5.3 Redlich–Peterson isotherm
The Redlich–Peterson (R–P) isotherm model is a hybrid
isotherm [182]. It combines both Langmuir and Freundlich
isotherms [68, 165]. The isotherm is expressed mathemati-
cally as:
KR Ceq
q= , (5)
𝛽
1 + aR Ceq
where K R : Redlich–Peterson isother m constant
(L/g).a R: Redlich–Peterson isotherm constant (1/mg).
β: Redlich–Peterson isotherm exponent. (R–P) isotherm
approaches the Freundlich model at high concentration
(as the exponent β tends to zero [95] and is in accord with
the low concentration limit of the Langmuir equation [68,
104, 165] (as the β values are all close to one [95]. The
isotherm is valid over a wide range of concentration and
can be applied for both homogeneous and heterogeneous
systems [67].
5.4 Adsorption kinetics
Adsorption is a mass transfer phenomenon that includes the
diffusion of an adsorbate onto the surface of an adsorbent.
Diffusion can be external (from the bulk of the solution into
the surface of the adsorbent), internal (from the adsorbent
surface into the pores) or surface diffusion [69, 81]. Kinetic
models can predict whether the rate controlling step of the
adsorption process is a diffusion mechanism or a chemi-
cal interaction between the adsorbate and the adsorbent.
There are various kinetic models available that describe the
dynamics of adsorption process. However, in this section
only the two most encountered kinetic models (second order
kinetics and intra-particle diffusion model) are discussed.
5.4.1 Intra‑particle diffusion model
This model is applied to test if the rate limiting step of the
overall adsorption process is an intra-particle diffusion
mechanism. If this is the case, the adsorption can be con-
trolled by surface diffusion or by diffusion into the pores or
by both of the mechanisms [87]. The model is mathemati-
cally expressed as:
qt = Ki t1∕2 , (6)
and
qt = Ki t1∕2 + C, (7)
where qt is the amount of adsorbate adsorbed per unit
mass of the adsorbent (mg g−1), at any time (t) within the
Utilization of carbon nanotubes in removal of heavy metals from wastewater: a review of the CNTs’…
boundaries (t = 0 and t = tequilibrium). T is the time at which
each ­qt is measured Ki is the intra-particle diffusion rate con-
stant (mg g−1 min−0.5). C is the intercept of the line, which
is related to the thickness of the boundary layer.
By plotting qt against t1/2, the result can be a single linear
relation or two linear relations. In case of a single relation;
this represents surface diffusion of adsorbate particles, occu-
pying the most readily available active site on the adsorbent
surface (Eq. 6). If this linear relation does not pass through
the origin, this is an indication that other mechanisms
(besides the intra-particle mechanism) are rate-limiting.
The second linear relation (Eq. 7) represents the diffusion
of adsorbate particles into the pores of the adsorbate, and the
intercept (C) represents external diffusion [35].
5.4.2 Pseudo second‑order model
In this model, the mechanism that controls adsorption is
the chemisorption process, through which the removal from
a solution is due to physicochemical interactions between
the two phases (Wang et al. [225, 228]. The interactions
(chemical bonding) involve sharing or exchange of electrons
between the adsorbate and the adsorbent [180]. The linear
form of pseudo second order equation is expressed as Eq. 8
[23]
t 1 1
= 2
+ t,
qt k2 qe qe
whereqt and t have the same designations as in the previous
model. k2 is the equilibrium rate constant of pseudo sec-
ond-order adsorption (g mg−1 ­min−1). Qe are the amounts
of adsorbate adsorbed at equilibrium at the specified experi-
mental conditions (mg g−1).
Table 3  Regeneration behavior of CNTs versus activated carbon for nickel and zinc metal ions
Adsorbent Metal ion Regeneration method Ion recoveries of sorbents Capacity before
under various n (1–10) (%) and after 10 cycles
MWCNTs Ni2+ HNO3 solution (reduce pH) 100–76
SWCNTs 100–78
GAC​ 100–13
SWCNTs Zn2+ HNO3 solution (reduce pH) 100–80
MWCNTs 100–77
PAC 100–13
Page 25 of 33  38
6 Desorption and regeneration of CNTs
Regenerating and reusing an adsorbent are crucial factors to
evaluate the availability of the process implementation. The
recycle efficiency of an adsorbent as well as its adsorption
capacity must be considered when estimating the cost of the
process. The regeneration efficiency of CNTs is compared
with that of the commonly used adsorbent (i.e., activated
carbon) for a couple of heavy metals (zinc and nickel) and
the results are introduced in Table 3. The estimated number
of cycles shown in the Table 3 are obtained by linear curve
fitting method which offers a degree of error, yet provides a
good approximation of the actual behavior. It is obvious that
CNTs are much more durable than activated carbon (AC) in
terms of regeneration effectiveness. AC is more soluble in
aqueous solutions than CNTs, which explains the difference
in weight loss of the two adsorbents. Therefore, in spite of
the higher capital cost of the nanotubes, they are advanta-
geous in capacity and durability, which lowers the operating
cost and reduces the environmental impact of the CNTs.
7 Present challenges for incorporation
of CNTs into the industrial wastewater
applications
(8) In the previous sections, the favorability of CNTs over
many other adsorbents was established. However, in order
to apply CNTs in real life, wastewater treatment applica-
tions some challenges and drawbacks must be overcome.
The main and most commonly addressed challenge is the
cost of the nanotubes. Currently, CNTs are manufactured in
relatively large amounts by the chemical vapor deposition
process [173]; and CNTs at a price as low as $10/kg were
available [42]. However, a tradeoff is made here. Reducing
the cost of manufacturing results in reducing the quality of
the produced CNTs. Large scale production of CNTs intro-
duce more impurities on the surface of the nanotubes and it
is also very difficult to control the uniformity of the textural
Estimated number of References
cycles to lose 50% of
(mg/g) capacity
33–25 40 [130]
42–32 28
22–2.5 3
34–25 37 [129]
27-21 28
12–3 1
13
38 
Page 26 of 33
properties of the produced CNTs. Therefore, to reduce the
overall cost of CNTs, extensive research must be done on
improving the manufacturing methodologies and finding
suitable cheap feed stocks for the nanotubes production.
Another challenge is that CNTs are inherently insoluble
in water [43]. From a mass transfer perspective, the two
phases present (i.e., water and solid CNTs) must come into
intimate contact in order for the transfer of pollutants from
water to CNTs to take place efficiently by adsorption. This
challenge can be overcome by introducing polar functional
groups into the surface of the nanotubes or by non-covalent
wrapping (these methods were discussed in Sect. 2).
8 Environmental impact of carbon
nanotubes
CNTs were reported to have a toxic effect of living systems
[92, 113]. CNTs can damage the external tissue of the cell
wall. They can also readily adsorb the cellular membrane
transporting toxics into the cell [207]. Various studies
reported that CNTs can penetrate the seeds of various plants
and affect the plant’s growth [76, 103, 111, 146] and can be
transported from the plant’s root to the upper parts, reaching
the plant’s leaves. Moreover, previous studies in the litera-
ture confirmed that, in most cases, CNTs are retained in the
soil, which can promote the contamination of plants by the
nanotubes [122]. CNTs showed various toxic effects on mice
and rats which varied based on the dimensions and morphol-
ogy of the nanotubes [44]. The long, needle-like structured
MWCNTs exhibited more intense effects than other struc-
tures of the nanotubes, damaging the DNA in lung cells and
causing inflammation in cultured macrophages [187].
CNTs’ solubility in water must therefore be compro-
mised in order to achieve good separation with extremely
low dissolution in water, which also increases its replace-
ment lifetime (explained in the previous section). Moreover,
the CNTs’ traces that have passed into wastewater should
be recovered to a high extent by available techniques such
as membrane filtration and ultracentrifugation [43, 205].
Another route is converting CNTs to a safer form by biologi-
cal degradation using particular enzymes [100, 134]; Zhao
et al. [254, 255].
9 Conclusion
This work views the application of CNTs as an effective
adsorbent in wastewater treatment for removal of heavy
metals. Functionalized as well as pristine CNTs have excel-
lent properties for wastewater treatment; the large pore vol-
ume, diameter and specific surface area of the nanotubes
offer great advantage in the adsorption of heavy metals.
13
M. Bassyouni et al.
Different morphologies of CNTs modified with several tech-
niques showed a variety of adsorption capacity. Remarkable
removal of mercury (II) is achieved using CNTs at neutral
pH (6.5–7.5). The highest removal of Zn ions using CNTs
can be obtained. At low pH, H ­ + ions will compete with
2+
­Zn ions for the active sites on the CNTs’ surface. Removal
efficiency of zinc ions using MWCNTs can be enhanced
in the presence of 8-hydroxyquinoline up to 96%. Modi-
fied MWNCTs using PDDA are able to remove 100% of
Cr(VI) at pH 5.1. The optimum pH for As (III) and As (V)
adsorption is 8 and 3, respectively. Removal percentage of
lead of nearly 100% is achieved using modified CNTs at
pH 7. Dramatic decrease in lead ions removal was found at
lower pH. Significant increase in the pore volume of CNTs
can be achieved using nitric acid while H ­ 2O2, and K
­ MnO4
have no remarkable effect on pore size of CNTs. Removal
of Cu ions is sharply increased at pH1.8–6. Adsorption of
Ni (II) increased gradually from about zero to ~ 99% at pH
2–9. CNTs exhibited outstanding performance when com-
pared to other adsorbents in terms of adsorption capacity and
kinetics. CNTs are much more durable than activated carbon
(AC) in terms of regeneration effectiveness.
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