An overview of carbon nanotubes role in heavy metals removal from wastewater

doi:10.1007/s11705-018-1765-0

Front. Chem. Sci. Eng.

2019, Vol. 13

Issue (2) : 274-295 https://doi.org/10.1007/s11705-018-1765-0

REVIEW ARTICLE

An overview of carbon nanotubes role in heavy metals removal from wastewater

Leila Ouni, Ali Ramazani(

), Saeid Taghavi Fardood

Department of Chemistry, University of Zanjan, Zanjan, Iran

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Abstract

The scarcity of water, mainly in arid and semi-arid areas of the world is exerting exceptional pressure on sources and necessitates offering satisfactory water for human and different uses. Water recycle/reuse has confirmed to be successful and promising in reliable water delivery. For that reason, attention is being paid to the effective treatment of alternative resources of water (other than fresh water) which includes seawater, storm water, wastewater (e.g., dealt with sewage water), and industrial wastewater. Carbon nanotubes (CNTs) are called the technology of 21st century. Nowadays CNTs have been widely used for adsorption of heavy metals from water/wastewater due to their unique physical and chemical properties. This paper reviews some recent progress (from 2013 to 2018) in the application of CNTs for the adsorption of heavy metals in order to remove toxic pollutants from contaminated water. CNTs are expected to be a promising adsorbent in the future because of its high adsorption potential in comparison to many traditional adsorbents.

Keywords carbon nanotubes heavy metals removal water treatment

Corresponding Author(s): Ali Ramazani

Just Accepted Date: 10 July 2018 Online First Date: 18 February 2019 Issue Date: 22 May 2019

Cite this article:

Leila Ouni,Ali Ramazani,Saeid Taghavi Fardood. An overview of carbon nanotubes role in heavy metals removal from wastewater[J]. Front. Chem. Sci. Eng., 2019, 13(2): 274-295.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-018-1765-0
https://academic.hep.com.cn/fcse/EN/Y2019/V13/I2/274

Fig.1 Types of carbon nanotubes: (a) a SWCNT and (b) a MWCNT

Adsorbent	Adsorbate	Q_m /(mg?g^?¹)	Experimental conditions	Interaction mechanism	Best fitted isotherm model	Ref.
Functionalized MWCNTs	Zn(II)	1.05	pH 10, initial concentration= 1.1 mg/L, adsorbent mass= 0.09 mg, contact time= 120 min, T = 50°C, agitation speed= 120 r/min	Electrostatic interaction	Langmuir, Freundlich	[¹⁵⁸]
NN-mSiO₂@MWCNTs	Cu(II)	66.577	pH 6.2, initial concentration= 100 mg/L, adsorbent mass= 20 mg, contact time= 30 min, T = 25°C	Chemisorption	Langmuir	[¹⁶⁸]
SWCNT	Hg(II)	40.16	pH 5, initial concentration= 30 mg/L, adsorbent mass (m/v) = 0.25 mg/mL, contact time= 1 h, T = 25°C	Chemisorption	Langmuir, Freundlich	[¹⁶⁹]
Thiol-derivatized SWNTs	Hg(II)	131.58	pH 5, initial concentration= 30 mg/L, adsorbent mass (m/v) = 0.25 mg/mL, contact time= 1 h, T = 25°C	Strong chemisorption, soft acid-soft base interactions	Langmuir	[¹⁶⁹]
Raw MWCNTs	As(V)	2.995	pH 4, initial concentration= 94 µg/dm³, adsorbent mass= 100 mg/dm³, contact time= 45 min, T = 25°C	Electrostaticinteraction, chemisorption	Langmuir?Freundlich )Sips(	[¹⁷⁴]
Oxidized MWCNTs	As(V)	3.613	pH 4, initial concentration= 94 µg/dm³, adsorbent mass= 100 mg/dm³, contact time= 45 min, T = 25°C	Chemisorption, electrostaticinteraction, specific adsorption	Langmuir?Freundlich )Sips(	[¹⁷⁴]
e-MWCNTs	As(V)	12.175	pH 4, initial concentration= 94 µg/dm³, adsorbent mass= 100 mg/dm³, contact time= 45 min, T = 25°C	Chemisorption, electrostatic interaction, specific adsorption	Freundlich	[¹⁷⁴]
MWCNTs	Cu(II)	3.19 × 10⁻⁵ mol/g	pH 5, initial concentration=2.36 × 10 ^?⁴ mol/L,T = 30°C	Electrostatic interaction, surface complexation, surface precipitation	Langmuir	[¹⁷⁵]
SWNTs	Cr(VI)	20.3	pH 4, initial concentration= 500 µg/L, adsorbent mass= 100 mg/L, contact time= 720 min	Chemisorption, physisorption, electrostatic interaction	Langmuir	[¹⁷⁶]
MWNTs	Cr(VI)	2.48	pH 4, initial concentration= 500 µg/L, adsorbent mass= 100 mg/L, contact time= 720 min	Chemisorption, physisorption, electrostatic interaction	Langmuir	[¹⁷⁶]
MWCNT–HAP	Co(II)	16.26	pH 6, initial concentration= 1.69×10⁻⁴ mol/L, adsorbent mass= 0.6 g/L, T = 20°C	Surface complexation	Langmuir	[¹⁷⁷]
Sulphur containingMWCNTs (S-MWCNTs)	Hg(II)	72.8 µg/g	pH 12.15, initial concentration= 100 ppb, contact time= 60 min	Chemisorption, soft acid-soft base interactions, electrostatic interaction	Freundlich	[¹⁷⁸]
Ag-MWCNTs	Cu(II)	53.29	pH 6, initial concentration= 50 mg/L, adsorbent mass= 0.05 g, contact time= 100 min, T = 20?40°C, agitation speed= 180 r/min	Chemisorption, ion exchange	Langmuir	[¹⁷⁹]
Ag-MWCNTs	Cd(II)	51.97	pH 7, initial concentration= 50 mg/L, adsorbent mass= 0.05 g, contact time= 100 min, T = 20?40°C, agitation speed= 180 r/min	Chemisorption, ion exchange	Langmuir	[¹⁷⁹]
CF-CNTs-A	As(V)	16.84	pH 4, initial concentration= 5 mg/L, adsorbent mass= 0.2 g/L, contact time= 360 min, T = 25°C, agitation speed= 150 r/min	Electrostatic interaction, surface complexation	Freundlich	[¹⁸⁰]
CF-CNTs-A	As(III)	16.21	pH 7.5, initial concentration= 5 mg/L, adsorbent mass= 0.2 g/L, contact time= 300 min, T = 25°C, agitation speed= 150 r/min	Surface complexation	Langmuir	[¹⁸⁰]
CF-CNTs	As(V)	30.96	pH 4, initial concentration= 5 mg/L, adsorbent mass= 0.2 g/L, contact time= 360 min, T = 25°C, agitation speed= 150 r/min	Electrostatic interaction, surface complexation	Freundlich	[¹⁸⁰]
CF-CNTs	As(III)	28.74	pH 7.5, initial concentration= 5 mg/L, adsorbent mass= 0.2 g/L, contact time= 300 min, T = 25°C, agitation speed= 150 r/min	Surface complexation	Langmuir	[¹⁸⁰]
CS/MWCNTs	Cu(II)	454.55	pH 5.5, initial concentration= 100 mg/L, adsorbent mass= 0.05 g, contact time= 90 min	Surfacecomplexation, van der Waals interactions	Langmuir	[¹²⁹]
SWCNTs/WSh	Pb(II)	185.18	pH 5, initial concentration= 50 mg/L, adsorbent mass= 1 g/L, contact time= 30 min, T = 25°C, agitation speed= 65 r/min	Electrostaticinteractions, chemisorption, precipitation,	Langmuir	[¹⁶¹]
CNT	As(III) As(V)	0.124 0.373	pH 7, initial concentration= 500 µg/L, adsorbent mass= 2.5 g/L, contact time= 240 min	Electrostatic interactions	Langmuir	[¹⁶²]
ZCNT	As(III) As(V)	111.1 1666.7	pH 7, initial concentration= 500 µg/L, adsorbent mass= 2.5 g/L, contact time= 240 min	Complexation, chemisorption, diffusion processes	Langmuir	[¹⁶²]
NCs	Cr(VI)	264.5	pH 2, initial concentration= 100 mg/L, adsorbent mass= 2.5 g/L, contact time= 240 min, T = 30°C, agitation speed= 100 r/min	Electrostaticinteractions, chemisorption, intraparticle diffusion, external diffusion	Langmuir	[¹⁷⁰]
NCs	Cd(II)	229.9	pH 7.5, initial concentration= 100 mg/L, adsorbent mass= 2.5 g/L, contact time= 240 min, T = 30°C, agitation speed= 100 r/min	Electrostaticinteractions, complexation, chemisorption, intraparticle diffusion, external diffusion	Langmuir	[¹⁷⁰]
MWCNTs	Hg(II)	5.479	pH 6, initial concentration= 100 mg/L, adsorbent mass= 0.02 g, contact time= 90 min, agitation speed= 110 r/min	Ion exchange, physisorption, chemisorption, external diffusion	Langmuir	[¹⁸¹]
MWCNT-OX	Hg(II)	27.32	pH 6, initial concentration= 100 mg/L, adsorbent mass= 0.02 g, contact time= 90 min, agitation speed= 110 r/min	Ion exchange, physisorption, chemisorption, complexation, external diffusion	Langmuir	[¹⁸¹]
CNT-I	Hg(II)	123.45	pH 6, initial concentration= 100 mg/L, adsorbent mass= 0.02 g, contact time= 105 min, agitation speed= 110 r/min	Ion exchange, physisorption, chemisorption, complexation, external diffusion, soft-soft interaction	Langmuir	[¹⁸¹]
Sulfur incorporatedMWCNT (CNT-S)	Hg(II)	151.51	pH 6, initial concentration= 100 mg/L, adsorbent mass= 0.02 g, contact time= 105 min, agitation speed= 110 r/min	Ion exchange, physisorption, chemisorption, complexation, external diffusion, soft acid-soft base interaction	Langmuir	[¹⁸¹]
Amino and thiolated functionalized MWCNTs	Hg(II)	84.66	pH 6, initial concentration= 10 mg/L, adsorbent mass= 400 mg/L, contact time= 60 min, T = 25°C, agitation speed= 200 r/min	Physisorption, soft acid-soft base interaction	Langmuir	[¹⁸²]
p-MWCNTs	Cu(II)	NA 36.82 based on D-R model	pH 5, initial concentration= 20 mg/L	Physical adsorption	Freundlich	[¹⁸³]
Sulfonated MWCNTs (s-MWCNTs)	Cu(II)	NA 43.16 based on D-R model	pH 5, initial concentration= 20 mg/L	Electrostaticinteractions, physisorption, inner-spheresurface complexation	Freundlich	[¹⁸³]
Raw MWCNTs	Hg(II)	32.4	pH 4.3, initial concentration= 4.0 mg/L, agitation speed= 200 r/min	Electrostatic interactions, complexation, chemisorption, intraparticle diffusion	Langmuir	[¹⁸⁴]
OH-MWCNTs (with a phenolic hydroxyl functional group)	Hg(II)	120.1	pH 4.3, initial concentration= 4.0 mg/L, agitation speed= 200 r/min	Electrostatic interactions, complexation, chemisorption, external diffusion, intraparticle diffusion	Langmuir	[¹⁸⁴]
COOH-MWCNTs	Hg(II)	127.6	pH 4.3, initial concentration= 4.0 mg/L, agitation speed= 200 r/min	Electrostatic interactions, complexation, chemisorption, external diffusion, intraparticle diffusion	Langmuir	[¹⁸⁴]
As-produced MWCNT	Pb(II) Cu(II) Cr(VI) Cd(II) Ni(II)	48.0 45.0 43.0 39.0 35.0	pH 5.5, initial concentration= 20 mg/L, adsorbent mass= 1 g/L, contact time= 120 min, agitation speed= 200 r/min	Chemisorption, electrostaticinteractions	Langmuir, Freundlich	[¹⁵⁴]
Oxidized MWCNT	Pb(II) Cu(II) Cr(VI) Cd(II) Ni(II)	75.0 70.4 67.0 66.0 59.2	pH 5.5, initial concentration= 20 mg/L, adsorbent mass= 1 g/L, contact time= 120 min, agitation speed= 200 r/min	Chemisorption, electrostaticinteractions	Langmuir, Freundlich	[¹⁵⁴]
Oxidized MWCNT	Cu(II)	200.0	pH 6, initial concentration= 50 mg/L, adsorbent mass=0.03 g, contact time= 75 min, T = 25°C	Chemisorption, electrostatic interaction	Langmuir	[¹⁶³]
Raw MWCNTs	Sr(II)	3.13	pH 6, initial concentration= 30 mg/L, contact time= 24 h, T = 25°C, agitation speed= 150 r/min	NA	Langmuir	[¹⁶⁶]
Oxidized MWCNTs	Sr(II)	10.87	pH 6, initial concentration= 30 mg/L, contact time= 24 h, T = 25°C, agitation speed= 150 r/min	Chemisorption	Langmuir	[¹⁶⁶]
MWCNT/SMP (Hybrid)	Sr(II)	14.92	pH 6, initial concentration= 30 mg/L, contact time= 24 h, T = 25°C, agitation speed= 150 r/min	Chemisorption	Langmuir	[¹⁶⁶]
MnO₂-CNTs	Hg(II)	58.82	pH 5?7, initial concentration= 10 mg/L, adsorbent mass= 0.02 g/20 mL, contact time= 80 min, T = 25°C, agitation speed= 180 r/min	Electrostaticinteractions, physisorption	Freundlich	[¹⁷²]
Al₂O₃/MWCNTs	Cd (II)	27.21	pH 7, initial concentration= 1 mg/L, adsorbent mass= 1 g/L, contact time= 240 min, T = 25°C, agitation speed= 150 r/min	Electrostatic interactions, physisorption, surface complexation, surface precipitation, van der Waals interactions	Langmuir	[¹⁸⁵]
MWCNTs	Cr(VI)	13.2	NA	Electrostatic interactions	Langmuir	[¹⁸⁶]
IL-oxi-MWCNTs	Cr(VI)	85.83	pH 2.5?4.0, initial concentration= 20 mg/L, adsorbent mass= 0.15 g, contact time= 40 min, agitation speed= 150 r/min	Electrostatic interactions, cation-π interaction, anion-π interaction	Freundlich	[¹⁸⁶]
Raw CNTs	Cd(II)	1.66	pH 7, initial concentration= 1 mg/L, adsorbent mass= 50 mg, contact time= 120 min, agitation speed= 150 r/min	Electrostatic interactions	Langmuir	[¹⁸⁷]
O-MWCNTs	Pb(II) Cd(II) Cu(II) Zn(II)	76.7 32.2 15.3 13.6	pH 5, initial concentration= 40 mg/L adsorbent mass= 5 mg, contact time= 30 min, , T = 25°C	Electrostatic interaction	Langmuir	[¹⁸⁸]
Acid modified CNTs	Cd(II)	4.35	pH 7, initial concentration= 1 mg/L adsorbent mass= 50 mg, contact time= 120 min, agitation speed= 150 r/min	Electrostatic interactions, chemisorption, ion exchange	Langmuir	[¹⁸⁹]
MWCNTs	Hg(II)	25.641	pH 7, initial concentration= 0.1 mg/L, adsorbent mass= 0.5 g/L, contact time= 120 min, T = 25°C, agitation speed= 150 r/min	Chemisorption	Freundlich, Langmuir	[¹⁹⁰]
MWCNT-TA	Cu(II)	30.85	pH 6, initial concentration= 50 mg/L, adsorbent mass= 0.01 g, contact time= 240 min, T = 25°C, agitation speed= 220 r/min	Charge interaction	Langmuir	[¹⁹¹]
Raw CNTs	Cr(VI)	3.115	pH 4, initial concentration= 1 mg/L, adsorbent mass= 75 mg, contact time= 240 min, agitation speed= 200 r/min	Electrostatic interactions	Langmuir	[⁵²]
Acid modified CNTs	Cr (VI)	1.314	pH 3, initial concentration= 1 mg/L, adsorbent mass= 75 mg, contact time= 240 min, agitation speed= 200 r/min	Electrostatic interactions	Langmuir	[⁵²]
MWCNTs-NCO	Pb(II) Pb-201	196.10	pH 6, initial concentration= 10 mg/L, adsorbent mass= 5 mg, contact time= 30 min, T = 25°C	Electrostatic interactions	Langmuir	[¹²⁶]
As-synthesized CNTs	Cu(II)	55.25	pH 7, initial concentration= 800 mg/L, adsorbent mass= 50 mg, contact time= 300 min, T = 25°C	Chemisorption, diffusion-based process	Langmuir, Freundlich	[¹⁵²]
Acid-treated CNTs	Cu(II)	82.64	pH 7, initial concentration= 800 mg/L, adsorbent mass= 50 mg, contact time= 300 min, T = 25°C	Chemisorption, diffusion-based process	Langmuir, Freundlich	[¹⁵²]
Chitosan-treated CNTs	Cu(II)	120.48	pH 7, initial concentration= 800 mg/L, adsorbent mass= 50 mg, contact time= 300 min, T = 25°C	Chemisorption, diffusion-based process	Langmuir, Freundlich	[¹⁵²]
Acid–chitosan CNTs	Cu(II)	158.73	pH 7, initial concentration= 800 mg/L, adsorbent mass= 50 mg, contact time= 300 min, T = 25°C	Chemisorption, diffusion-based process	Langmuir, Freundlich	[¹⁵²]
PPy/O-MWCNTs	Pb(II) Ni(II) Cd(II)	408.2 409.4 392.0	pH 6, initial concentration= 100 mg/L, adsorbent mass= 60 mg/L, contact time= 60 min, T = 30°C, agitation speed= 200 r/min	Chemisorption, physisorption	Langmuir	[¹⁵³]
Fe₃O₄/O-MWCNTs	Pb(II)	67.25	pH 5, initial concentration= 200 mg/L, adsorbent mass= 1 g/L, contact time= 360 min, T = 25°C	Chemisorption, electrostatic interactions, complexation, chemical bonds’ interactions	Langmuir	[¹⁵⁵]
Fe₃O₄/O-MWCNTs	Zn(II)	3.759	pH 5, initial concentration= 30 mg/L, adsorbent mass= 1 g/L, contact time= 360 min, T = 25°C	Chemisorption, electrostatic interactions, complexation, chemical bonds’ interactions	Langmuir	[¹⁵⁵]
KM-CNTs	As(III)	23.40	pH 3, initial concentration= 1 mg/L, adsorbent mass= 20 mg, contact time= 55 min, agitation speed= 180 r/min	Chemisorption, complexation, ion exchange, electrostaticinteraction	Freundlich	[¹⁶⁴]
KB-CNTs	As(III)	14.23	pH 6, initial concentration= 1 mg/L, adsorbent mass= 20 mg, contact time= 55 min, agitation speed= 180 r/min	Chemisorption, complexation, ion exchange, electrostatic interaction	Langmuir	[¹⁶⁴]
PAMAM/CNTs	Ni(II) Co(II) Zn(II) As(III)	3900 3800 3650 3500	pH 7, initial concentration= 100 mg/L, adsorbent mass= 0.03 g/L, contact time= 15 min, T = 25°C, agitation speed= 14000 r/min	Chelating, chemisorption, electrostatic interactions, van der Waals, encapsulating interactions, complexation	Langmuir	[¹⁶⁵]
NaAlg-CNTs	Co(II)	456.5	pH 6.8, initial concentration= 400 mg/L, adsorbent mass= 0.1 g, contact time= 540 min, T = 21°C	Electrostatic interactions, π−π electron-donor/acceptor interactions	Freundlich	[¹⁹²]
NaAlg-HAp-CNT nanocomposite beads	Co(II)	1111.1	pH 6.8, initial concentration= 400 mg/L, adsorbent mass= 0.1 g ,contact time= 540 min, T = 21°C	Electrostatic interactions, π−π electron-donor/acceptor interactions	Freundlich	[¹⁹²]
N₂H₄-SH-Fe₃O₄/O-MWCNTs	Pb(II) Zn(II)	40.0 21.28	pH 6, initial concentration= 40 mg/L, adsorbent mass= 10 mg, contact time= 30 min	Chemisorption, physisorption	Freundlich	[¹⁹³]
pTSA-Pani@GO-CNT	Cr(VI)	142.85	pH 2, initial concentration= 200 mg/L, adsorbent mass= 0.02 g, contact time= 500 min, T = 30°C	Electrostatic interactions, hydrophobic interactions, π−π skating interactions	Langmuir	[¹⁵⁰]
PAMAM/CNTs	Cu(II) Pb(II)	3333 4870	pH 7, initial concentration= 100 mg/L, adsorbent mass= 0.03 g/L, T = 25°C	Chelating, electrostatic interactions, van der Waals, encapsulating interactions, complexation	Langmuir	[¹⁵¹]
MWCNTs	Cd(II)	43.103	pH 8?9, initial concentration= 50 mg/L, adsorbent mass= 20 mg, contact time= 60 min, T = 45°C, agitation speed= 250 r/min	Chemisorption, electrostaticinteraction,	Langmuir	[¹⁵⁶]
MWCNTs-COOH	Cd(II)	212.766	pH 8?9, initial concentration= 50 mg/L, adsorbent mass= 20 mg, contact time= 60 min, T = 45°C, agitation speed= 250 r/min	Chemisorption, electrostaticinteraction,	Dubinin–Radushkevich	[¹⁵⁶]
MWCNTs-f	Cd(II)	400	pH 8?9, initial concentration= 50 mg/L, adsorbent mass= 20 mg, contact time= 60 min, T = 45°C, agitation speed= 250 r/min	Chemisorption, electrostaticinteraction,	Temkin	[¹⁵⁶]
NiO/CNT	Pb(II)	24.63	pH 7, initial concentration= 20 mg/L, adsorbent mass= 0.1 mg, contact time= 10 min	van der Waals interaction, electrostatic attraction, chemisorption	Freundlich	[¹⁹⁴]
Acidified functionalized MWCNTs	Pb(II) Cu(II) Cd(II) Ni(II)	166 123 101 95	pH 9, initial concentration= 100 mg/L, adsorbent mass= 0.5 g, contact time= 10 h, agitation speed= 200 r/min	Chemisorption, complexation, ion exchange,	Langmuir, Freundlich	[¹⁹⁵]
MWCNTs	Hg(II)	71.1	pH 7, initial concentration= 100 µg/L, adsorbent mass= 0.5 g/L, contact time= 90 min, T = 20°C, agitation speed= 245 r/min	Chemisorption, electrostaticinteraction	Freundlich, Dubinin?Radushkevich	[¹⁹⁶]
MWCNTs-OH	Hg(II)	78.9	pH 7, initial concentration= 100 µg/L, adsorbent mass= 0.5 g/L, contact time= 90 min, T = 20°C, agitation speed= 245 r/min	Chemisorption, electrostaticinteraction	Freundlich, Dubinin?Radushkevich	[¹⁹⁶]
MWCNTs-COOH	Hg(II)	134.0	pH 7, initial concentration= 100 µg/L, adsorbent mass= 0.5 g/L, contact time= 90 min, T = 20°C, agitation speed= 245 r/min	Chemisorption, electrostaticinteraction	Freundlich, Dubinin?Radushkevch	[¹⁹⁶]
MWCNTs-NH₂	Hg(II)	205.0	pH 7, initial concentration= 100 µg/L, adsorbent mass= 0.5 g/L, contact time= 90 min, T = 20°C, agitation speed= 245 r/min	Chemisorption, electrostatic interaction	Freundlich, Dubinin?Radushkevich	[¹⁹⁶]
Fe₃O₄/CNT	Pb(II)	21.55	pH 6, initial concentration= 20 mg/L, adsorbent mass= 0.10 g, contact time= 40 min, T = 25°C	Chemisorption, physisorption	Langmuir, Freundlich	[¹⁹⁷]

Tab.1 Adsorption of heavy metals using non-modified and functionalized CNTs, and their maximum adsorption capacities*

Fig.2 Schematic diagram of the acid modification of CNTs by various methods and the major mechanism for adsorption of divalent metal ions on the modified CNTs surface

Fig.3 Adsorption mechanism of metal ions by functionalized CNT with increasing the solution pH

Fig.4 Adsorption mechanism of Hg(II) with the (a) CNT-OX, (b) CNT-I, (c) CNT-S

Fig.5 Schematic diagram of the proposed mechanism for adsorption of (a) As(V) and (b) As(III) on the CF-CNTs

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