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1 Challenges and opportunities in functional carbon nanotubes for membrane-based water treatment and desalination Sharafat Ali, a Syed Aziz Ur Rehman, a Hong-Yan Luan, a Muhammad Usman Farid, c Haiou Huang a,b* a State Key Joint Laboratory of Environmental Simulation and Pollution Control, School of Environment, Beijing Normal University, No. 19, Xinjiekouwai Street, Beijing, 100875, China b Department of Environmental Health Sciences, Bloomberg School of Public Health, The John Hopkins University, 615 North Wolfe Street, MD 21205, USA c School of Energy and Environment, City University of Hong Kong, Tat Chee Avenue Kowloon, Hong Kong, China ⁎ Corresponding author at: State Key Joint Laboratory of Environmental Simulation and Pollution Control, School of Environment, Beijing Normal University, No. 19, Xinjiekouwai Street, Beijing 100875, China. E-mail address: [email protected] (H. Huang). Supporting information contain two figures and four tables.

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Challenges and opportunities in functional carbon nanotubes for membrane-based water

treatment and desalination

Sharafat Ali,a Syed Aziz Ur Rehman,a Hong-Yan Luan,a Muhammad Usman Farid,c Haiou

Huanga,b*

a State Key Joint Laboratory of Environmental Simulation and Pollution Control, School of Environment,

Beijing Normal University, No. 19, Xinjiekouwai Street, Beijing, 100875, China

b Department of Environmental Health Sciences, Bloomberg School of Public Health, The John Hopkins

University, 615 North Wolfe Street, MD 21205, USA

c School of Energy and Environment, City University of Hong Kong, Tat Chee Avenue Kowloon, Hong

Kong, China

Corresponding author at: State Key Joint Laboratory of Environmental Simulation and Pollution Control,⁎

School of Environment, Beijing Normal University, No. 19, Xinjiekouwai Street, Beijing 100875, China.

E-mail address: [email protected] (H. Huang).

Supporting information contain two figures and four tables.

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Figure S1. Research articles published on CNTs/f-CNT membranes for desalination and water

treatment. (Database “web of Science” and date of analysis 3rd July, 2018).

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Figure S2. Research articles published on nanomaterials for desalination and water treatment.

(Database “web of Science” and date of analysis 3rd July, 2018). NMs represent nanomaterials.

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Table S1. List of publications related to the removals of arsenic or heavy metals by f-CNTs and f-CNT membranes.

Types of contaminants

CNT Adsorbents b Mass loading of CNTs

Removal Mechanism Comments Ref;

Types aAC or RE

Diameter (nm)

cIC

As(III) Multi-walled carbon nanotube-zirconia nanohybrid (MWCNT-ZrO2)

2mg/g 20-40 nm 0.1mg L-1 100mg/10ml Chemisorption/Physisorption

The adsorption capacity of AS (III) is not associated with pH value.

(Ntim and Mitra, 2012)

Iron oxide coated multi-walled carbon nanotubes

1.73mg/g 20-40 nm 0.1 mg L-1 10mg/10ml Electrostatic interaction, surface complexation

Suggesting that modifying MWCNTs with other groups can develop potential adsorbents for water treatment.

(Ntim and Mitra, 2011)

As(V) Fe(III) oxide coated ethylene-diamine modified MWCNTs

23.4mg/g 5-10 nm 0.1 mg L-1 50mg/10ml Ion exchange Greater efficiency to remove As(V) due to enormous adsorbing sites.

(Veličković et al., 2012)

Multi-walled carbon nanotube-zirconia nanohybrid (MWCNT-ZrO2)

5mg/g 20-40 nm 0.1 mg L-1 100mg/10ml Chemisorption/Physisorption

The adsorption capacity of As(V)) is not associated with pH value.

(Ntim and Mitra, 2012)

Iron oxide coated multi-walled carbon nanotubes

0.18mg/g 20-40 nm 0.1 mg L-1 10mg/10ml Electrostatic interaction, surface complexation

Suggesting that modifying MWCNTs with other groups can develop potential adsorbents for water treatment.

(Ntim and Mitra, 2011)

Cr(III) Nitrogen-doped Magnetic CNTs

638mg/g N/A 200 mg L-1 10mg/500ml Chemical adsorption 10 fold greater removals than activated carbon due to large SSA.

(Shin et al., 2011)

Acid modified MWCNTs 0.5mg/g 24 nm 1 mg L-1 120000 mg/ 500ml

Electrostatic interaction Increasing removal of Cr with increasing the dose of CNTs.

(Atieh et al., 2010)

Cr(VI) Acid treated CNTs N/A N/A N/A 10mg/2ml Ion exchange f-CNTs can be potentially use for heavy metal removals.

(Xu et al., 2011)

Activated carbon coated CNTs 9mg/g 10-20 nm 0.2-0.5 mg L-1

2mg/50ml N/A The f-CNT can be used largely for the removal of Cr ions.

(Atieh, 2011)

Functionalized MWCNTs 95% 10-30 nm 0.1 mg L-1 100mg/10ml Ion exchange, Intraparticle diffusion

The regeneration of Cr(VI) > 95% can be easily achieved via high pH.

(Pillay et al., 2009)

CeO2/ACNTs 31.55 mg/g

20-80 nm 35.3mg L-1 100mg/100ml Ion exchange Suggesting that CeO2/ACNTs has high potential for heavy metal removals.

(Di et al., 2006)

Pb(II) MPTS grafted MWCNTs/Fe3O4

65.40 mg/g

N/A 50 mg L-1 100mg/100ml Lewis acid–base interactions

Better efficiency for the removal of heavy metal ions in various pH

(Zhang et al., 2012)

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Types of contaminants

CNT Adsorbents b Mass loading of CNTs

Removal Mechanism Comments Ref;

Types aAC or RE

Diameter (nm)

cIC

value.Magnetic-functionalized MWCNTs

> 80% N/A 100 mg L-1 1000mg/4ml N/A High removal efficiency due to intrinsic properties, large SSA and porous structure.

(Wang et al., 2012)

MWCNTs/Fe3O4 41.77 mg/g

10-20 nm 30 mg L-1 500mg/1000ml Electrostatic, hydrophobic and π-π interactions

Easily regenerate the adsorbent by external magnetic field after several cycles.

(Ji et al., 2012)

MWCNTs/Fe3O4 modified with APTS

75.02 mg/g

10-20 nm 30 mg L-1 500mg/1000ml Electrostatic, hydrophobic and π-π interactions

Easily regenerate the adsorbent by external magnetic field after several cycles.

(Ji et al., 2012)

MWCNTs grafted/PAAM membrane

98% N/A 10 mg L-1 1000mg/ 1000ml

Electrostatic interaction The f-CNT membrane potentially enhances the water flux and removal of heavy metals.

(Yang et al., 2011)

Oxidized CNT sheets 101.05mg /g

N/A 1200mg L-1 50mg/25ml Chemical interaction Considering the oxidize CNT sheets promising material for the removal of heavy metal ions.

(Tofighy and Mohammadi, 2011)

MWCNTs grafted with 2-vinylpyridine (VP)

37mg/g N/A 10 mg L-1 640mg/1000ml Ion exchange, electrostatic interaction

Showed high suitability for preconcentration and immobilization of heavy metal ions from water.

(Wang et al., 2011)

Oxidized MWCNTs 95 % 10-30 nm 10 mg L-1 3000mg/100ml Chemical, electrostatic, hydrophobic and π-π interactions

High removal efficiency toward heavy metal ions in waste water.

(Li et al., 2011)

Alumina-coated MWCNTs >75 % N/A Different IC 10mg/25ml N/A The composite can be used largely to remove lead from industrial waste water.

(Gupta et al., 2011)

Nitrogen-doped Magnetic CNTs

139mg/g N/A 200 mg L-1 10mg/500ml Chemical adsorption High removal efficiency toward Pb compared to Cr.

(Shin et al., 2011)

TiO2/MWCNT composites 137mg/g N/A 1 mg L-1 20mg/10ml N/A Important adsorption ability to remove large amount of Pb in short period.

(Xiaowei Zhao, 2010)

Chitosan grafted MWCNTs (MWCNT-g-CS)

35mg/g N/A N/A 1000mg/ 1000ml

N/A Significant for the preconcentration and immobilization of heavy metal ions in waste water.

(Shao et al., 2010a)

Oxidize MWCNTs 90 % 20-30 nm 10 mg L-1 3000mg/ N/A The sorption of Pb largely depend (Xu et al.,

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Types of contaminants

CNT Adsorbents b Mass loading of CNTs

Removal Mechanism Comments Ref;

Types aAC or RE

Diameter (nm)

cIC

1000ml on foreign ions and ionic strength. 2008)

Mn oxide-coated CNTs 98 % 2.60 nm 10-60mg L-1

50mg/100ml Electrostatic interaction, Surface complexation

300% greater adsorption capacity than raw CNTs.

(Wang et al., 2007b)

Acidified MWCNTs 85mg/g 30 nm 50 mg L-1 25mg/50ml Physical adsorption The regeneration of Pb increasing with decreasing pH and can be used for several cycles.

(Wang et al., 2007a)

Oxidized CNTs 83.6mg/g 20-30 nm 10-60mg L-1

20mg/100ml N/A Proposing higher adsorption capacity to Pb.

(Li et al., 2006)

Cd(II) Alumina-decorated MWCNTs 0.948 mg/g

10-20 nm 1 mg L-1 1000mg/ 1000ml

Electrostatic interaction, Physical adsorption, surface precipitation

Capable of removing both metallic and organic Contaminants.

(Liang et al., 2015)

Oxidized MWCNTs 22.32 mg/g

16.09 nm 5 mg L-1 1mg/10ml Chemisorption The sorption capacity is strongly dependent on pH due to surface charge and showed best performance in the pH range of 6-10.

(Vuković et al., 2010)

Ethylenediamine functionalized MWCNTs

21.23 mg/g

21.25 nm 5 mg L-1 1mg/10ml Chemisorption The sorption capacity is strongly dependent on pH due to surface charge and showed best performance in the pH range of6-10.

(Vuković et al., 2010)

Magnetic-functionalized MWCNTs

> 85% N/A 100 mg L-1 1000mg/4ml N/A Excellent removal efficiency to heavy metals because of intrinsic properties and large SSA.

(Wang et al., 2012)

Oxidize CNT sheets 75.84 mg /g

N/A 1200 mg L-1 50mg/25ml Chemical interaction Considering the oxidize CNT sheets promising material for the removal of heavy metal ions.

(Tofighy and Mohammadi, 2011)

Acid modified CNTs 98% 10-20 nm N/A 250mg Electrostatic interaction Potential material for water purification.

(Ihsanullah et al., 2015)

MWCNTs modified with Chitosan

> 90 % 60-100 nm N/A 2000mg Electrostatic interaction The removal efficiency increases with increase of mass of both MWCNTs and Chitosan.

(Salam et al., 2011)

Hg(II) MnO2-coated CNTs 200% > thanraw CNTs

30-50 nm 10 mg L-1 200mg/20ml Electrostatic interaction Higher adsorption affinity to other heavy metals rather than Hg.

(Moghaddam and Pakizeh, 2015)

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Types of contaminants

CNT Adsorbents b Mass loading of CNTs

Removal Mechanism Comments Ref;

Types aAC or RE

Diameter (nm)

cIC

Thiol-derivatized SWCNTs 99.8% N/A 40 mg L-1 0.04mg/ml Electrostatic interaction Easily desorb/regenerate Hg after treatment of water.

(Bandaru et al., 2013)

Amino and thiolated functionalized-MWCNTs

84.66 mg/g

5-10 nm 100 mg L-1 10mg/1000ml Physisorption Highly efficient removal from real waste water and further research is necessary to commercialize.

(Hadavifar et al., 2014)

Functionalized- MWCNTs 121.45mg/g

10-20 nm 100-500mg L-1

2500mg/ 1000ml

Ion exchange Easily use to adsorb and desorb Hg(II) from waste water.

(Gupta et al., 2014)

Sulphur containing MWCNTs (S-MWCNTs)

0.07mg/g N/A 0.1 mg L-1 100mg/20ml Chemisorption Greater treatment ability for industrial waste water containing Hg and other anions and cations.

(Pillay et al., 2013)

MPTS grafted MWCNTs/Fe3O4

65.52 mg/g

N/A 50 mg L-1 1000mg/100ml Lewis acid–base interactions

Better removal of heavy metals in different pH concentration.

(Zhang et al., 2012)

Oxidized MWCNTs 3.83mg/g N/A 1-10 mg L-1 25mg/50ml Electrostatic interaction Small diameter of CNTs removing greater amount of Hg(II) from aqueous solution.

(El-Sheikh et al., 2011)

Nitrogen-doped Magnetic CNTs

519mg/g N/A 12.82mg L-1

10mg/500ml Chemical adsorption The removal efficiency is not very good compared to Cr.

(Shin et al., 2011)

Zn(II) Functionalized MWCNTs 99% 10-25 nm 1.1 mg L-1 90mg/100ml Electrostatic interaction Potential candidate to utilize for the removal of heavy metals.

(Mubarak et al., 2013)

Oxidize CNT sheets 58mg/g N/A 1200 mg L-1 50mg/25ml Chemical interaction Considering the oxidize CNT sheets promising material for the removal of heavy metal ions.

(Tofighy and Mohammadi, 2011)

MWCNTs modified with Chitosan

90% 60-100 nm N/A 2000mg Electrostatic interaction The removal efficiency increases with increase of mass of both MWCNTs and Chitosan.

(Salam et al., 2011)

Nitrogen-doped Magnetic CNTs

609mg/g N/A 12.8 mg L-1 10mg/500ml Chemical adsorption Better removal efficiency due to the presence of nitrogen and large surface area.

(Shin et al., 2011)

Oxidize MWCNTS 18mg/g 15 nm 15 mg L-1 5mg/5ml Electrostatic interaction Further research is necessary to understand the full mechanism.

(Cho et al., 2010)

MWCNTs purified with sodium hypochlorite

34.36 mg/g

< 10 nm 10-80 mg L-

150mg/100ml Electrostatic interaction Zinc ion could be easily regenerate

and the adsorbent can be used for many cycles.

(Chungsying Lu, 2006)

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Types of contaminants

CNT Adsorbents b Mass loading of CNTs

Removal Mechanism Comments Ref;

Types aAC or RE

Diameter (nm)

cIC

Cu(II) Sulfonated MWCNTs 58.9% > N/A 20 mg L-1 25mg/50ml Electrostatic interaction, surface complexation

Enabling MWCNTs for waste water treatment and composite formation or physical blending.

(Ge et al., 2014)

Magnetic-functionalized MWCNTs

97% N/A 100 mg L-1 1000mg/4ml N/A Excellent removal efficiency to heavy metals because of intrinsic properties and large SSA.

(Wang et al., 2012)

Magnetic MWCNTs (M-MWCNTs)

38.91 mg/g

10-20 nm 30 mg L-1 200mg/1000ml Electrostatic interaction, physical interaction

Easily regenerate the Cu after removal from polluted water.

(Zhang et al., 2012)

Oxidize CNT sheets 50.37 mg /g

N/A 1200 mg L-1 50mg/25ml Chemical interaction Considering the oxidize CNT sheets promising material for the removal of heavy metal ions.

(Tofighy and Mohammadi, 2011)

Amino functionalized MWCNTs (MWCNTs-NH2)

11.1mg/g 5-20 nm 30 mg L-1 0.5-2 wt% Ion exchange No loss in the adsorption capacity after four regeneration cycle.

(Salehi et al., 2012)

MWCNTs modified with Chitosan

> 95 % 60-100 nm N/A 2000mg Electrostatic interaction The removal efficiency increases with increase of mass of both MWCNTs and Chitosan.

(Salam et al., 2011)

Chitosan grafted MWCNTs (MWCNT-g-CS)

24mg/g N/A 10 mg L-1 1000mg/ 1000ml

N/A Significant for the preconcentration and immobilization of heavy metal ions in waste water.

(Shao et al., 2010a)

Co(II) Poly(acrylic acid) grafted/MWCNTs

N/A N/A 4 mg L-1 N/A Surface complexation Promising ability to use in water purification.

(Chen et al., 2012)

MWCNTS/iron oxide 2.88mg/g N/A 4.2 mg L-1 500mg/1000ml Ion exchange, surface complexation

Highlights the interaction between heavy metals and organic substances in waste water.

(Wang et al., 2011)

Oxidize CNT sheets 69.63 mg /g

N/A 1200 mg L-1 50mg/25ml Chemical interaction Considering the oxidize CNT sheets promising material for the removal of heavy metal ions.

(Tofighy and Mohammadi, 2011)

Ni(II) HNO3-treated MWCNTs 17.86 mg/g

10-20 nm 20 mg L-1 < 5 wt% Ion exchange Better removal efficiency towards heavy metal ions. (Mobasherpo

ur et al., 2012)

MWCNTs modified with Chitosan

< 90 % 60-100 nm N/A 2000mg Electrostatic interaction The removal efficiency increases with increase of mass of both MWCNTs and Chitosan.

(Salam et al., 2011)

Nitrogen-doped Magnetic 473mg/g N/A 12.8 mg L-1 10mg/500ml Chemical adsorption The removal efficiency is not very (Shin et al.,

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Types of contaminants

CNT Adsorbents b Mass loading of CNTs

Removal Mechanism Comments Ref;

Types aAC or RE

Diameter (nm)

cIC

CNTs good to Ni compared to Cr. 2011)Poly(acrylic acid) (PAA)-oxidized MWCNTs

N/A N/A 5 mg L-1 N/A Electrostatic interaction,π-π interaction

Suitable material for the preconcentration and solidification of Ni(II) from aqueous solution.

(Yang et al., 2009)

NaClO-modified SWCNTs 47.86 mg/g

< 2 nm 10-180mg L-1

50mg/100ml Electrostatic interaction High removal affinity to heavy metals and can be used for water treatment.

(Lu et al., 2009)

MWCNTs/Iron oxide > 82% N/A 6 mg L-1 N/A Ion exchange Promising candidate for the solidification and preconcentration of heavy metal ions as well as for radionuclides from water.

(Chen et al., 2009)

Oxidized MWCNTs 49.26 mg/g

5.5-14 nm 10-200mg L-1

20mg/50ml Electrostatic interaction Greater adsorption ability than raw MWCNTs in water.

(Kandah and Meunier, 2007)

Oxidized MWCNTs > 80% 10-30 nm 6-20 mg L-1 150mg/200ml Electrostatic interaction Excellent material for the adsorption of metal ions.

(Wang, 2006)

NaClO- Oxidized CNTs 47mg/g 2-10 nm 10-80 mg L-

150mg/100ml Ion exchange, surface

complexation, chemical interaction

Adsorption of Ni increasing with functional groups, total acidic sites, and negatively charged carbons.

(Lu and Liu, 2006)

a AC - adsorption capacity of pollutants % and mg/g, or RE – percentage removal efficiency. b The mass loading of CNTs mg/ml. c IC - initial

concentration mg/L. N/A represents not available.

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Table S2. List of publications related to the removal of organic contaminants by f-CNTs or f-CNT membranes.

Types of contaminants

CNT Adsorbents b Mass loading of CNTs

Removal Mechanism Comments Ref;Types aRE Diameter

(nm)c IC

PPCP CNT nanocomposite Improve 45% RE

Different diameters

0.1 mg L-1 22g/m2 Chemical adsorption High removal efficiency to PPCP from aqueous solution.

(Wang et al., 2016)

CNT nanocomposite 95% >10 nm 1 mg L-1 22g/m2 Electrostatic interactions, hydrogen bonding,π–π interaction

Increasing removal rate with increasing aromatic rings.

(Wang et al., 2015)

Humic Acid M-MWCNTs coated with Calcium

90.2% N/A 20 mg L-1 0.5 g/L Chemical adsorption Excellent removal efficiency and after 5 cycles the removal is still 89.2%.

(Li et al., 2017a)

Functionalized CNT buckypaper

>93% 41 nm 5 mg L-1 0.05g/20mm Physical interaction/ surface complexation

Superior adsorption capacity to NOMs and significantly increasing water flux.

(Yang et al., 2013b)

Dye (brilliant blue)

Calcium alginate/Carboxyl MWCNTs

98.2% N/A 6-50 mg L-1 5 wt% Physical interaction Greater rejection rate for small organic molecules.

(Guo et al., 2016)

Magnetic MWCNTs 98.8% 40-60 nm 1-37 mg L-1 0.5g/L Electrostatic attraction,Van der Waals interactions

Superior removal efficiency to dyes compare with other adsorption treatment.

(Gong et al., 2009)

Neutral red Magnetic MWCNTs 98.33% 40-60 nm 1-37 mg L-1 0.5g/L Electrostatic attraction,Van der Waals interactions

Superior removal efficiency to dyes compare with other adsorption treatment.

(Gong et al., 2009)

Methylene blue Magnetic MWCNTs 99.16% 40-60 nm 1-37 mg L-1 0.5g/L Electrostatic attraction,Van der Waals interactions

Superior removal efficiency to dyes compare with other adsorption treatment.

(Gong et al., 2009)

BSA Dodecylamine-Functionalized MWCNTs

N/A 5-10 nm 200 mg L-1 0.5 wt%/42cm2

N/A Showing ant-fouling resistant to Protein and increase water flux.

(Khalid et al., 2015)

Polyelectrolyte CNTs 99.9% N/A 1 mg L-1 N/A Electrostatic interaction Greater antifouling behavior of membrane making its suitable for recycling utilization.

(Liu et al., 2013)

Hyperbranched poly (amine-ester) functionalized MWCNTs

94.7% 10-20 nm 1mg/ml 0-2 wt% Hydrogen bonding Greater resistant to biofouling and protein in water and waste water treatment.

(Zhao et al., 2012)

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Types of contaminants

CNT Adsorbents b Mass loading of CNTs

Removal Mechanism Comments Ref;Types aRE Diameter

(nm)c IC

Phenols Alumina-impregnated CNTs 99.4% 10-20 nm 2 mg L-1 0.25g Ionic exchange High removal capacity to phenol via Langmuir adsorption model.

(Ihsanullah et al., 2015)

Polychlorinated biphenyls

b-cyclodextrin grafted MWCNTs (MWCNT-g-CD)

> 96% N/A 4.14 mg L-1 N/A π-π interactions, steric hindrance effect

Excellent adsorption capacity than raw MWCNTs.

(Shao et al., 2010b)

Atrazine SMWCNTs > 35 mg/g 10-20 nm 0.87-26.04mg L-1

0.002g/20ml N/A The adsorption capacity of SMWCNTs to atrazine is less compared with raw MWCNTs.

(Yan et al., 2008)

a RE – percentage removal efficiency of pollutants %. b The mass loading of CNTs g/L or g/ml. c IC - initial concentration mg/L. N/A represents

not available.

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Table S3. List of publications related to the removals of microorganism by f-CNT membranes.

Types of contaminants

CNT Adsorbents b Mass loading of CNTs

Removal Mechanism Comments Ref;Types aRE Diameter

(nm)c IS

Escherichia coli (E. coli)

silver doped-CNT membrane 100% 10-20 nm 1 × 106 CFU/ml 19.8g/600ml Physical interaction High anti-biofouling and can be used for water purification.

(Ihsanullah et al., 2015)

CNT-Ag nanohybrid 89.3% 5-15 nm 106 CFU/ml 0.004g/ml N/A Demonstrating high potential to inactivate large number of pathogenic microbes in waste water.

(Nie et al., 2017)

Chitosan/CNT nanocomposites

3.62 log reduction

60-110 nm

1.5 × 108 -5.0 × 108

CFU/ml5 wt% Physical interaction

and surface complexation

Superior antimicrobials capacity in short contact time.

(Morsi et al., 2017)

A-MWCNTs N/A 20-40 nm 106–109 CFU/ml 0.02g/100ml Electrostatic repulsion/steric obstruction

Dispersion of CNTs is not only responsible for the antibacterial effect but also dependent on the nutrition level.

(Chi et al., 2016)

MWCNTS-(C18) interaction with Microwaves

100% 20-40 nm 3.5 × 107 CFU/ml 1g/250ml Polarization The interaction of microwaves with f-CNTs is innovative approach which has the potential to employ for water disinfection.

(Al-Hakami et al., 2013)

Staphylococcusaureus

CNT-Ag nanohybrid 95% 5-15 nm 106 CFU/ml 0,004g/ml N/A Demonstrating high potential to inactivate large number of pathogenic microbes in waste water.

(Nie et al., 2017)

Chitosan/CNTs nanocomposites

5.2 log reduction

60-110 nm

1.5 × 108 -5.0 × 108

CFU/ml5 wt% Physical interaction

and surface complexation

Superior antimicrobial capacity in short contact time.

(Morsi et al., 2017)

Aspergillus flavus

Chitosan/CNTs nanocomposites

4.3 log reduction

60-110 nm

1.5 × 108 -5.0 × 108

CFU/ml5 wt% Physical interaction

and surface complexation

Superior antimicrobial capacity in short contact time.

(Morsi et al., 2017)

a RE – percentage removal efficiency of microorganism %. b The mass loading of CNTs g/ml or m2. c IC - initial counts of microorganism in the

suspension, CFU/ml. N/A represents not available.

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Table S4. List of publications related to desalination of salty water by f-CNT membranes.

Types of contaminants

Adsorbents b Mass loading of CNTs

Removal Mechanism Comments Ref;

Types aRE Diameter (nm)

Matrix c IC

Na2SO4 Sulfonated MWCNT-OH

96.8% < 8 nm PES 1000mg L-1

1g/12.56 cm2 Electrostatic interaction/ Donnan effect

High antifouling efficiency to organic matter and greater rejection ability toward salts.

(Zheng et al., 2017)

PMMA–MWNTs >99% 20-30nm PSf 2000mg L-1

0.67g/19.62cm2 N/A Significantly improve selectivity and permeability.

(Shen et al., 2013)

amine-functionalized MWCNTs

65% 5-20 nm PES 200 mg L-1

0.045wt%/19.6 cm2 Electrostatic interaction/ Donnan effect

High water flux and strong antifouling to BSA, while removing greater amount of Na2SO4.

(Vatanpour et al., 2014)

Acid modified MWCNTs-nAg/TFN membrane

95.6% 5-10 nm PSf 2000mg L-1

5.0wt%/0.01764 cm2

Chemical interaction High permeability, rejection and anti-biofouling properties.

(Kim et al., 2012)

NaCl E-CNTs 99% N/A PVDF 35000 mg L-1

2g/9.3 cm2 Chemical interaction Greatly enhancing water permeability.

(Lee et al., 2017)

amine-functionalized MWCNTs

20% 5-20 nm PES 200 mg L-1

0.045wt%/19.6 cm2 Electrostatic interaction/Donnan effect

High water flux and strong antifouling to BSA, while removing greater amount of NaCl.

(Vatanpour et al., 2014)

carboxyl-functionalized MWCNTs

> 90% 5 nm PSf 584 mg L-1

2% w/v/18.1 cm2 Electrostatic interaction/surface complexation

Better antifouling and Anti-oxidative properties.

(Zhao et al., 2014)

Zwitterion Functionalized CNTs

100% 15-20 nm PES 1000mg L-1

0.00075g/10 cm2 Steric hindrance/ electrostatic repulsion

Capable of rejecting both positive and negative ions, high antifouling and enhancing water flux.

(Wai-Fong et al., 2013)

COOH-MWCNTs 98.5% 5-15 nm Poly-amide RO

2000mg L-1

0.025%/36 cm2 Surface complexation High water permeability and antifouling behavior to BSA and removing greater than 98% of NaCl.

(Vatanpour and Zoqi, 2017)

Oxidized CNTs > 98% 10-20 nm PSf 2000mg L-1

0.4g/3.3×68 cm2 Surface complexation, electrostatic interaction

Excellent anti-biofouling properties toward DOM.

(Kim et al., 2014)

acid modified MWCNTs-nAg/TFN membrane

88.1% 5-10 nm PSf 2000mg L-1

5.0wt%/0.01764 cm2

Chemical interaction High permeability, rejection and better anti-biofouling capacity.

(Kim et al., 2012)

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MgSO4 amine-functionalized MWCNTs

45% 5-20 nm PES 200mg L-1

0.045wt%/19.6 cm2 Electrostatic interaction/Donnan effect

High water permeability and strong antifouling to BSA, while removing greater amount of MgSO4.

(Vatanpour et al., 2014)

Sodium alginate

Iron oxide doped-CNTs

90% 10-30 nm CNT matrix

4000mg L-1

19.88g/27mm Chemical adsorption High water flux and strong antifouling capacity.

(Ihsanullah et al., 2016b)

a RE - removal efficiency of salts, %. b The mass loading of CNTs g/cm2 or wt%/cm2 area of membrane. c IC - initial concentration, mg/L. N/A

represent not available.

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