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Nanomaterials-Based Devices
Nanomaterials-Based Devices
Edited by
Shadpour Mallakpour
Chaudhery Mustansar Hussain
Editors All books published by WILEY-VCH are carefully
produced. Nevertheless, authors, editors, and
Shadpour Mallakpour publisher do not warrant the information
Department of Chemistry contained in these books, including this book, to be
Isfahan University of Technology free of errors. Readers are advised to keep in mind
8415683111 Khomeini Shahr that statements, data, illustrations, procedural
Isfahan details or other items may inadvertently be
Iran inaccurate.
Chaudhery Mustansar Hussain Library of Congress Card No.:

Department of Chemistry and applied for
Environmental Science
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© 2022 WILEY-VCH GmbH, Boschstraße 12,

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10 9 8 7 6 5 4 3 2 1
v
Contents
1 Graphene-Based Nanomembranes for Sustainable Water

Purification Applications 1
Uluvangada T. Uthappa, Dusan Losic, and Mahaveer D. Kurkuri
1.1 Introduction 1
1.2 Graphene and GO-Based Membrane Characteristics and Properties 2
1.3 Fabrication of Graphene-Based Nanomembranes for Water Treatment
Applications 4
1.3.1 Desalination 4
1.3.2 Treatment for Dyes 5
1.3.3 Graphene Nanomembranes for Salt and Dye Rejection 5
1.3.4 Translation of Graphene Nanomembranes for Real Applications 23
1.4 Graphene Nanomembranes for Heavy Metals Treatment 24
1.4.1 Heavy Metals 24
1.5 Conclusion and Future Perspectives 25
Acknowledgments 26
Important Websites 26
References 26
2 Magnetic Graphene Oxide and Its Composite Nanomaterials: Application

in Environmental Decontamination 33
Karan Chaudhary and Dhanraj T. Masram
2.1 Introduction 33
2.2 Synthesis of Magnetic Graphene Oxide and Its Composite
Nanomaterials 35
2.3 Application of Magnetic Graphene Oxide and Its Composite
Nanomaterials 36
2.3.1 Removal of Toxic Metal Contaminants 36
2.3.2 Removal of Toxic Organic Contaminants 41
2.3.3 Removal of Other Contaminants 45
2.4 Conclusion 46
Further Reading 46
References 47
vi Contents
3 Biomass- or Biowaste-Derived Carbon Nanoparticles as Promising Materials

for Electrochemical Sensing Applications
Anila R. Cherian, Vinay S. Bhat, Anitha Varghese, and Gurumurthy Hegde
3.1 Introduction 53
3.2 Electrochemical Sensors 54
3.3 The Choice of Electrode Materials 54
3.4 Biomass-Derived Porous Carbons 56
3.4.1 Synthesis 56
3.4.1.1 Hydrothermal Carbonization (HTC) 56
3.4.1.2 Pyrolysis 58
3.4.2 Structure and Properties 58
3.5 Biomass-Derived Carbons in Electrochemical Sensing 61
3.5.1 H2O2 Sensing from Okra-Derived Carbons 61
3.5.2 Acetaminophen (AC) Detection by Seaweed-Derived Carbons 62
3.5.3 4-Nitrophenol Detection from Mango Leave-Derived Carbons 65
3.5.4 Bisphenol-A (BPA) Detection Using Bamboo Fungi-Derived Carbon 67
3.5.5 Nitrite Ion Detection by Areca Nut-Derived Carbons 69
3.5.6 Catechin Sensing Using Bougainvillea spectabilis-Derived Carbons 72
3.5.7 Progesterone Sensing by Onion Peel-Derived Carbons 73
3.5.8 Butein Detection from Oil Palm Leave-Derived Carbons 75
3.6 Conclusion and Future Perspective 79
Acknowledgment 79
Website Links 80
References 80
4 Applications of Carbon-Based Nanomaterials

for Wastewater Treatment 87
Ramesh K. Guduru, Anurag A. Gupta, Parwathi Pillai, and Swapnil Dharaskar
4.1 Introduction 87
4.2 Wastewater 88
4.3 Wastewater Treatment Methods 89
4.4 Nanomaterials 90
4.5 Carbon-Based Nanomaterials 92
4.6 Adsorption Mechanisms of CNTs and Graphene 93
4.6.1 Adsorption Through Physical and Chemical Methods 93
4.6.2 Adsorption Through Biological Methods 114
4.6.3 Adsorption Using Deep Eutectic Solvents (DESs) 114
4.6.4 CNT- and Graphene-Based Composite Adsorbents 114
4.7 Membrane-Based Filtration of Contaminants Using CNTs
and Graphene-Based Materials 115
4.8 Use of CNTs and Derivative Materials as Disinfecting Agents for Water
Purification 121
4.9 Commercial Use of CNMs in Wastewater Treatment 122
Contents vii
4.10 onclusions 122

C
Recommendations 123
References 123
5 Electrochemical Determination of Indigotine

Based on Poly(Gibberellic Acid)-Modified Carbon
Nanotube Paste Electrode 135
Girish Tigari, Jamballi G. Manjunatha, and Chenthattil Raril
5.1 Introduction 135
5.2 Experimental 136
5.2.1 Chemicals 136
5.2.2 Bare Carbon Nanotube Paste Electrode (BCNTPE) Preparation 136
5.3 Results and Discussion 136
5.3.1 Electropolymerization of BCNTPE with GA 136
5.3.2 FE-SEM Characterization of BCNTPE and PGAMCNTPE 137
5.3.3 EIS Characterization for PGAMCNTPE and BCNTPE 137
5.3.4 CV Behavior of IT at PGAMCNTPE and BCNTPE 137
5.3.5 Variation of IT Behavior at Different pHs 137
5.3.6 Effect of Voltage Sweep Rate 139
5.3.7 Calibration Curve 140
5.3.8 Reproducible and Stable Sensor 141
5.3.9 Interference Analysis 141
5.3.10 Water Sample Analysis 141
5.4 Conclusion 142
Acknowledgment 143
Important Websites for Reference 143
References 143
6 Toxicity of Carbon Nanomaterials 147

Arpita Adhikari and Joydip Sengupta
6.2 Carbon Nanomaterials 149
6.2.1 Fullerene 149
6.2.2 Carbon Nanotube 149
6.2.3 Graphene and Graphene Derivatives 149
6.3 Nanotoxicology and Resulting Cytotoxicity or Cellular Toxicity 151
6.4 Assessment of Nanocytotoxicity 155
6.4.1 Respiratory or Pulmonary Toxicity 155
6.4.2 Dermal or Skin Toxicity 157
6.4.3 Cardiovascular Toxicity 158
6.4.4 Reproductive and Developmental Toxicity 158
6.4.5 Hepatotoxicity or Liver Toxicity 159
6.4.6 Ocular Toxicity 160
viii Contents
6.5 onclusions 160

C
References 161
7 Fundamentals of Functionalized Carbon Nanomaterials (CNMs)

for Environmental Devices and Techniques 173
Kiran Soni and Rekha Yadav
7.2 Synthesis 174
7.2.1 Carbon Nanotubes 174
7.2.2 Graphene 175
7.2.3 Fullerenes 176
7.2.4 Carbon Nanocones 176
7.2.5 Functionalization of Nanomaterials 176
7.3 Applications 177
7.3.1 Nanowires 177
7.3.1.1 Carbon Nanotube as Environmental Sensor 177
7.3.1.2 Carbon Nanotubes in Wastewater Treatment 178
7.3.1.3 Carbon Nanotubes in Green Nanocomposite Design 179
7.3.1.4 CNT as Biological Sensor 179
7.3.1.5 CNT as Filler 180
7.3.2 Graphene 181
7.3.2.1 Graphene as Environmental Sensors 182
7.3.2.2 Graphene in Wastewater Treatment 183
7.3.2.3 Graphene as Biological Sensors 185
7.3.2.4 Graphene for Removing Organic Pollutants 186
7.3.3 Fullerenes 188
7.3.3.1 Fullerene as Environmental Sensor 188
7.3.3.2 Fullerene in Wastewater Treatment 188
7.3.3.3 Fullerene as Biological Sensor 188
7.3.3.4 Fullerene in Agriculture 189
7.3.4 Carbon Nanocones 189
7.3.4.1 Carbon Nanocones as Environmental Sensors 189
7.4 Conclusion 190
Useful Links 190
References 190
8 Fundamental of Functionalized Carbon Nanomaterials for Environmental

Devices and Techniques 197
Baskaran Ganesh Kumar, P. PonSathieshkumar, and K.S. Prakash
8.2 Results and Discussion 199
8.2.1 What Are Carbon Nanomaterials? 199
8.2.1.1 Fullerene 199
8.2.1.2 Carbon Nanotubes 199
Contents ix
8.2.1.3 Graphene 200

8.2.2 Functionalization of CNMs 200
8.2.2.1 Need for Functionalization 200
8.2.2.2 Covalent Functionalization 201
8.2.2.3 Non-covalent Functionalization 208
8.2.3 CNMs for Environment Devices 209
8.2.3.1 Solar Cell 213
8.2.3.2 Gas Sensors by Functionalized CNMs 214
8.2.3.3 Humidity Sensors by Functionalized CNMs 215
8.2.3.4 LEDs by Functionalized CNMs 215
8.2.3.5 Metal Absorption by Functionalized CNMs 216
8.2.3.6 Water Purification by Functionalized CNMs 217
8.3 Conclusion, Challenges, and Future Prospects 218
Acknowledgments 218
Related Web Links 219
References 219
9 Functionalized Magnetic Carbon Nanomaterials for Environmental

Remediation 227
Ambika and Pradeep Pratap Singh
9.2 Types of Carbon-Based Magnetic Nanocomposites Used in Pollutants
Removal from Environment 228
9.2.1 Carbon Nanotubes Based Magnetic Nanocomposites 228
9.2.2 Graphene and Its Derivative Based Magnetic
Nanocomposites 228
9.2.3 Fullerenes Based Magnetic Nanocomposites 229
9.2.4 Nanodiamond-Filled Magnetic Nanocomposites 229
9.2.5 Graphitic Carbon Nitride Based Magnetic
Nanocomposites 229
9.3 Different Processing Methods for Magnetic Carbon-Based
Nanocomposites 229
9.3.1 Melt Blending 229
9.3.2 Hydrothermal Method 230
9.3.3 Co-Precipitation Method 230
9.3.4 In Situ Polymerization 230
9.3.5 Sol–Gel Method 231
9.4 Applications of Magnetic Carbon-Based Nanocomposites 231
9.4.1 Adsorption of Heavy Metals 231
9.4.2 Adsorption of Organic Dye 234
9.4.3 Other Organic Pollutants 236
9.5 Future Prospects 237
9.6 Conclusions 238
References 238
x Contents
10 Functionalized Carbon Nanotubes for Ammonia Sensors 251

Rakshith K. Srinivasreddy and Ravi-Kumar Kadeppagari
10.2 Ammonia Sensors 251
10.3 Types and Synthesis of Carbon Nanotubes 253
10.4 Carbon Nanotube-Based Ammonia Sensors 254
10.5 Functionalization of Carbon Nanotubes 257
10.6 Functionalized Carbon Nanotubes for Ammonia Sensors 258
10.7 Conclusions and Future Perspectives 259
Acknowledgments 259
Websites 259
References 259
11 Functionalized Carbon Nano Lab-on-a-Chip Devices

for Environment 265
RaviPrakash Magisetty, Naga Srilatha Cheekuramelli, and Radhamanohar Aepuru
11.2 Need for Carbon Nano Lab-on-a-Chip Devices for Environment, and Its
Advancement 266
11.3 Carbon Nano Lab-on-a-Chip Devices for Environment 267
11.3.1 Renewable Energy Applications 267
11.3.2 Agriculture Applications 268
11.3.3 Biomedical Applications 270
11.3.4 Ocean and Atmospheric Applications 274
11.4 Conclusion 278
References 279
12 Functionalized Carbon Nanotubes (FCNTs) as Novel Drug Delivery Systems:

Emergent Perspectives from Applications 283
Shikha Gulati, Sanjay Kumar, Ayush Mongia, Anchita Diwan, and Parinita Singh
12.1 About the Chapter 283
12.3 Carbon Nanotubes (CNTs) 284
12.4 Classification of CNTs 286
12.4.1 Advantages of Carbon Nanotubes (CNTs) 287
12.4.2 Disadvantages of Carbon Nanotubes (CNTs) 287
12.5 Synthetic Methodologies of CNTs 288
12.5.1 Laser Ablation (LA) Method 288
12.5.2 Electric Arc Discharge (EAD) Method 289
12.5.3 Catalytic Chemical Vapor Deposition (CCVD) Method 289
12.5.4 Electrolysis Method 289
12.6 Purification Techniques of CNTs 290
12.6.1 Vacuum Oven Treatment 291
12.6.2 Microwave Treatment 291
Contents xi
12.6.3 Chemical Oxidation 291

12.6.4 Piranha Treatment 291
12.6.5 Annealing 292
12.6.6 Ultrasonication 292
12.6.7 Magnetic Purification 292
12.6.8 Cutting 292
12.6.9 Chromatography 292
12.7 Need of Functionalization of Carbon Nanotubes (CNTs) 293
12.8 Functionalization Strategies of CNTs 293
12.8.1 Covalent Functionalization 293
12.8.2 Non-covalent Functionalization 295
12.9 Advantages of Functionalized Carbon Nanotubes (FCNTs) 296
12.10 Medicinal Applications of Functionalized Carbon
Nanotubes (FCNTs) 296
12.10.1 FCNTs in Drug Delivery 296
12.10.2 FCNTs in Drug Loading 298
12.10.3 FCNTs in Drug Targeting 301
12.10.3.1 Cancer Targeting 301
12.10.3.2 Brain Targeting 302
12.10.3.3 Lymphatic Targeting 302
12.10.3.4 Tuberculosis Targeting 303
12.11 Biocompatibility and Toxicity Considerations of FCNTs 303
Some Important Websites 306
References 306
13 Adsorptive Removal of Fluoride by Carbon Nanomaterials 313

Tanvir Arfin
13.2 Geochemistry of Fluoride 314
13.3 Fluoride in Water 314
13.3.1 Dynamics of Fluoride in Groundwater 315
13.4 Fluoride Solubility and Temperature 316
13.5 Sources of Fluoride in the Environment 316
13.6 Health Effects of Fluoride 316
13.7 Removal Technologies 316
13.8 Classification of Adsorbents 317
13.9 Carbon-Based Adsorbents 317
13.9.1 Carbon Nanomaterials (CNM) 318
13.9.1.1 Carbon Nanotube (CNT) 319
13.9.1.2 Graphene 319
13.10 Conclusion 320
Acknowledgment 321
References 321
xii Contents
14 Functionalized Carbon Nano-Membranes Based Devices for Water

Purification Technology 331
Lindomar Cordeiro A. de Araújo and Luiz Pereira da Costa
14.2 Desalination 333
14.3 Removal of Particles (Ions, Heavy Metals) 335
14.4 Removal of Microorganisms 336
14.5 Final Considerations 339
Websites on the Topic 339
References 339
15 Functionalized Bio-carbon Nanomaterials for Environmental

Utilizations 347
Mahtabin R. Rozbu, Ahmedul Kabir, and Paulraj M. Selvakumar
15.2 Carbon Nanomaterial 349
15.3 Synthesis of Fullerenes 349
15.4 Synthesis of CNTs 350
15.5 Synthesis of Graphenes 350
15.6 Bio-carbon Nanomaterials 351
15.7 Functionalization of Nanom\aterials 351
15.7.1 Importance of Functionalization 352
15.8 Nanocellulose 352
15.8.1 Synthesis of Nanocellulose (NC) 352
15.8.2 Synthesis of CNCs 353
15.8.3 Synthesis of CNFs 353
15.8.4 Synthesis of DCCs 354
15.8.5 Synthesis of BNC 354
15.8.6 Applications 354
15.8.6.1 NC in Purification Technology as Films and Foams 354
15.8.7 NC as Solar Cells 355
15.8.8 NC as Stabilizing Agent 355
15.8.9 NC in Biomedicine 355
15.9 Nitrogen and Sulfur Co-doped Bio-carbon 356
15.9.1 Application Co-doped Bio-carbon 356
15.10 Biochar 356
15.10.1 Application of Biochar 357
15.10.1.1 Application of Bio-carbon Derived from Sisal Leaves 357
15.11 Biopolymers 357
15.11.1 Biopolymers in “Green” Synthesis of Nanoparticles 357
15.11.2 Biopolymers in Waste Water Treatments 358
15.11.3 Biopolymers as Bioplastics 358
15.11.4 Nanocomposites 358
15.11.5 Peptide Nanoparticles 359
15.11.5.1 Dipeptides 359
Contents xiii
15.11.5.2 Peptide Amphiphiles 359

15.11.5.3 Dendrimers 360
15.11.5.4 Coiled-Coil Peptides 360
15.11.5.5 Peptide–Nucleic Acid Complexes 360
15.11.5.6 Casein Micelles 360
15.11.5.7 Peptide Nanotubes 360
15.11.6 Further Application of Bio-carbon Nanomaterials as Devices 361
15.11.7 Characterization Technique 361
15.12 Conclusion 362
References 363
16 Carbon-Based Nanomaterials in Drug Delivery Systems 375

Subhendu Chakroborty and Suban K. Sahoo
16.2 Carbon Nanomaterials in Drug Delivery 375
16.2.1 Carbon Nanotubes (CNTs) in Drug Delivery 375
16.2.2 Graphene Oxide (GO) in Drug Delivery 379
16.2.3 Carbon Dots (CDs) in Drug Delivery 384
16.2.4 Nanodiamonds (NDs) in Drug Delivery 387
16.3 Conclusions 389
Important Websites on Drug Delivery Systems 389
References 389
17 Functionalized Carbon Nanomaterials (FCNMs): A Green and Sustainable

Vision 395
Upasana Issar and Richa Arora
17.2 Environment-Friendly and Greener Ways to Synthesize FCNMs 396
17.3 Applications of FCNMs for a Green and Sustainable Environment 398
17.3.1 FCNMs in Wastewater Remediation 398
17.3.2 FCNMs in Air Pollution Remediation 400
17.3.3 FCNMs in Nuclear Waste Management 401
17.3.4 FCNMs as Electrocatalysts and Photocatalysts 402
17.3.5 FCNMs for Energy Storage 403
17.3.5.1 FCNMs and Solar Cells 403
17.3.5.2 FCNMs and Supercapacitors 405
17.3.5.3 FCNMs and Hydrogen Storage 406
17.3.5.4 FCNMs and Fuel Cell 407
17.3.6 FCNMs and Biofuels 408
17.3.7 FCNMs as Nanofertilizers 409
17.3.8 Miscellaneous Applications 409
17.4 Summary 410
Some Important Weblinks Related to Applications of FCNMs 410
References 410
xiv Contents
18 Functionalized Carbon Nanomaterials for Impending Pharmaceutical

Applications: A Green and Sustainable Vision 423
Vaneet Kumar, Saruchi, and Harsh Kumar
18.2 Carbon Nanotubes: Functionalization for Biomedical Applications 424
18.2.1 Applications of Functionalization Carbon Nanotubes in the Pharmaceutical
Field 426
18.2.2 Treatments of Tumors by Functionalized CNT 428
18.2.3 Treatment of Infectious Diseases by Functionalized CNT 428
18.2.4 Functionalized CNT as Antioxidants 429
18.2.5 Functionalized CNTs as Diagnostics 429
18.2.6 Solid Phase Extraction of Drugs and Biochemical’s with CNTs 430
18.2.7 Toxicity Contemplation of CNTs 431
18.3 Conclusion and Future Perspectives 432
Important Websites about the Topic 433
References 433
Index 439
1
Graphene-Based Nanomembranes for Sustainable Water

Purification Applications
Uluvangada T. Uthappa1, Dusan Losic2,3, and Mahaveer D. Kurkuri1
1
JAIN University, Centre for Nano and Material Sciences, JAIN Global Campus, Bengaluru, Karnataka, 562112, India
2
The University of Adelaide, School of Chemical Engineering, Adelaide, SA, 5005, Australia
3
The University of Adelaide, ARC Research Hub for Graphene Enabled Industry Transformation, Adelaide, SA, 5005, Australia
1.1 Introduction
The global crisis on water scarcity ranks top among the world’s major problems. Provided
with recent statistics, two-thirds of the world population will face major difficulties by 2025
due to the lack of water facilities. Due to the rapid population expansion, industrial devel-
opment, and water pollution, it incessantly depleted freshwater resources. The extreme
consumption of freshwater resources, particularly for developing countries, due to the
growth of agriculture and industrial activities completely dependent on water resources
and continuous utilization leads to severe ecological disasters. Thus, the shortage of water
resources is an alarming issue that needs urgent resolution. To address these problems, it is
crucial to conserve water resources [1].
On the other hand, membrane technology is a separation process that permeates certain
species to pass via membrane while controlling the others, which is completely dependent
on the properties of the membrane material. Based on their properties, membranes can be
categorized as dense and porous membranes according to the driving force and ionic and
molecular movement transported through membranes. Usually, it is well recognized that
diverse species permeate based on the specific diffusion rates via the membranes, which
are generally influenced based on solubility, diffusivity, and the membranes’ porosity, as
represented in Figure 1.1.
It is believed that the smaller molecules might pass through the membrane and whereas
others could be blocked based on the pore sizes of the membranes. The ceramic and poly-
mers are the most widely used membranes for water purifications plants. Typically, ceramic
membranes retain better thermal and mechanical properties. However, it is difficult to con-
trol the pore size accurately with low-cost approaches. In contrast, polymeric membranes
are economically and extensively utilized in microfiltration (MF), ultrafiltration (UF), nano-
filtration (NF), and reverse osmosis (RO) process due to the rapid permeation and high
Environmental Applications of Carbon Nanomaterials-Based Devices, First Edition.

Edited by Shadpour Mallakpour and Chaudhery Mustansar Hussain.
© 2022 WILEY-VCH GmbH. Published 2022 by WILEY-VCH GmbH.
2 1 Graphene-Based Nanomembranes for Sustainable Water Purification Applications
(a) (b)
Figure 1.1 Transport mechanism for dense (a) and porous membrane (b). Source: Lyu et al. [2].
© 2018 Royal Society of Chemistry.
selectivity. However, polymers are hydrophobic that can easily adsorb target pollutants that
lead to membrane fouling. Compared to ceramic and polymeric membranes, the new aston-
ishing classic example used in membrane technology is recently discovered graphene oxide
(GO). Also, reduced graphene oxide (rGO) is an important alternative class that belongs to
the graphene derivative that has been explored for the development of a new generation of
membrane separation technology [2]. Since from past few years’ research expansion in gra-
phene known as two-dimensional (2D) carbon allotrope and their oxidized derivatives (GO)
has rapidly developed by the drastic increase in publications and patents. It is important to
mention that graphene and GO have distinctive favorable material advantages compared
to carbon nanotubes (CNTs) concerning separation and purification technologies. GO can
be easily fabricated and engineered with favorable size, surface chemistry/modification, and
structural properties. Moreover, its industrial process consumes a lesser amount of energy,
making their production cost economic (for example: 500–1000 MJ/kg by solvent exfoliation
of graphite or chemical reduction of GO, when compared to CNTs 100 000 MJ/kg) [3].
This chapter summarizes the very recent advances on graphene-based nanomembranes
for water purifications. The properties of GO-based membranes and fabrication strategies
of various graphene-based nanomembranes and their applications in desalination and
dyes and some highlights on heavy metals treatment are elucidated and discussed. Finally,
a conclusion and future perspectives have been provided. This current book chapter could
help the researchers and experts in membrane technology working on GO-based nanomem-
branes for water treatment applications.
1.2 Graphene and GO-Based Membrane Characteristics

and Properties
For the first time, graphene was witnessed in electron microscopes in 1962 supported on
the metal surfaces. Further, it was again rediscovered in 2004 by Novoselov and Geim and
awarded Nobel Prize in Physics 2010 due to their groundbreaking experiments on 2D
1.2 Graphene and GO-Based Membrane Characteristics and Propertie 3
material graphene. Since 2010, graphene has fascinated major attractions in several
applications, including water purification. Graphene contains carbon atoms bonded to
each other in hexagonal patterns. The monolayered and double-layered graphene is very
thin, and so it can be regarded as 2D material. Graphene’s flat based honeycomb arrange-
ments are responsible for favorable characteristic features such as strongest, lightest, most
conductive, transparent materials [4], high specific surface area (2600 m2/g), flexibility
[5, 6], and large scale production from cheap raw material (graphite) [7]. GO is an oxidized
form of graphene, made up of carbon atoms bonded in hexagonal honeycomb lattice struc-
tures. Based on strong oxidations surrounding environment and based on the synthetic
protocol such as Hummers or Staudenmaier method, enormous groups of oxygen epoxide,
hydroxyl, and carboxyl acid functional groups present in GO are represented in Figure 1.2.
Such diverse functional groups are responsible for better hydrophilicity and permit better
dispersion of GO flakes in aqueous media. These substantial features significantly enable
GO deposition from solution using water as an environmentally benign solvent. From the
past few years, GO showed unlimited attention as a novel 2D membrane in water treatment
applications due to its exceptional mechanical [8] and antifouling properties [9], atomically
thin thickness, and outstanding dispersion in water [8]. Various composite membranes are
obtained by mixing GO with different polymers and other surface enriched materials. Such
studies have been carried to enhance surface properties such as conductivity, tensile
strength, and or elasticity of materials [4]. These surface properties impart GO-based func-
tionalized nanomembranes for advanced water treatment technologies. The selective per-
meation path of graphene-based membranes that allow separation via the nanopore
structure originated within the basal plane of hexagonal crystalline structures.
O O
O
HO
O
OH OH
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O
O O
O
HO
O O O O
H H
Figure 1.2 Typical chemical structure of GO showing graphene sheet derivatized by phenyl
epoxide, hydroxyl groups on the basal plane, and carboxylic group on the edge.
Size exclusion Electrostatic interactions
(a)
Size exclusion Electrostatic interactions
Ion adsorption
Electrostatic binding
Ions Cation-π
Metal coordination
(b) Water
Figure 1.3 Selective permeation routes in nanoporous graphene and stacked sheets of
GO. (a) Nanoporous graphene membrane and (b) stacked graphene oxide membrane.
Source: Dervin et al. [9]. © 2016 Royal Society of Chemistry.
On the other hand, ions or molecules are selectively transported or passed via interlayer
spacing of 2D graphene-based materials. The stacked nanosheets of GO form a multilayer
laminate that shows abundant mechanical strength for application in pressure-assisted
water filtration due to strong hydrogen bonds among distinct sheets. The oxygen compris-
ing functional groups deposited haphazardly beside the edges of GO sheets, which main-
tain both significant interlayer spacing between and empty spaces among non-oxidized
areas, constituting a network of nanocapillaries within the film. These nanochannels allow
penetration of water molecules and successive transport laterally on hydrophobic non-
oxidized regions of membranes that could support the rapid flow of water molecules. Thus
liquid, vapors, and gases are opposed, as shown in Figure 1.3. In addition, water-soluble
oxygen functional groups present beside the GO sheets, which adsorb water molecules and
further diffused between the non-polar hydrocarbon present on the backbone of GO. Such
permeation of water escalates the interlayer spacing in the middle of stacked GO sheets
and helps in water flux over nanochannels at a higher flow rate. It has also been recognized
that smaller ions enter GO membranes considerably superior to simple diffusion.
Conversely, enlargement of nanochannels during the hydrated state only accepts ions of
analogous sizes [9].
1.3 Fabrication of Graphene-Based Nanomembranes

for Water Treatment Applications
1.3.1 Desalination
The membrane-based desalination method is classified based on membrane pore size and
rejection mechanisms [10]. Desalination is a process of removing salts from seawater or
1.3 Fabrication of Graphene-Based Nanomembranes for Water Treatment Application 5
brackish water, and it is known to be the core technology for improving freshwater scarcity
[11]. To improve the desalination process and enhance water treatments, innovative tech-
nological classes of membrane systems are advanced. However, to overcome the costs and
energy demands accompanied by membrane treatment, advanced, innovative, and
economical membranes are highly desirable [9].
1.3.2 Treatment for Dyes

Many dyes are used to color the products from various industries such as food, paints,
leather, plastics, and textiles. The significant amount of effluents from those industries cre-
ates serious ecological complications to the environment for most of the underground and
surface water bodies. Moreover, dye waste turbidity results in blocking sunlight and reduc-
ing diffusion into the water that could obstruct the biological process. As far as concerned,
organic dyes are highly stable, toxic, carcinogenic, and mutagenic. In some cases, these
properties lead to organ damage and abnormalities in living creatures. As a result, it is
crucial to treat or remove such dyes before discharging them into environments [12].
1.3.3 Graphene Nanomembranes for Salt and Dye Rejection

In this report, charged nanochannels produced in polyelectrolyte intercalated amine
reduced graphene oxide membranes (PE-ArGO membrane) were reported. The overall syn-
thetic process is shown in Figure 1.4. The PE-ArGO membrane with a rejection sheet of
around 160 nm in thickness with laminate structural topographies with a smooth top sur-
face of low roughness of around 17.2 nm. The PE-ArGO membrane was in situ modified
SOCI2 PAH
EDA
1 2 3
Wash Wash
EDA PAH PAH@ArGO

GO
Oxygen PSS PSS@GO
Figure 1.4 Schematic showing synthetic for PE-ArGO membrane. Source: Song et al. [13]. © 2017
American Chemical Society.
(m-PE-ArGO) using free chlorine scavenging to adjust the charge, though keeping modifi-
cation to the layered structure in a nominal way. The PE-ArGO and m-PE-ArGO mem-
brane surface charge were +4.37 and −4.28 mC/m2. Using the pressure-assisted technique,
pure water permeability for PE@ArGO and m-PE@ArGO membrane was 2.8 and
10.8 LM2/h/bar. The salt rejection is extremely dependent on the charge density of mem-
branes, valence of co-ions, and size of hydrated ions. The rejection of slats for positively
charged PE-ArGO membrane follows in the order of: R (MgCl2), 93% > R (NaCl), 88% = R
(MgSO4), 88% > R (Na2SO4), 65%, whereas R (Na2SO4), 90% > R (NaCl), 85% > R (MgSO4),
68% > R (MgCl2), 42% followed trend for negatively charged m-PE-ArGO membranes.
Altogether, this is the first report on high density positive/negative charge gated ion trans-
port behavior studies reported in GO-based membranes [13].
Stationary repulsion force and π–π contact among GO nanosheets have been tuned using
interlayer functionalization and external treatment. Negatively charged congo red (CR) dye
with π orbital adsorbed on the nonoxide domain of GO nanosheets, interlayers cross-linked
by Ca2+ ions via chelating reaction. The GO–CR nanosheets π–π stacking interactions
altered by thermal reduction of GO/Ca/CR membrane using the hot pressing method. The
interlayer spacing of GO/Ca/CR membranes tuned from 3.20 to 5.7 Å under dry conditions
is observed. In wet conditions, 7.7–11 Å. In the meantime, modified GO membranes’ swell-
ing behavior decreased compared to the bare GO bare membrane. Notably, the prepared
membrane showed a permeation flux of 17 LM2/h/bar, and the rejection for methylene
blue (MB) was 99.5% [14].
Wang et al. demonstrated exfoliated hydrotalcite/graphene oxide (EHT/GO) nanosheet
combined through flocculation deposition and homogeneously dispersed in polyethyle-
neimine (PEI) solution used as an aqueous phase for interfacial polymerization. An over-
view of the synthetic process is shown in Figure 1.5. The prepared hybrid membranes
EHT/GO displayed improved positively charged property after integrating EHT/GO into
polyamide (PA) membrane compared with pristine NF and GO incorporated NF mem-
brane. EHT/GO exhibited a more promising transport channel of water molecules
Mixture
Exfoliation Flocculation
NO3–-HT Exfoliated HT Exfoliated GO EHT/GO
Immersion Crosslinking
Aqueous Organic
phase phase
Heat treatment
Figure 1.5 Overview of the synthetic process of EHT/GO hybrid nanosheets and nanofiltration
membranes. Source: Wang et al. [15]. © 2019 Elsevier.
resulting in improved water flux of 26 LM2/h/bar at 0.8 MPa. To this, the membrane rejec-
tion performances were 97% and 32% for 1000 ppm of Mg2Cl2 and Na2SO4 feed solutions,
presenting prospective use in hard water softening applications [15].
The high rejection of organic dyes graphene oxide/attapulgite (GO/APT) composite
nanofiltration membrane was developed using the vacuum-assisted filtration method. The
composite membrane was fabricated by a meticulous assembly of APT nanorods incorpo-
rated into the interlayers of GO nanosheets. The APT nanorods are easily intercalated into
the stacked GO lamellar layers to form stable C─O─Si bonds undergoing 3D network lami-
nate assembly through the surface grafting functionalization. It showed a significant role
in enhanced performance in water permeability. Compared with the bare GO membrane,
the GO/APT membrane showed fourfold water flux performance while maintaining a high
rejection rate of almost 100% for rhodamine b (RhB) dye molecules. The reason could be
due to d-spacing, hydrophilicity, and 3D network lamellar structural properties. The sepa-
ration mechanism was also evaluated for the GO/APT membrane with different positively/
negatively charged and neutral dyes. Based on the size exclusion and electrostatic interac-
tions, selective permeation could be done using GO/APT membranes [16]. An overview of
the synthetic process is shown in Figure 1.6.
Thin-film nanocomposite (TFN) acts as an ideal platform to enhance water permeability
of commercially available PA membranes in RO desalination. Thus, nitrogen-doped gra-
phene oxide quantum dots (N-GOQD) fabricated PA/N-GOQD TFN membranes by inter-
facial polymerization for RO desalination applications. It is noteworthy to mention after
the addition of 0.02 wt/v% N-GOQD into the PA membrane, there was a sudden enhance-
ment of water permeability by almost three times, retaining identical salt rejection of pris-
tine PA membrane. Improved water permeability leads to enhanced hydrophilicity of the
OH OH OH
OH OH OH
PC filter
APT Ultrasonication, Vacuum
mixed, stirred filtration
COOH
COOH
O
C O
OH OH
GO GO/APT suspension
COOH
OH OH
HO O
O OH
O COOH O O
O
O O
O O O O COOH
O HO
C O
HO COOH OH COOH GO/APT

membrane
Figure 1.6 Synthetic process for GO/APT nanocomposite membrane. Source: Wang et al. [16].
© 2019 Elsevier.
membrane surface, enhanced actual membrane surface area, and a large cavity at the inter-
face between N-GOQD and PA matrix [17].
Cheng et al. fabricated reduced graphene oxide-gold nanoparticle (rGO-AuNP) mem-
brane by vacuum filtration for wastewater dye treatment applications. Using the TEM tech-
nique, the size of AuNPs on the rGO surface measured about 8–10 nm in size. The layer by
layer (LBL) stacking of rGO-AuNP showed a high flux of 204 LM2/h/bar and retention of
99% for RhB dye molecules [18].
GO membranes are recognized as potential candidates in separation technology.
Nonetheless, their instability in aqueous environments is the drawback in real-time appli-
cations. Ma et al. designed facile eco-friendly intercalation of montmorillonite (MMT)
nano patches on GO to form stable membranes, addressing such complications. The devel-
oped stable membranes showed a high water flux of 139.5 LM2/h/bar under 0.01 MPa.
Further, for various organic dye molecules such as congo red (CR), RhB, crystal violet (CV),
methylene blue (MB) showed 98.75%, 99.44%, 99.90%, and 99.94% respectively [19].
In this study, carboxylation of GO nanosheets was carried out through a series of multiple
oxidation methods and nucleophilic substitution reactions. Graphene acidic (GA) membrane
fabricated using carboxylation of GO nanosheets through the multiple oxidation process. The
developed GA membranes showed high water permeability and enhanced salt rejections
when associated with bare GO and modified GO membranes with surface negative charge
and hydrophilicity. GA membrane showed pure water flux of 73.5 LM2/h/bar and peak rejec-
tion of 64% and 95% for 2000 mg/l NaCl and Na2SO4 feed solutions at 1.5 MPa [20].
In an aqueous solution in the absence of organic solvents GO, rGO, and graphene oxide/
polyacrylamide (GO/PAM), nanofiltration membranes are prepared using vacuum filtra-
tion. The hydrophilicity of such developed graphene-based membranes was analyzed using
contact angle measurements by using X-ray diffraction interlayer spacing of various mem-
branes such as GO (0.85 nm), GO/PAM (0.68 nm), and rGO (0.36 nm). The performance
studies of all these graphene-based membranes were carried out using dead-end filtration
mode. The water flux and retention for RhB dye showed 399 LM2/h/bar, 85% for GO and
188.89 LM2/h/bar, 95.43% for GO/PAM and 85.85 LM2/h/bar, 97% for rGO membranes. The
GO/PAM membranes showed the best separation performance due to the actual fine-tuning
of interlayer spacing. These could be potential membranes for high performance in water
purification applications [21].
To address global water issues, forward osmosis (FO) based water treatment showed an
immense impact. However, it has some limitations in practical application, like the lack of
FO membranes with high permeability and selectivity. The novel reduced GO/CNT hollow
fiber through electrophoretic deposition coupling with chemical reduction process with
high FO performances was evaluated. Two main factors were noted. One is due to the ultra-
low friction, and distinct interlayer spacing of rGO showed higher water permeability and
selectivity. The second factor is high porosity, and improved wettability warranted the CNT
hollow fiber with low internal concentration polarization ensured and enhanced water
flux. Using deionized water feed at a 0.5 M NaCl draw solution (DS), reduced GO/CNT
showed exceptional water flux of 22.6 LMH, indicating 3.3 times greater than the commer-
cial membrane. In the meantime, its reverse salt flux displayed only 1.6 gMH compared to
2.2 gMH for commercial membrane. The obtained results suggest that the rGO/CNT mem-
brane could be a substituent for clean water supply in the FO process [22].
Cellulose acetate (CA)/GO nanocomposites were fabricated for seawater desalination

using the phase inversion method. GO nanosheets with grain size 2.7 nm were added to the
CA matrix and casting CA/GO onto polyester fabric to enact asymmetric CA (RO) mem-
branes to enhance thermal and mechanical stability. Further, the addition of GO into the
CA matrix altered the porosity structure. Meanwhile, synthetic seawater rejection of CA
membrane modified with 1 wt% GO showed almost 90% (80% more salt rejection of bare
CA membrane) for 25 000 ppm NaCl at 25 bar, which is 1.8 more when compared to bare
CA membrane. Also, the flux of the CA membrane showed minor reduction (30% decrease)
in the presence of 1 wt% GO showing prospective in seawater desalination [23].
Kang et al. developed graphene oxide-oxidized carbon nanotubes-layer by layer assembly
(GO-OCNTs-LBL) with different bilayers on polyethersulfone (PES) membranes. The
insertion of OCNTs on the GO interlayer for GO-OCNTs-LBL membrane controls the
enlargement of GO. Few other studies were inspected using various salts such as NaCl,
MgCl2, Na2SO4, sucrose as DSs, and deionized water as feed. GO-OCNTs-LBL membranes
showed high water flux than GO-LBL (control) for NaCl, MgCl2, Na2SO4, and sucrose as
DS. The solute flux of GO-OCNTs-LBL membrane for NaCl decreased by 70% than that of
GO-LBL membrane. Consequently, the GO-OCNTs-LBL membrane showed superior
rejection performances for NaCl than the GO-LBL membrane alone [24].
A polydopamine (PDA) functionalized reduced graphene oxide-metal organic frame-
works (rGO-MOFs-HKUST-1) nanocomposites were developed with expeditious rejection
capacity for organic dye. In this work, MOFs-HKUST-1 based on rGO was functionalized
with PDA. These PDA-rGO-MOFs-HKUST-1 nanocomposites formed on the surface of
commercially available CA membrane. The addition of HKUST-1 and cross-linking func-
tionalization of PDA showed excellent rejection, flux, hydrophilic, and antifouling perfor-
mances. The prepared nanocomposite membrane (PDA-rGO-MOFs-HKUST-1) could
successfully reject methylene blue (99.8%) and congo red (CR) 89% efficiently. Further, it is
important to note that the flux of the PDA-rGO-MOFs-HKUST-1 membrane showed a
drastic increase of 31-fold due to HKUST-1 and PDA [25]. The schematic showing mecha-
nisms involved in PDA-rGO-MOFs-HKUST nanocomposites shown in Figure 1.7.
PDA
HKUST-1
Methylene blue
Congo red
H2O
Figure 1.7 Schematic showing mechanisms involved in PDA-rGO-MOFs-HKUST nanocomposites.

Source: Liu et al. [25]. © 2019 Elsevier.
Assembly
GO ATP
Figure 1.8 Schematic self-assembly of GO/ATP membranes. Source: Luo et al. [26]. © 2019 Elsevier.
Lee et al. effectively surface-functionalized EDTA-rGO membranes for nanofiltration.

The EDTA-rGO membranes’ surface was eventually treated with oxygen plasma to boost its
water permeability and denoted (P-EDTA-rGO). The P-EDTA-rGO showed 80% of rejection
for NaCl salt and water permeance of 150 LM2/h/bar, showing 15 times greater than before
plasma surface treatment. The developed P-EDTA-rGO nanofiltration membrane caused
high rejection rates. Permeabilities of the small interlayer spacing (5.7 Å) is due to EDTA
functionalization and improved hydrophilicity from enhanced plasma treatment [25].
In this work, the attapulgite (ATP) nanofibers/GO composite membrane is self-assem-
bled by mixed solutions containing both ATP and GO shown in Figure 1.8. ATP nanofibers
intercalated on GO nanosheets interlayers, acting as laminate structures for effectual trails
for water molecules GO. Besides, ATP nanofibers able to widen mass transfer channels and
able to promote hydration capacity. The permeate flux from 28.64 LM2/h/bar for GO mem-
branes (control) to 221 LM2/h/bar for ATP/GO membranes was observed and showed
extraordinary rejection rates for organic dye molecules such as CBB R250 99.88% and
99.93% for TMPyP [26].
In membrane studies, particularly in water treatment, stability is one of the major prob-
lems. In this work, Fang et al. constructed a highly water stable GO-based metal-organic
framework (MOF) (UiO66) composite membrane was designed. The construction of sub-
strate involves two main steps: (i) doping GO nanosheets into the membrane casting solu-
tion comprising polyacrylonitrile (PAN) that forms 2D–3D inter-connecting pores by phase
inversion mode designated as GO-PAN, and (ii) immersing GO-PAN into dopamine solu-
tion, which undergoes self-polymerization undergoes to form better compatible and flexi-
ble substrate denoted as PGP. The UiO66 layer was assembled by vacuum-assisted filtration
technique on porous PGP support illustrated in Figure 1.9. The stable GO-based UiO66/
PAN, known as thin-film composite membrane, showed higher water flux 31.33 LM2/h/bar
and maintaining an effective rejection rate of >94% for various dyes such as congo red,
methyl orange (MO), methylene blue, and RhB [27].
In other work, the graphene oxide framework (GOF) was designed via “from” and “to”
cross-linking approaches. GOF with compact nanochannels were fabricated by LBL using
branched polyethyleneimine (BPEI), GO, and thiourea particles as the well-defined
PAN GO
Phase inversion
Casting solution GP substrate
CuSO4/H2O2 PDA self-

induced polymerization
Vacuum filtration
UiO-66/PGP TFC PGP support layer

membrane
Figure 1.9 Overview process involved in the UiO66/PGP-TFC NF membrane process. Source: Fang
et al. [27]. © 2020 Elsevier.
building blocks. The surface morphology of BPEI/GO/thiourea membranes revealed with

compact GOF arrangement with very narrow interlamellar spacing (0.49 nm) when
matched to BPEI/GO membranes (0.52 nm). Structural interpretation revealed thiourea
partially reduced GO molecules mediated as “to” cross-linker linking adjacent GO
nanosheets. While the GO deposition BPEI accomplished as “from” cross-linker by binding
thiourea linked GO laminates to form highly stable membranes. The GOF membrane per-
formances showed rejection of 99.5% for both anionic and cationic dyes like methyl orange
and RhB. The BPEI/GO/thiourea membrane synthesized with 12 bilayers using 0.25 mg/
ml of GO concentrations showed pure water flux of 24 LM2/h/bar and Na2SO4 rejection of
94%, showing permeability 2.5 times when compared with commercially available nanofil-
tration membrane. More importantly, BPEI/GO/thiourea showed excellent stability in
both acid and basic aqueous solutions [28].
A 3D graphene oxide hydrogel membranes (GOHMs) designed by gelation of GO with
ferrous ions through vacuum aided filtration and their application shown in Figure 1.10. In
this work, ferrous ions assisted as cross-linkers, which enhanced bonding strength between
Ferrous ions Methylene blue

Congo red Silver nanoparticle
Vacuum filtration Adsorption Electrostatic repulsion Physical screening
Figure 1.10 Schematic of GOHMs membrane preparation and retention mechanisms of target
pollutants. Source: Chen et al. [29]. © 2019 Royal Society of Chemistry.
DPA
Ultrasound
ChNCs D-ChNCs
Graphene oxide
D-ChNCs/GO
Vacuum dispersion
filtration
D-ChNCs/GO
membrane
Figure 1.11 Schematic illustration of D-ChNCs and D-ChNCs/GO composite membranes.

Source: Ou et al. [30]. © 2019 American Chemical Society.
GO nanosheets to prompt microstructure formation of GO via cation π interactions to form

3D lamellar porous structures. In contrast, with pristine GO membranes, the GOHMs
exhibited superior water stability and enhanced water permeability of 111 LM2/h/bar and
retention performances of >99% for methylene blue and congo red dyes [29].
In this work, free-standing chitin nanocrystals (ChNCs) was modified by dopamine (D)
to form GO composites and labeled as D-ChNCs-GO, and their schematic is shown in
Figure 1.11. The hydrophilicity is purely based on the contents of D-ChNCs that displays a
very sharp increase in water flux from 8.8 for bare GO to 135.6 LM2/h/bar for D-ChNCs-GO
composite membranes. Additionally, the rejection rates for methylene blue and congo red
dye showed 99.3% and 98.3% of removal performances [30].
Januario et al. modified the PES microfiltration membrane with sulfuric acid, titanium
dioxide (TiO2), and GO solutions using the LBL self-assembly method through an electro-
static interactions pressure-driven filtration system. The separation performances of the
designed membrane for various charged dye molecules were twilight yellow (TY) (69.98%),
red bordeaux (BR) (93%), and safranin orange (SO) (100%) based on several factors such as
size exclusion, electrostatic repulsion, and adsorptive processes [31].
The graphene oxide/MIL-88A(Fe) (GO/M88A) membrane was fabricated using the vac-
uum filtration method. The intercalation of M88A on graphene nanosheets showed
enhanced separation performances. The designed membrane was utilized for the photo-
Fenton degradation process showing 99.81% separation efficiency for methylene blue (MB)
dye with enhanced 26.3 LM2/h/bar of flux rate [32].
In this report, a nominal strategy was adapted to design graphene oxide-methylene blue
(GO/MB) membrane composites. GO was surface modified by MB through electrostatic
interactions and π–π conjugation systems. The rejection study for GO/MB membrane for
various dyes (methyl orange, disperse black9, and RhB showed 93%, 99.85%, and 82.56% of
rejections, and pure water flux was 7.67 LM2/h/bar [33].
The GO with the 2D lamellar arrangement and single-atom thickness showed several
benefits in water treatment applications assembled with the continuous membrane.
Nevertheless, a suitable process to advance the improved separation property of GO mem-
brane is highly imperative. Also, damage to the membrane during the large-scale applica-
tion route, which results in a significant loss, are the main drawbacks that to be addressed.
In this work, a hierarchically self-assembled GO hybrid membrane was designed to achieve
superior efficiency in the water purification process and self-healing property, which leads
to the synergetic effect of MOF and hydrophilic coating of chitosan biopolymer.
Intercalated MOF effectually extended the available channel space of GO and capable of
molecule sieving properties. In the meantime, the chitosan-coated layer could particularly
adsorb water molecules and attain self-healing via cross-linking reaction. Developed GO
hybrid membrane showed enhanced water flux 14.62 LM2/h/bar, showing an effective
344% improvement when compared with water flux of GO alone. Meanwhile, the GO
hybrid membrane was able to show a rejection rate of >99% for methylene blue (MB),
methyl orange (MO), acid orange (AO), and direct red 80 (DR) dyes. The damaged GO
hybrid membranes can also recover their original water purification 95% for water flux and
99% of rejection ratios [34]. The schematic process of MOF–GO–CS composite membranes
used for the water purification process is shown in Figure 1.12.
Due to the extraordinary permeance of GO, it has an inherent application in membrane
separation. Fang et al. designed rGO by green hydrothermal reduction method. Further,
the rGO membrane was synthesized on polyvinylidene fluoride (PVDF) supporting mem-
branes by vacuum-assisted filtration. At this point, the interlayer structure of GO and the
permeability of rGO membranes can be fine-tuned by altering the reduction degree of GO
via altering the hydrothermal reaction time. Due to the defects of rGO nanosheets, less
oxygen-bearing functional groups and improved hydrophobicity enable transport of water
molecular in relatively smaller interlayer space due to hydrothermal reduction. In contrast,
with the bare GO membrane, the hydrothermal reduced rGO membrane revealed excellent
permeability with a rejection ratio of 99% for methyl blue, congo red, and crystal violet
dyes [35].
Li et al. have designed polysulfone grafted graphene oxide nanosheets (GO-g-PSf)
through nucleophilic substitution reaction between hydroxyl groups present in GO and
chloromethyl groups of chloromethylated polysulfone (CMPSf). The GO-g-PSf dispersion
in N-methyl pyrrolidone (NMP) is used to produce via vacuum filtration using PA
Damaged Self-healed
H2O Dye Chitosan GO MOF
Figure 1.12 Schematic process of MOF-GO-CS composite membranes used for water purification
process. Source: Chang et al. [34]. © 2019 American Chemical Society.
composite membrane as supports. GO-g-PSf hybrid membrane with a deposition rate of

31.8 μg/cm2 showed superior water flux of 88 LM2/h than pristine GO composite mem-
brane 12.8 LM2/h at 2 bar the enlarged interlayer spacing among the developed GO-g-PSf
nanosheets. The rejection rate of GO-g-PSf membranes displayed 90% for acid black 1,
99.5% for congo red, and 99.8% for methylene blue dyes under cross-flow process at 2 bar.
Notably, the water permeance of GO-g-PSf membrane endured at 25.9 LM2/h after 60 hours
of operation process for congo red separation. It is also worth noting that GO-g-PSf mem-
brane showed enhanced structural stability after two hours of ultrasonic irradiation due to
the physical enlargement of PSf chains [36]. The preparation strategies involved for GO-g-
PSf and their chemical reaction showed in Figure 1.13.
A covalent organic framework-1 (COF-1) with systematically arranged structure and
controlled pore size was covalently functionalized on the GO surface through in situ mode
and schematically shown in Figure 1.14. The fabricated GO/COF-1 nanocomposites
enhanced the dispersivity and stability in water over COF-1, permitting GO/COF-1 nano-
composites in water purification applications. The nanocomposites assembled on the PAN
support to form ultrafiltration nanomembranes through dead-end filtration mode. The
enhanced water permeation of 310 LM2/h and high rejection rates for various dyes such as
congo red, direct red 23, and methylene blue showing >99% of rejection rate and superior
permeability for ion salts, were observed [37].
A nano graphene oxide particles (NGO), by the aid of multi-scale arrangement, were
designed. In this work, divalent metal cations (Ca2+, Cu2+, and Mg2+) engaged as cross-
linking agents in order to stack nano NGO particles on both surface and pore channels of
CH3 O
* O C O S *
n HO
CH3 O COOH
Si(CH3)3CI O
PSF
(CH2O)3 O
SnCI4
CH3 O OH
* O C O S *
n
CH3 O O
CH2CI
CMPSf COOH GO
K2CO3
CH3 O
* O C O S *
n
CH3 O
CH2
O
COOH
O
O
OH
GO-g-PSf COOH
Figure 1.13 Preparation strategies involved for GO-g-PSf. Source: Li et al. [36]. © 2020 Elsevier.
N2
Drying
GO/COF-1 Dead-end filtration device
Polymer substrate GO/COF-1 GO/COF-1 substrate

dispersion
substrate
Figure 1.14 Schematic overview of GO/COF-1 membrane fabrication. Source: Zhang et al. [37].
© 2019 Elsevier.
poly(p-phenylene sulfide) (PPS) formed over electrostatic and coordination bonds. Metal
NGO frameworks presented identical MOFs structure with nanoscale openings, and Metal-
NGO/PSS membranes displayed outstanding water permeability and superior dye rejec-
tions. Compared with the transversal interlayer molecular transport chamber present in
existing GO membranes, Metal-NGO/PSS membranes exhibited condensed permeable
channel, maximum pore opening attaining designed membrane with rapid water molecu-
lar transport rate and superior pure water flux of 3109 LMH/MPa. Also, the Metal-NGO/
PSS membranes showed a high rejection rate >98% for various dyes [38].
In another work, hybrid nanosheets were obtained by grafting GO and covalent organic
frameworks (COFs) and organized building blocks. The covalent triazine framework
(CTF) COFs exfoliated into nanosheets and reacted with GO to form GO-CTF hybrid
nanosheets. The addition of CTF helps to change the interlayer distance between GO-CTF
nanomembranes exhibiting high rejection for organic dyes >90%. Additionally, GO-CTF
membranes showed a water flux of 226 LM2/h, which is more than 12-fold higher than
pristine GO membranes. Besides, chemical bonds between GO and COFs showed
enhanced stability [39].
Multifunctional thin-film nanocomposites (MTFNs) nanofiltration membrane is
designed using the combination of rGO@TiO2@Ag into the PA layer was developed. The
definite features of the graphene-based nanocomposites were obtained by microwave irra-
diation process, which recommended water channelization and provided with super
hydrophilicity features. The MTFN-rGO@TiO2@Ag preparation process is shown in
Figure 1.15. Moreover, high permeability of 52 LM2/h, desalination performances of 96%
for 1 g/l Na2SO4 feed solution, and dye rejection of 98% for rose bengal dye feed solution of
0.5 g/l were observed [40].
In other work, unique, low-pressure nanofiltration membranes (LMPs) consisting of
MoS2 nano-supporting spacer among the GO layers are synthesized by pressure-driven
assembly and heat treatment. The GO/MoS2 showed pure water permeability of 10 LM2/h
at low pressure (2 bar), having greater than 13.6 times more when compared to pristine GO
GO
Dispersion in EG
Ultrasonication
30 min
Microwave irradiation rGO@TiO2@Ag

5 min, 600 W
TiO2 AgNO3
Figure 1.15 Schematic showing fabrication of rGO-TiO2-Ag nanocomposites through microwave

irradiation. Source: Abadikhah et al. [40]. © 2019 American Chemical Society.
Pressure driven
GO/MoS2 GO
Figure 1.16 Schematic showing fabrication of GO and GO/MoS2. Source: Zhang et al. [41]. © 2019
Elsevier.
membrane 0.75 LM2/h. Also, high rejection for different charged dyes >95% was observed.
Also, moderate salt rejections of 43%, 65%, 26.5%, and 23% for NaCl, Na2SO4, MgCl2, and
MgSO4 respectively [41]. The formation of GO and GO/MoS2 are shown in Figure 1.16.
It is well-known that the structural instability and flux deterioration factors hinder the
real-time application of GO-based membranes. Thus, an innovative GO/DTiO2-PDA-PEI
dopamine modified TiO2 hybrid nanofiltration membrane was obtained through multi
couple strategy, self-assembly, co-polymerization, and surface grafting method. Fine-
tuning the nanoscale interspace among the GO nanosheets and fabricating the membrane
with a positively charged surface and negatively charged subsurface with a pore size of
0.87 nm was developed. The designed membranes showed water permeance of
41.675 LM2/h. The rejection rate for the high molecular weight of positively charged crystal
violet dye 99.9%, positively charged safranine 96%, negatively charged EBT 99.9%, and low
molecular weight of negative dye Alizarin yellow GG 89.4% of less performance was
observed [42].
Yang et al. designed a novel nanofiltration membrane via rapid co-deposition of metal
phenolic networks (MPNs) and piperazine (PIP) on a porous substrate of trimesoyl chlo-
ride using a cross-linking approach. Motivated by the catechol chemistry, tannic acid sur-
face modified to tether PIP monomers are formed by co-deposition through coordination
bonds with Fe3+ ions on the substrate to form Fe3+/TA-PIP complex. The designed mem-
brane showed improved water permeability of 13.73 LM2/h and 89.52% of MgSO4 rejection.
Furthermore, to enhance the membrane performance, modified GO nanosheets were
embedded on Fe3+/TA-PIP complex, exhibiting improved water permeability of 21.66 LM2/h
and MgSO4 rejection of 91% [43].
Another work revealed polyethersulfone micro-filtration membranes (mPES) function-
alized with polyethilenimine and GO by LBL assembly approach through electrostatic
interactions pressure-driven filtration system. The highly positively charged polyethilen-
imine allows easy to assemble on PES substrate to accept negative layers of GO. Finally, the
designed combinations of GO/PEI showed the best performance for Blue Corazol (BC)
with dye rejection of 97.8% and pure water permeability of 99.4 LM2/h. Also, the mem-
brane showed a flux recovery of >80% after hydraulically cleaning. Also, rejection of BC
dye in real dye bath wastewater showed outstanding performance with >96% of rejection
rate was observed [44].
In other reported work, ultra-thin GO films with better salt rejection made-up through
contra-diffusion-induced cross-linking constructed on cation-π and electrostatic interac-
tions between cations and GO flakes. Moreover, it is a rapid process. Only five minutes is
required to design a defect-free GO film. Several cations such as Na+, K+, Mg2+, Ca2+, and
Fe3+ are used as “cross-linkers” to design GO membranes with high separation perfor-
mances. The designed membranes showed a 90% rejection for Na2SO4 salts with a perme-
ance of 4.3 LM2/h/bar [45].
In this report, UV reduced graphene oxide (UrGO) membranes supported on PVDF was
designed for wastewater treatment applications. The weak reduction GO membrane
showed optimal performances for removing pollutants. Due to the weak reduction of GO
membrane, pristine graphitic sp2 domains increased with a minor decrease in d-spacing.
Therefore, UrGO membranes revealed a high water flux of 38.27 LM2/h/bar by enhanced
flux more than 270% compared to GO membrane alone. Also, the rejection rate of 99% was
observed for RhB dye, and for other dyes such as EBT, methylene blue, crystal violet showed
>96% of rejection performances [46].
To sieve small inorganic salt ions number of reports are projected by reducing the inter-
layer spacing down to several angstroms. On the other hand, the major challenge for such
compacted graphene oxide membranes (GOMs) is a very low water flux of <0.1 LM2/h/bar
that hinders real-world applications. Planar heterogeneous graphene oxide membranes
(PHGOM) with definite salt rejection and high water flux is reported. A horizontal ion
transport via oppositely charged GO multi-layer heterojunction showed bi-unipolar
transport performance by blocking the conduction of both cations and anions. Furthermore,
supported by the forward electric field, salt concentrations are depleted in the neutral tran-
sition area of PHGOM. In this condition, deionized water is extracted from the depletion
zone. Further, undergoing all these mechanisms high rejection rate for NaCl and water flux
of 1529 LM2/h/bar was observed [47].
In other work, starch modified GO was added to the polypiperazinamide network to give
superior flux hyper-branched starch functionalized graphene oxide composites (HGOST)
nanofiltration membranes. The modified GO starch composites are embedded in the PA
top layer by esterification. The membranes are negatively charged with the top layer and
showed high rejection with 96% for Na2SO4 salts and pure water flux of 10 LM2/h/bar [48].
Wang et al. proposed new multiple tailored assembly ethylenediamine cross-linked GO
nanocomposites membrane on a macroporous tubular ceramic substrate. In this work,
the GO nanosheets are well orderly stacked, showing the construction of efficient nano-
channels for mass transfer. The subsequent membrane showed permeance of
375.75 LM2/h/bar, which is 5.62 times superior to GO membranes, and rejection of 98.6%
for EBT dye. The flux for Na2SO4 salt was 232.72 LM2/h/bar, and a 78% rejection rate was
observed [49].
Nonetheless, effectual tuning of rGO laminar arrangements for improved membrane
performance remains a challenging task. In this work, novel 1-D graphitic carbon nitride
nanotubes (g-C3N4-NTs) intercalated rGO nanofiltration (NF) membrane with the better
photo-induced self-cleaning property. The g-C3N4-NT enlarged the rGO interlayer spacing
for enhanced water permeability and has visible light photocatalytic properties to remove
dye pollutants. The g-C3N4-NT/rGO membranes exhibited water permeability of
4.87 LM2/h/bar and RhB removal rate of >98% for long term operation [50].
It is known that rGO membranes with narrow channels display salt rejection compared
to conventional nanofiltration (NF) membranes. However, their water permeance is less
due to the high tortuosity of water permeation. This report includes a simple approach to
creating in-plane nanopores on the GO sheets before reduction, decreasing the tortuosity,
increasing water permeance, and maintaining effective salt rejection. Holey graphene
oxide (HGO) nanosheets synthesized by chemical etching using hydrogen peroxide by
depressing porous support by vacuum filtration and reduction through contact with hydri-
odic acid solutions to create r-HGO membranes. Formation of nanopores improves water
permeance from 0.4 to 6.6 LM2/h/bar and with a Na2SO4 rejection rate of 98.5%. More
importantly, water permeance and Na2SO4 rejection reached the first time to the level of
commercial PA-based NF membranes [51].
In another work, the enhanced nanofiltration ability of graphene-based membranes was
designed by adding graphene oxide nanoribbons (GONRs) to the graphene nanochannels.
The designed membranes could efficiently filter small molecules with a high rejection rate
of >95% for various dyes (methyl red, methyl orange, methylene blue, and rose bengal)
with high water permeance 312.8 LM2/h/bar. The improved nanofiltration was observed
due to the electrically charged and expanded nanochannels [52].
The GO membranes in the aqueous solution limit their wastewater treatment in mem-
brane separation applications. The nanocomposite membrane made up of sarium-MOFs
and GO nanosheets were synthesized through the filtration of Sm-MOFs dispersions via in
situ growth. In this work, GO sheets disallowed the adjacent GO layers expanding in
aqueous solutions, undergoes a stable skeleton membrane structure. Sm-MOFs’ addition

helps in the enlargement of composite membrane space, which would favorable for higher
permeance. On the other hand, the designed composite membranes showed high perme-
ance of 26 LM2/h/bar indicating three times superior to pristine GO membrane; >91% high
rejection rate for RhB and methylene blue dyes proved with long term stability perfor-
mances [53].
Generally, poor chlorine resistance reduces the service life of the PA membrane in RO. In
this work, N-GOQDs were grafted and integrated on the PA membrane surface. Usually,
grafting investigations reduces water flux. However, in this work, the flux of the grafted
membrane showed enhanced performance compared with commercial bare membranes.
The grafted membrane with concentrations of 0.002 mg/ml showed better desalination of
water flux of 40 LM2/h/bar and NaCl rejection of 96.2% compared to bare membrane
36 LM2/h/bar with 94% rejection rate [54].
Yang et al. developed a GO/AgNPs nanocomposites membrane prepared to determine
the side effects of AgNPs for nanofiltration performances. Different AgNPs sizes such as 8,
20, and 33 nm were coated on GO membranes, and the filtration process was evaluated on
dead-end filtration mode. Among different sized AgNPs, only 20 nm AgNPs coated GO
membranes showed the highest water flux of 106 LM2/h/bar and 97.73% rejection rate for
RhB dye molecules. The mechanism involved in nanofiltration is interlaying spacing and
defect size of designed GO/AgNPs membranes [55].
The swelling of GO membranes is one of the disadvantages of liquid separation applica-
tions. To avoid this, cross-linking is commonly used to stabilize GO membranes and helps
in the enlargement of d-spacing. The hybrid GO/boron nitride membrane is formed
through physical and chemical bond formations. Changing the GO nanosheets and amino-
modified boron nitride facilitates plane-plane confirmation, edge–edge covalent bonding,
which helps develop compactly packed laminar structure, preventing membrane swelling.
Further, the designed stable membrane was able to show 99.98% of rejection rate and
4.15 LM2/h/bar of flux performances for methylene blue target pollutant [56].
It is important to note that most GO laminar membranes have poor water flux and
high rejections for both dyes and salts, which is usually not recommended for dye/salt
separations. In this work, NH2-Fe3O4 was introduced on GO nanosheets through vac-
uum filtration method. The advantages of NH2-Fe3O4 act as a rigid spherical nanospacer
to fine-tune GO interlayer spacing and cross-linkers to enhance the stability of GO
membranes. The 8 wt% loading of NH2-Fe3O4 exhibited improved water flux of 78 LM2/h/bar,
which is 4.8 superior to pristine GO membrane. Also, it showed 94% of congo red rejec-
tion rate and low NaCl rejection performances suggesting effective dye/salt mixture
separation [57].
Wu et al. fabricated glycine mediated GO/g-C3N4 lamellar membranes for nanofiltration.
In this work, glycine acts as a linker for the improved interactions among GO and g-C3N4.
Also, g-C3N4 and glycine help to increase the interlayer spacing of GO membranes. When
compared to bare GO membranes, composite membranes showed rapid water transporta-
tions. Furthermore, surface modifications by introducing hyperbranched polyethyle-
neimine (HPEI) coating showed excellent separation performances. The developed
membranes showed rejection rates for RhB 77.7, Alcian blue (AB) 89.5, Eosin Y (EY) 91,
Evas blue (EB) 99.4%, respectively, with permeance of 15.7 and 42.9 LM2/h/bar [58].
Bulk MoS2
MoS2/GO dispersion
Exfoliation
MoS2 nanosheets
Mixing
Fabricating membrane
GO nanosheets
MoS2/GO membrane
Figure 1.17 Fabrication of MoS2/GO nanocomposite membrane. Source: Ma et al. [59]. © 2020
Elsevier.
A facile method was established to decrease the repulsive hydration among GO sheets
by intercalating MoS2 on GO nanosheets, and their fabrication process is shown in
Figure 1.17. The strong van der Waals forces among MoS2 and GO, weak interactions
between MoS2 and water molecules and swelling of GO membranes were prominently
reduced. The smooth surface of MoS2 provides with high water flux of 48 LM2/h/bar.
Additionally, separation performance with rejection rates for various dyes 99.99%, 99.90%,
99.76%, 99.66% for DR80, CR, RhB, and MB dyes. Also, rejection rates for various salts
96.85% K3Fe(CN)6, 66.76% Na2SO4, 58.31% MgSO4, 56.00% NaCl, and 44.85% for MgCl2
was observed [59].
In another work, solvothermal induced 2D rGO-TiO2 with laminar structure was con-
structed as building blocks for the enhanced separation permeance. The specific properties
of designed rGO-TiO2 membranes such as high surface area, interfacial effects, and narrow
layer spacing for size exclusion showed >97% rejection rates for various dye molecules
RhB, methyl orange, methylene blue, and congo red. Also, it attained good permeance of
9.36 LM2/h/bar under the cross-flow filtration process [60].
The graphene oxide nanomembranes (GONMs) with different reduction degrees from
diverse graphitic resources proved for water purification performances. The main differ-
ences in various functionalities present on the GO surfaces such as (carboxyl (–COOH) or
C-GO, hydroxyl (–OH) or H-GO, and epoxy (–COC) or E-GO which is not clearly under-
stood the role of oxygen-bearing groups in the purification process. Thus, in this report, a
systematic study was performed on C-GO, H-GO, and E-GO among three oxygen-bearing
functional groups. To know the surface properties (Zeta analysis) and d-spacing (XRD) was
performed. The obtained results showed oxygen functional groups with diverse hydrophi-
licity and electricity changed the d-spacing of GONMs and C-GONMs with more negative
GO
um
cu Assembly
Mixing Va
Filtrati
on
MXene
Figure 1.18 Fabrication and assembly of GO/MXene via vacuum filtration process. Source: Liu
[62]. © 2020 Elsevier.
charges showed best performances >99% of rejection rate for Trypan blue (TB) dye due to
electrostatic effects [61].
In this work, a novel composite membrane based on GO and MXene is demonstrated,
and fabrication strategies are represented in Figure 1.18. The important heterogeneous
structure of GO/MXene membranes with a different synergistic effect in substrate rejection
and permeability was observed. The designed GO/MXene based membranes showed a
higher water flux of 71.9 LM2/h/bar than the pristine GO membrane showed only
6.5 LM2/h/bar. The rejection of various organic dye molecules such as neutral red (NR),
methylene blue (MB), crystal violet (CV), and brilliant blue (BB) exhibited >99.5% efficien-
cies indicating effective membranes in water treatment [62].
A hierarchical carbon membrane (HCM) was fabricated through a successive vacuum
filtration of carbon fiber (CF) substrate, a CNT intermediate supportive layer, and a GO
layered membrane. Fabricated HCM membranes were evaluated by capillary flow porom-
etry, thermogravimetric analysis, and membrane performance evaluation. HCM mem-
branes showed an 85% rejection rate for sulfate ions and 1.3 LM2/h/bar of permeability [63].
In this report, hydrophobic nanofibrous composites for vacuum membrane distillation
(VMD) comprising of hydrophobic PVDF nanofibrous layer and hydrophobic polypropyl-
ene (PP) nonwoven fabric (NWF) substrate were prepared. The PVDF nanofibrous layer
was directly fabricated on the surface of the PP NWF substrate through the electrospinning
method. 1H, 1H, 2H, 2H-perfluorooctyltriethoxysilane (FTES) modified GO nanosheets
were integrated with the PVDF nanofiber layer electrospinning process to improve the
hydrophobicity and water flux in VMD. For the designed membranes, the water flux was
36.4 LM2/h/bar, and NaCl salt rejection was 99.9% [64]. The preparation process and hydro-
phobic modification of GO nanosheets with FTES are shown in Figure 1.19.
Halakoo and Feng reported surface functionalization of thin-film composite PA mem-
branes for desalination of high salinity water through pervaporation. The surface modifica-
tion includes treating the PA membrane with chlorine via LBL assembly of positively
charged PEI and negatively charged GO. The chlorination treatment improved water per-
meability, and combining PEI and GO to the chlorine-treated PA membrane helps in
enhanced salt rejections. Designed PEI/GO/LBL membranes for the various aqueous salts
such as NaCl, Na2SO4, MgSO4, and MgCl2 showed water flux of 8 kg/m2 h with superior slat
rejections of >99.9% [65].
In this work, the significance of nanowrinkles in rGOMs for non-selective water and salt
transport by fine-tuning 2D nanochannels and nanowrinkles with three reduction methods
F
F F F
F F
F F
F F F F
F F F F
F F F
F F
F F F F
F F F F
F F F F
F F
F
F F F F
F F Hydroxylation F F Adsorption Si Si
F O O O
F O O
F F F
F
F F O O
Si Si
O O O O OH
O CH3 O O O O OH
H3C HO OH HO OH
CH3 OH
O O
OH
FTES OH
O HO
GO
Figure 1.19 Schematic showing a hydrophobic modification of GO nanosheets with FTES. Source: Li et al. [64].
© 2020 Elsevier.
were demonstrated. In the oxidizing atmosphere of air, non-selective nanowrinkles are

reduced mild and moderate air thermal reduction process, which is very important for
specific water and salt separations. Thus, designed Air-rGO membranes exhibited a
high 83% NaCl rejection with enhanced water flux through a hydraulic pressure-driven
separation system [66].
In this current work, improving the stability of GO membranes surface was modified by
intercalating ionic polymers rich in benzene and cationic imidazolium (or anionic sul-
fonic) functionalities helps in cross-linking the adjacent nanosheets through non-covalent
interactions. The 2D C-GO (imidazolium interactions/cationic) and A-GO (sulfonic inter-
actions/anionic) in the solvated state could preserve their constancy for a longer period. In
contrast, solvated GO membranes would instantly decompose when immersed in water. In
nanofiltration applications, both 2D C-GO and A-GO showed high permeances of 1111, and
600 LM2/h/bar under 5 bar compared to pristine GO membrane showed only 65 LM2/h/bar.
Also, in desalination, the 2D C-GO membranes with high water flux of 2.49 LM2/h/bar and
NaCl salt rejection of 95% compared with GO membrane 1.66 LM2/h/bar and rejection of
76% was observed [67].
GO and rGO significantly used as membranes in water treatment applications.
Nevertheless, the main drawbacks are swollen nature and unstable after contact with
aqueous solutions. In this work, membranes produced from GO were synthesized using
liquid-phase exfoliation, having less oxygen content, unlike the GO/rGO systems used.
Its application in ion sieving is reported. Less oxygen content graphene membranes
formed from flakes changing size are used to know the effects of flake morphology on ion
transport. Especially, reducing flake length and thickness helps improve the number of
tortuosity of nanochannels among the layers, resulting in a substantial ion transport
reduction. The smaller flakes showed better surface charge due to defects that inhibit
chloride mobility permitting for physical sieving and charge repulsions. As designed,
graphene membranes showed outstanding Na+ rejection 97% and water permeance ~10
times higher than those reported GO-based membranes with higher stability with no
witnessed swelling [68].
1.3.4 Translation of Graphene Nanomembranes for Real Applications

In this chapter, many modification concepts and applications are reported, proof of con-
cept stage in researcher labs. There are no many examples of their translation to indus-
trial scale, and the main reason is their scalability and competitiveness compared with
established and low-cost nanofiltration membranes (https://www.graphene.manchester.
ac.uk/learn/applications/membranes). In recent years, there are several successful
examples of scalable production of GO membranes fabricated by coating commercial
filtering material. One of the most successful and advanced examples of this develop-
ment comes from Monash University (Professor M. Majumder) group who collaborated
with local graphene company Ionic Industries and developed the first scalable GO
membrane production in Figure 1.20. The demonstration and production were able to
process and manufacture several hundreds of long membranes using this process. This
company is currently in the process of applying this technology to clean water
production.
Figure 1.20 Photos showing industrial-scale production of GO membranes in Melbourne,

Australia, developed by Monash University and Ionic Industries. Source: https://www.monash.edu/
engineering/about-us/news-events/latest-news/articles/2018/monash-pours-enery-into-clean-
water-future. Reproduced with permission.
1.4 Graphene Nanomembranes for Heavy Metals Treatment
1.4.1 Heavy Metals

Heavy metallic ions present in the water system are very troublesome to biodegrade. It can
easily enter the human body via food chain, instigating a series of irreversible physiological
diseases. For example, mercury ions can severely damage the central nervous system,
which leads to headaches and gastroenteritis. Lead ions can damage brain tissue, and the
excessive amount of lead ions in the body leads to loss of appetite, developmental delay,
and hearing impairment. Similarly, other heavy metals have their disadvantages, so it is
very important to treat such toxic pollutants safely [69].
An investigation based on the influence of GO nanosheet lateral size on the microstruc-
ture and liquid separation performance of ethylene diamine (EDA) cross-linked mem-
branes was studied. Three groups of GO nanosheets with different lateral sizes separated by
centrifugation used for membrane preparation in the presence of cross-linker EDA. The
designed membrane performed long term stability and exhibited with higher flux rate
and >99% of rejection for Cr(VI), showing membrane advantages with constricted d-spac-
ing and enlarged ion size in acidic conditions [70].
The GO and GOMs display excellent rejection for ions, particularly in water treatment.
Though, processing and scale-up of GOMs with stability issues persists as one of the major
limitations. In this report, fabrication of GOMs with blade casting technique with various
cations (K+, Na+, Li+, Mg2+, Ca2+, and Ba2+) intercalation with variable thickness and
interlaying spacing. The average water flux obtained for GO-K+, GO-Ba2+ GO-Ca2+,
GO-Mg2+, and was 106.35, 46.59, 39.7, and 36.64 LMH. The rejection of Na+ was 82.57%
(GOM-K+) > 78.6% (GOM-Ba2+) > 75.4% (GOM-Ca2+) > 72.3% (GOM-Mg2+) whereas rejec-
tion for Mg2+ 98.84% (GOM-K+) > 97.7% (GOM-Ba2+) > 96.6% (GOM-Ca2+) > 95.57%
(GOM-Mg2+). In addition, GOM-Ca2+-R showed highest flux rates and rejection rates for
Mg2+ (99.5%) followed by Cu2+ (98.4%), Ni2+ (97%), Pb2+ (96%), Na+ (88.6%) due to the
interlayer spacing when associated to other GOMs [71].
Chen et al. reported GO and PES membrane fabricated for separation performance of
Hg2+ ions, where the GO membrane assembled on PES microfiltration membrane through
GO solution
PES membrane
Pump
Figure 1.21 GO-PES vacuum-assisted process. Source: Chen et al. [72]. © 2019 American Chemical
Society.
vacuum-assisted technique shown in Figure 1.21. The designed GO/PES membranes

showed Hg2+ retention of 80% and flux of 26.2 LM2/h bar. Further, the membranes with
three circulations maintained the retention rate of 60.63% [72].
In other work, a dual functionalized PmGn@PVDF membrane was fabricated by doping
GO and followed by PDA coating. The developed membranes showed pure water flux of
188 LMH/h, and Pb2+ could remove successfully in the water volume of 2106 LM2/h/bar.
The doping of GO helped maintain Pb2+ rejection, which can be ascribed due to the chela-
tion of amino groups present on the PDA layer. Also, actual Pb2+ removal was attained to
5029 LM−2 due to the addition of citric acid [73].
In this work, TFN FO as a support layer and fabricated in the presence of different
concentrations (0–8 wt%) of polyethylene glycol 400, polysulfone, and 1-methyl-2-pyrrolidone
through phase inversion process. An active layer is obtained by integrating different
weight ratios of (0–0.012 wt%) GO, 1,3-Phenylenediamine, and 1,3,5-benzene trichloride
into the PA layer via interfacial polymerization process. The water flux for TFN mem-
brane was 34.3 LMH, enhanced by 174% and 129% compared to TFC membranes
12.5 LMH and commercial FO membrane 15 LMH. Also, the rejection ratios for various
metal ions followed the trend lead (99.9%), cadmium (99.7%), and chromium (98.3%) [74].
Harun et al. demonstrated the use of jatropha oil in the fabrication of membrane and
their comparison with GO into the polymer matrix. The jatropha oil-based polyol (JOL)
was blended with hexamethylene diisocyanate (HDI) to yield jatropha polyurethane mem-
branes (JPU). Further, GO with different loading was prepared to obtain a JPU/GO com-
posite membrane. The water flux enhanced from 223 to 523 LM2 /h. Later, filtration for
copper ions showed rejections from 33% to 71.60% [75].
1.5 Conclusion and Future Perspectives
Membrane separation technology authenticated a significant role in wastewater treat-

ments. Many research studies have been focused on separation performances using GO
and GO modified/functionalized membranes in water treatment applications in recent
years. It has been demonstrated that GO alone and GO modified membranes showed
enhanced membrane properties in terms of mechanical strength, selectivity, flux, rejection,

and thermal properties. Various fabrication strategies adapted and reported for GO/GO
surface-modified nanomembranes in the desalination process (removal of salts), various
dye and heavy metals separation or treatment showed inspiring results. In addition, some
of the most promising results paved the information that GO-based nanomembranes could
replace some of the existing commercial membranes is demonstrated. Even though several
important challenges need to be addressed, such as long-term stability issues and industrial
productions, graphene-based nanomembranes are potential low-cost candidates in water
treatments. However, the primary key success includes a proper balanced direction toward
production costs, and facile manufacturing operations are highly required. Accordingly, it
is imperative to advance the expansion of research and development on GO-based
nanomembranes. Finally, successful development in GO-based nanomembranes will pro-
vide one of the most promising platforms for overcoming the expected global water crisis
near future.
Acknowledgments
MDK acknowledges DST, India (DST/BDTD/EAG/2019) and DST Nanomission, India

(SR/NM/NS-20/2014) for financial support. DL acknowledges support from ARC Research
Hub for Graphene Enabled industry transformation (IH150100003). The authors also
thank Jain University, India, for providing facilities.
Important Websites
https://www.google.com/search?q=Graphene+based+nanomembranes+for+sustainable+
water+purification+applications&rlz=1C1CHBF_enUS858US858&oq=Graphene+
based+nanomembranes+for+sustainable+water+purification+applications&aqs=chr
ome..69i57.1483j0j7&sourceid=chrome&ie=UTF-8.
https://www.google.com/search?q=Graphene+based+nanomembranes+ for+sustainable+
water+purification+applications&newwindow=1&rlz=1C1CHBF_enUS858US858&
sxsrf= ALeKk03uoBKVyKKhJQH-BtDrCM_2hYmkpA: 1603719599866&source=lnms&
tbm=isch&sa=X&ved=2ahUKEwjF0MaIsdLsAhWQilwKHcI_AAcQ_AUoAnoECAUQ
BA&biw=1368&bih=802&dpr=2.
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Another random document with
no related content on Scribd:
Al darle ahora la bienvenida, llevando vuestra voz, experimento,
Sres. Académicos, una de las satisfacciones más grandes de mi
vida. Hijo de una de las ciudades más antiguas y gloriosas del viejo
Reino sevillano, la ciudad de los Guzmanes, tengo á orgullo, y es
para mí eterno vínculo de gratitud y de cariño, haber recibido mi
educación literaria é histórica en las aulas hispalenses y en el trato y
comunicación de los ingenios de Sevilla, y que el nuevo Académico
fuese de los que con mayor interés y afecto me alentasen en mis
primeras tentativas y ensayos. ¡Quién me dijera entonces que en
acto de la solemnidad del presente habría de disfrutar la grata y
honrosa participación con que vuestra bondad se ha dignado
favorecerme!
Entre los muchos é interesantes asuntos que las ricas y variadas
aptitudes y conocimientos del nuevo compañero le habrían permitido
escoger como tema de su discurso de ingreso, el docto americanista
ha preferido oportunamente el de mayor alcance y trascendencia de
todos, esto es, el examen de las últimas doctrinas y trabajos
referentes á Cristóbal Colón, examen que acabáis de coronar con
vuestros aplausos, y que ha evidenciado una vez más el acierto y
elocuencia peculiares á su entendimiento y á sus facultades
literarias. Mis enhorabuenas más cordiales por la elección y el
desempeño.
La celebración del cuarto Centenario del descubrimiento de
América dió origen, como era de esperar, dentro y fuera de la
Península, á numerosos estudios relativos á los dos grandes é
inseparables factores de aquel acontecimiento sin igual en la
historia: Colón y España. Natural era que el docto americanista
sevillano siguiese con vivo interés las nuevas publicaciones,
estudiando cuanto en ellas se dijese tocante á las mismas
cuestiones que había tratado en su Vida de Colón, á fin de
comprobar y perfeccionar sus propias investigaciones.
La Academia, que cuenta en su seno americanistas
mantenedores de distintas y encontradas opiniones sobre puntos
capitales de la historia colombina, debía oir de igual modo las del
nuevo Académico, que no son otras, en esencia, que las que ya
consignó en su obra magna, robustecidas ahora con los datos y
materiales con que el Centenario ha contribuido al esclarecimiento
de cuestiones sobrado graves y empeñadas para que nadie pueda
osar resolverlas todas y en absoluto, máxime dada la naturaleza de
los conocimientos históricos.
Por mucho tiempo la leyenda colombina y la leyenda
anticolombina han de disputar tenazmente la plaza que sólo cumple
de derecho á la verdad histórica. Panegiristas de Colón y
panegiristas de España seguirán luchando con apasionamiento,
hasta que al fin luzca el día sereno de la justicia, así para el
incomparable marino genovés como para la nación generosa que
amparó é hizo posible la hazaña más prodigiosa de la Edad
Moderna.
Mis sentimientos y mis convicciones coinciden, de antiguo y casi
por completo, en estas materias, con las del nuevo Académico, y ahí
están que lo prueban los trabajos que dí á luz en el Centenario; sin
que por eso deje de reconocer en ningún caso que ni está ni es
posible que esté cerrada la puerta á ulteriores investigaciones, en
esta, como en toda clase de controversias históricas.
Creo más, señores Académicos: creo plenamente que, á pesar de
las exageraciones, aun de las injusticias con que la pasión haya
podido tratarla, en lo antiguo y en lo moderno, la figura gigantesca
del descubridor del Nuevo Mundo ha resistido victoriosamente los
embates de la ceguedad y del encono, llegando incólume á los días
del Centenario, y, como dijo magistralmente nuestro ilustre Director,
en su discurso de apertura del Congreso de Americanistas
celebrado en el Convento de la Rábida, «en puesto único, al que
nadie puede acercarse, ni de lejos, en la Historia.»
Después de todo, por fortuna nuestra, Colón no fué considerado
nunca en los trabajos del Centenario como llegó á serlo, por el
mismo tiempo, en algunas de las publicaciones italianas, esto es,
como simple ejecutor del pensamiento de Toscanelli; ni tratado
tampoco con la crueldad incalificable con que algunos portugueses
escribieron del Infante Don Enrique en los días mismos de la
celebración de su Centenario, ni como tratan hoy otros, con motivo
del que ha de celebrarse dentro de pocos días, al glorioso
Taumaturgo de Lisboa.
Y es que las divisiones religiosas, políticas y científicas de nuestro
tiempo, y aun más, si cabe, el espíritu crítico, cuando no escéptico,
dominante, tenían que ejercer su propio y natural influjo aun en
ocasiones tan extraordinarias y solemnes. Lo verdaderamente
extraño es que se nieguen ó regateen tanto la admiración y el
aplauso á las grandes figuras de la historia, y se prodiguen con
largueza, mejor dicho, con verdadero escándalo, en ocasiones, á
entidades subalternas, como lo prueban las apoteosis pomposas
que vemos celebrar en gloria de algunas y las estatuas erigidas en
honor de otras, careciendo, como aún carecen de ellas, el Cid,
Guzmán el Bueno, el Rey Católico y tantas otras glorias
indisputables y legítimas de la patria.
¡Dichosos los que, como el nuevo Académico, han sabido
conservar siempre inextinguibles en su alma el entusiasmo y la
admiración debidas á lo verdadero y lo justo, lo grande y lo sublime!
He dicho.
ÍNDICE
Páginas.
Prólogo v
Las Conferencias americanistas del Ateneo 1
Los Reyes Católicos en el descubrimiento de 33
América
El Cardenal Mendoza en el descubrimiento 61
de América
Colón y Fray Diego de Deza 73
El Nuevo Mundo descubierto por Colón, 87
comedia de Lope de Vega
La patria de Colón 99
Españolismo de Colón 111
La Duquesa de Alba 121
El Maestro Lebrija y el descubrimiento de 135
América
La Aurora en Copacavana 147
Pedro de Valdivia 157
Gonzalo Jiménez de Quesada en la poesía y 167
en la historia
El Alférez Doña Catalina de Erauso 179
La Historia de la Conquista de México, de 199
Solís
Los restos de Pizarro 207
Sor Juana Inés de la Cruz 221
El Centenario en Chile 231
El Centenario en Colombia 239
Los Americanos en el Ateneo 247
Colón en las publicaciones italianas del 265
Centenario
Un americanista notable 287
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(PDF Download) Environmental Applications of Carbon Nanomaterials-Based Devices 1st. Edition Shadpour Mallakpour Fulll Chapter

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Environmental Applications of Carbon

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Industrial Applications of Nanocrystals Shadpour

Chapter 6 - Water treatment and environmental

Carbon Nanomaterials for Agri-food and Environmental

Food, Medical, and Environmental Applications of

Nanostructured Carbon Nitrides for Sustainable Energy

Bio-Based Nanomaterials : Synthesis Protocols,

Bio-Based Nanomaterials: Synthesis Protocols,

Industrial Applications of Carbon Nanotubes 1st Edition

Chaudhery Mustansar Hussain Library of Congress Card No.:

Cover Design: Wiley Bibliographic information published by the Deutsche

© 2022 WILEY-VCH GmbH, Boschstraße 12,

All rights reserved (including those of translation

Print ISBN: 978-3-527-34865-7

Typesetting Straive, Chennai, India

Printed on acid-free paper

1 Graphene-Based Nanomembranes for Sustainable Water

2 Magnetic Graphene Oxide and Its Composite Nanomaterials: Application

3 Biomass- or Biowaste-Derived Carbon Nanoparticles as Promising Materials

4 Applications of Carbon-Based Nanomaterials

4.10 ­ onclusions 122

5 Electrochemical Determination of Indigotine

6 Toxicity of Carbon Nanomaterials 147

6.5 ­ onclusions 160

7 Fundamentals of Functionalized Carbon Nanomaterials (CNMs)

8 Fundamental of Functionalized Carbon Nanomaterials for Environmental

8.2.1.3 Graphene 200

9 Functionalized Magnetic Carbon Nanomaterials for Environmental

10 Functionalized Carbon Nanotubes for Ammonia Sensors 251

11 Functionalized Carbon Nano Lab-on-a-Chip Devices

12 Functionalized Carbon Nanotubes (FCNTs) as Novel Drug Delivery Systems:

12.6.3 Chemical Oxidation 291

13 Adsorptive Removal of Fluoride by Carbon Nanomaterials 313

14 Functionalized Carbon Nano-Membranes Based Devices for Water

15 Functionalized Bio-carbon Nanomaterials for Environmental

15.11.5.2 Peptide Amphiphiles 359

16 Carbon-Based Nanomaterials in Drug Delivery Systems 375

17 Functionalized Carbon Nanomaterials (FCNMs): A Green and Sustainable

18 Functionalized Carbon Nanomaterials for Impending Pharmaceutical

Graphene-Based Nanomembranes for Sustainable Water

Environmental Applications of Carbon Nanomaterials-Based Devices, First Edition.

1.2 ­Graphene and GO-Based Membrane Characteristics

Size exclusion Electrostatic interactions

Size exclusion Electrostatic interactions

1.3 ­Fabrication of Graphene-Based Nanomembranes

1.3.2 Treatment for Dyes

1.3.3 Graphene Nanomembranes for Salt and Dye Rejection

EDA PAH PAH@ArGO

NO3–-HT Exfoliated HT Exfoliated GO EHT/GO

HO COOH OH COOH GO/APT

Cellulose acetate (CA)/GO nanocomposites were fabricated for seawater desalination

Figure 1.7 Schematic showing mechanisms involved in PDA-rGO-MOFs-HKUST nanocomposites.

Lee et al. effectively surface-functionalized EDTA-rGO membranes for nanofiltration.

Casting solution GP substrate

CuSO4/H2O2 PDA self-

UiO-66/PGP TFC PGP support layer

4.10 onclusions 122

6.5 onclusions 160

1.2 Graphene and GO-Based Membrane Characteristics

1.3 Fabrication of Graphene-Based Nanomembranes

1.4 Graphene Nanomembranes for Heavy Metals Treatment

1.5 Conclusion and Future Perspectives