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- Herausgeber: John Wiley & Sons
- Kategorie: Wissenschaft und neue Technologien
- Sprache: Englisch
The book is a comprehensive deep-dive into the developments and advancements of emerging carbon-based nanocomposites for wastewater applications. Science and technology development are tackling one of the world's most pressing concerns--water contamination and effective treatment. Carbon-based nanocomposites have emerged as one of the leading materials in this treatment push because of their properties and high ability for the catalytic degradation of contaminants from aqueous segments. The 10 chapters in this timely book cover the follows areas: * Carbon-based nanocomposites for remediation of heavy metals and organic pollutants from wastewater * Functional green carbon nanocomposites for heavy-metal treatment in water * Green nanocomposites and applications in environmentally-friendly carbon nanomaterials * Carbon-based nanocomposites as heterogeneous catalysts for organic reactions in environment-friendly solvents * Carbon-based polymer nanocomposite applications * Biochar-based adsorbents for the removal of organic pollutants from aqueous systems * Carbon nanomaterial-based green nanocomposites * The removal of trihalomethanes from water using nanofiltration membranes * Nanocomposite materials as electrode materials in microbial fuel cells for the removal of water pollutants * Plasmonic smart nanosensors for the determination of environmental pollutants.
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Veröffentlichungsjahr: 2020
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Table of Contents
Cover
Title Page
Copyright Page
Preface
1 Emerging Carbon-Based Nanocomposites for Remediation of Heavy Metals and Organic Pollutants from Wastewater
1.1 Introduction
1.2 Graphene Oxide
1.3 Carbon Nanotube
1.4 Conclusion
Acknowledgements
References
2 Functional Green Carbon Nanocomposites for Heavy Metal Treatment in Water: Advance Removal Techniques and Practices
2.1 Introduction
2.2 Water Contamination by Heavy Metals
2.3 Functional Green Carbon Nanocomposites
2.4 Advanced Removal Techniques in Water
2.5 Conclusion and Future Directions
References
3 Green Nanocomposites: Advances and Applications in Environmentally Friendly Carbon Nanomaterials
3.1 Introduction
3.2 Nanocomposites and their Processing Methods
3.3 Structures of Carbon Materials
3.4 Polymer/Carbon-Based Nanocomposite
3.5 Removal of Chemical Contaminants
3.6 Energy Sector
3.7 Gas Sensors
3.8 Conclusion and Outlook
Acknowledgment
References
4 Carbon-Based Nanocomposites as Heterogeneous Catalysts for Organic Reactions in Environment Friendly Solvents
4.1 Introduction
4.2 Carbon-Based Nanocomposites for Coupling Reactions
4.3 Carbon-Based Nanocomposites for Oxidation Reactions
4.4 Carbon-Based Nanocomposites for Reduction Reactions
4.5 Carbon-Based Nanocomposites for Other Organic Transformation Reactions
4.6 Conclusion and Perspectives
References
5 Carbon-Based Polymer Nanocomposite and Environmental Perspective
5.1 Introduction
5.2 The Vision of the Study
5.3 The Vast Scientific Doctrine of Carbon-Based Polymer Nanocomposites
5.4 Environmental Sustainability and the Vision for the Future
5.5 Environmental Protection, the Scientific Ingenuity, and the Visionary Future
5.6 Recent Advances in the Field of Nanocomposites
5.7 Recent Advances in the Field of Carbon-Based Polymer Nanocomposites and Environmental Pollution Control
5.8 Carbon-Based Polymer Nano-Composites for Adsorbent Applications
5.9 Carbon-Based Polymer Nanocomposites as Anti-Microbial Agents and Membranes
5.10 Applications of Carbon Nanocomposites in Removal of Hazardous Organic Substances
5.11 Water Purification, Groundwater Remediation, and the Future of Science
5.12 Arsenic and Heavy Metal Groundwater Remediation and Composite Science
5.13 Integrated Water Resource Management, Human Factor Engineering, and Nanotechnology— A Definite Vision
5.14 Technology Management, Environmental Protection, and Water Resource Management
5.15 Future of Nanocomposite Applications and Future Research Trends
5.16 Conclusion, Summary, and Vast Scientific Perspectives
References
Important Websites for Reference
6 Biochar-Based Adsorbents for the Removal of Organic Pollutants from Aqueous Systems
6.1 Introduction
6.2 Biosorbents
6.3 Biochar Production Techniques
6.4 Application of Biosorbents for the Sequestration of Selected Organic Pollutants
6.5 Removal Mechanisms
6.6 Challenges Associated With Biochar Technology
6.7 Conclusion
6.8 Future Scenario
References
7 Advances in Carbon Nanomaterial-Based Green Nanocomposites
7.1 Introduction
7.2 Carbon Nanomaterial-Based Green Nanocomposites
7.3 Methods of Processing for Carbon-Based Nanocomposites
7.4 Unique Properties of Carbon-Based Green Nanocomposites
7.5 Applications of Carbon-Based Green Nanocomposites
7.6 Future Prospects
7.7 Conclusions
References
8 Removal of Trihalomethanes from Water Using Nanofiltration Membranes
8.1 Introduction
8.2 Factors Influencing the Removal of THMs From Water
8.3 Summary and Outlook
References
9 Nanocomposite Materials as Electrode Materials in Microbial Fuel Cells for the Removal of Water Pollutants
9.1 Introduction
9.2 Microbial Fuel Cells: An Emerging Wastewater Treatment and Power Technology
9.3 Pollutants Removal Using MFCs System
9.4 Conclusion and Outlook
Acknowledgement
References
10 Plasmonic Smart Nanosensors for the Determination of Environmental Pollutants
10.1 Introduction
10.2 Principle of Plasmonic Nanosensors
10.3 Applications of Plasmonic Nanomaterials in Sensing
10.4 Plasmonic Nanosensors
10.5 Plasmonic Nanosensors for Pollution Control and Early Warning
10.6 Conclusion, Key Trends and Perspectives
References
Index
End User License Agreement
List of Tables
Chapter 1
Table 1.1 Dye adsorption on GO-based materials.
Table 1.2 Metal ion adsorption on GO materials.
Table 1.3 Organic pollutants’ adsorption on GO base materials.
Table 1.4 Maximum adsorption capacities for different dyes with CNTs.
Chapter 3
Table 3.1 Commonly used carbon-based nanomaterials, nanocomposites for treati...
Chapter 4
Table 4.1 Effect of aryl halides on the catalytic conversions in Suzuki-Miyau...
Table 4.2 Diversity of the Heck coupling reactions using the catalyst (Pd/Fe
3
Table 4.3 Comparison of catalytic activity of different catalysts for CuAACRe...
Table 4.4 Catalytic oxidation of various types of alcohols over the catalysts...
Table 4.5 Oxidation of amines to imines catalyzed by GO [41]
a
.
Table 4.6 Optimization of the oxidative conversion of p-xylene by NGO carbo-c...
Table 4.7 Catalytic transfer hydrogenation of various nitro compounds to the ...
Table 4.8 Optimization of nitrobenzene reduction conditions [46]
a
.
Table 4.9 Reactivity of the photoactive catalyst Ru–g-C
3
N
4
for catalytic hydr...
Table 4.10 The graphene oxide-catalyzed aza-Michael addition reaction [69]
a
....
Table 4.11 α-position functionalization of primary amines via tandem reaction...
Table 4.12 Synthesis of benzamide from benzyl alcohol and ammonia [74]
a
.
Chapter 6
Table 6.1 Illustrative studies of the adsorption of selected organic pollutan...
Table 6.2 Biomass pyrolysis methods and amount of biochar produced.
Table 6.3 Application of different sorbents and the respective experimental c...
Chapter 8
Table 8.1 Comparison between different membranes.
Chapter 9
Table 9.1 List of powering microbes with different types of contaminant remed...
Chapter 10
Table 10.1 DNA/RNA aptamers for binding to targets in the literature.
Table 10.2 SPR nanosensors for environmental monitoring applications.
List of Illustrations
Chapter 1
Figure 1.1 A schematic representation for the different process of water rem...
Figure 1.2 Hybridization states of carbon-based nanomaterials.
Figure 1.3 Functional groups attached on basal plane of GO.
Figure 1.4 Removal of organic dyes from water using hierarchical sandwiched ...
Figure 1.5 Schematic illustration of the synthetic route to mGO/PVA CG.
Figure 1.6 Adsorption behavior of GAs toward different dyes; adsorption spec...
Figure 1.7 Schematic diagram of the preparation of IRMOF-3/GO and the adsorp...
Figure 1.8 Diagrams of (a) single-walled CNTs (SWCNTs) and (b) multi-walled ...
Figure 1.9 Effect of functionalization of CNTs on adsorption of polar and no...
Chapter 2
Figure 2.1 Types of materials combination for heavy metals treatment in aque...
Figure 2.2 The structures of (a) carbon nanoparticle with an attached metal ...
Figure 2.3 (a) Mechanism of chemical reduction; (b) Macroscopic photos of (i...
Figure 2.4 Removal mechanism of Cr(VI) over fibrillar and particulate magnet...
Figure 2.5 (a) Beads preparation (i) SA and GO completely dispersed in water...
Figure 2.6 Decomposition of synthetic nanocomposites (a) III [Ani:Dex (1:3)]...
Chapter 3
Figure 3.1 Application of carbon-based nanocomposites [23].
Figure 3.2 Different forms of carbon nanostructure [27].
Figure 3.3 General reaction mechanism for wastewater treatment.
Chapter 4
Figure 4.1 Schematic representation of various carbon-based nanocomposites a...
Figure 4.2 Schematic representation of microwave assisted hydrothermal synth...
Figure 4.3 Nitrogen-doped graphene nanosheets as metal free catalysts cataly...
Figure 4.4 Schematic representation of rGO@Ru-RM β-CD catalyst for on-water ...
Figure 4.5 One-pot total synthesis of brittonin A in aqueous medium using rG...
Figure 4.6 Au-Pd/CNT catalyzed aerobic oxidation of 5-hydroxymethylfurfural ...
Figure 4.7 Ru-GCN catalyzed organic transformation under visible light irrad...
Figure 4.8 Reduction of aromatic nitro compound over the Fe
3
O
4
@BRAC catalyst...
Figure 4.9 Cooperative effect of cobalt redox catalysis and g-CN photocataly...
Figure 4.10 Physical characterization of NCNTs. (a, b) SEM images of NCNTs a...
Figure 4.11 Schematic illustration of improvement of butenes selectivity on ...
Figure 4.12 Fe@g-C
3
N
4
catalyzed reduction of styrene in the presence of visi...
Figure 4.13 Plausible reaction mechanism for hydrogenation of alkene using F...
Figure 4.14 Use of p-GO for tandem functionalization of primary amines via c...
Figure 4.15 Sulfonated g-C
3
N
4
catalyzed transformation of (a) xylose to furf...
Chapter 6
Figure 6.1 Materials flows through agroecosystems, human waste/sanitation sy...
Figure 6.2 The fabrication of biosorbents from different types of biomass
Figure 6.3 Illustration of sorption mechanisms for the sequestration of orga...
Chapter 7
Figure 7.1 Applications of polymer nanodiamond nanocomposites.
Figure 7.2 Applications of carbon-based green nanocomposites.
Figure 7.3 Nanoparticle-loaded carbon black-chitosan fibers.
Chapter 8
Figure 8.1 Trihalometane; Halogen (F, Cl, I, and Br) and cellulose acetate’s...
Chapter 9
Figure 9.1 Research publication trends on microbial fuel cell for pollutants...
Chapter 10
Figure 10.1 Scanning electron micrographs of different types of periodic pla...
Figure 10.2 Dissociation constant values of As
3+
to arsenate, arsenite, and ...
Figure 10.3 Scanning electron microscopy and atomic force microscopy images ...
Figure 10.4 The selectivity of the quaternary ammonium group-capped gold nan...
Figure 10.5 The colorimetric response of the assay. (a) Photographs of gold ...
Figure 10.6 Scheme of the metal ions, amino acids, and AuNP interactions: (a...
Figure 10.7 The SNZ, SMZ, and ATZ detection at different concentrations [138...
Figure 10.8 Preparation and schematic representation of the SPR nanosensor [...
Figure 10.9 (a) Scheme of the magnetic polydopamine nanoparticles preparatio...
Figure 10.10 Schematic diagram of instrumentation used for surface enhanced ...
Figure 10.11 Structure and spectroscopic characterization of Au and Au/Ag co...
Guide
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Scrivener Publishing100 Cummings Center, Suite 541JBeverly, MA 01915-6106
Publishers at ScrivenerMartin Scrivener ([email protected])Phillip Carmical ([email protected])
Emerging Carbon-Based Nanocomposites for Environmental Applications
Edited by
Ajay Kumar Mishra, Chaudhery Mustansar Hussain and Shivani Bhardwaj Mishra
This edition first published 2020 by John Wiley & Sons, Inc., 111 River Street, Hoboken, NJ 07030, USA and Scrivener Publishing LLC, 100 Cummings Center, Suite 541J, Beverly, MA 01915, USA© 2020 Scrivener Publishing LLCFor more information about Scrivener publications please visit www.scrivenerpublishing.com.
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Library of Congress Cataloging-in-Publication Data
ISBN 9781119554851
Cover image: Pixabay.ComCover design by Russell Richardson
Preface
The advances in science and technology is tackling a vital concern to both humans and the environment: Water contamination is one of the foremost and extreme alarming problems that demands effective treatment. Environmental contamination has emerged as a most exigent problem. Hybrid materials possess higher specific stiffness and strength, toughness, corrosion resistance, low density, and thermal insulation. Carbon-based nanocomposites have been widely studied due to the small size of fillers increases the interfacial area as compared to conventional composites. Carbon is an excellent host material for the nanoparticles and semiconductor. Carbon nanostructures such as carbon nanotubes, fullerene, and graphene with prominent electrical and structural characteristics have drawn much attention, as they contribute to the development of composites with improved catalytic performance. Carbon-based material such as graphene-composite have been synthesized and explored as it has great potential for the removal of noxious pollutants from wastewater. Much attention has been focussed recently using carbon-based nanocomposites due to the application of magnetic separation technology to solve the various environmental problems.
Carbon-based nanocomposites have unique magnetic separability and potential adsorption for pollutants. Carbon matrices avoid the agglomeration of iron oxide nanoparticles, and magnetic separation is a substitute to filtration or centrifugation as it avoids the loss of materials. Magnetic separation has been considered to be a quick and operative technique. Functionalized magnetic nanocomposites have distinct advantages over conventional materials due to their selective absorptivity, strong magnetic responsiveness, favorable water dispensability, and benign biocompatibility. Carbon-based nanocomposites have therefore revealed high ability for the catalytic degradation of contaminants from aqueous segment. The application of photocatalysis using heterogeneous semiconductor is inexpensive, non-toxic, broad absorption spectra with higher absorption coefficients and capability for multi-electron transfer.
The current book provides the comprehensive summary of the development and advancements based on emerging carbon-based nanocomposites for wastewater applications. It consists of 10 chapters. Chapter 1 provides details about emerging carbon-based nanocomposites for remediation of heavy metals and organic pollutants from wastewater, whereas Chapter 2 is focused on functional green carbon nanocomposites for heavy-metal treatment in water: advance removal techniques and practices. Chapter 3 summarizes green nanocomposites: advances and applications in environmentally-friendly carbon nanomaterials, whereas Chapter 4 discusses the carbon-based nanocomposites as heterogeneous catalysts for organic reactions in environment-friendly solvents. Chapter 5 consists of carbon-based polymer nanocomposite and environmental perspective. Chapter 6 presents biochar-based adsorbents for the removal of organic pollutants from aqueous systems, whereas Chapter 7 details advances in carbon nanomaterial-based green nanocomposites. Chapter 8 describes the removal of trihalomethanes from water using nanofiltration membranes. Chapter 9 details the nanocomposite materials as electrode materials in microbial fuel cells for the removal of water pollutants, whereas Chapter 10 describes the plasmonic smart nanosensors for the determination of environmental pollutants.
The book elucidates the scientific advancements and recent scientific development in the field of emerging carbon-based nanocomposites. Researchers involved in nanomaterials, environmental science, and water research will be the major beneficiaries of the book. The book will be highly beneficial to students who are working for their graduate and postgraduate degrees in this area.
Ajay Kumar Mishra, Chaudhery Mustansar Hussain and Shivani Bhardwaj MishraEditorsJuly 2020
1Emerging Carbon-Based Nanocomposites for Remediation of Heavy Metals and Organic Pollutants from Wastewater
Prasenjit Kar1, Pratyush Jain1, Raju Kumar Gupta1,2* and Kumud Malika Tripathi3†
1 Department of Chemical Engineering, Indian Institute of Technology Kanpur, Uttar Pradesh, India
2 Center for Environmental Science and Engineering, Indian Institute of Technology Kanpur, Uttar Pradesh, India
3 Department of Bionanotechnology, Gachon University, Seongnam-daero, Sujeong-gu, Seongnam-si, Gyeonggi-do, Republic of Korea
Abstract
Nano-carbons are emerging as promising materials for environmental remediation applications. Unique and extraordinary optical, electrical, and surface properties of nano-carbons in all of their forms have substantially and successfully been investigated widely for water remediation for the removal of diverse range of contaminants. Furthermore, revolutions in synthesis of nano-carbons–based composites led to the facile and fast adsorbent technologies for remediation applications. Ease in synthesis along with a wide scope to engineer the surface structure, porosity, electronic and magnetic properties of nano-carbons is the most significant criteria to the rational design of diverse adsorbent. In this chapter, carbon-based nanomaterials, especially graphene oxide (GO) and carbon nanotubes (CNTs) have been explored for their water remediation capabilities via adsorption process. Mechanistic insights and the interactions responsible for the adsorption are highlighted. Structural engineering of these materials into more suitable form for handling purposes has shown their practical application for treatment of water resources. Dyes, toxic metals, and other organic pollutants have been described for their removal via adsorption through GO and CNTs.
Amphiphilic nature of GO helps it to remove pollutants from water easily where most of the adsorption occurs due to the electrostatic interactions between functional group on GO and pollutants present. CNTs have shown very high specific area with tunable functionality, which can be used for removing polar and non-polar pollutants.
Keywords: Graphene oxide, carbon nanotube, organic pollutants, heavy metals, adsorption, water remediation
1.1 Introduction
Water soluble toxic pollutants are one of the vital concerns to both human and environment health worldwide in recent past few decades. Ever increasing world population, expanded use of chemical products and their demands toward the exploitation of natural resources has made it inevitable to develop unique methods and materials for the environmental remediation [1–4]. Hazardous industrial wastes, unethical agricultural practices, and unplanned human waste management have caused intoxication of water resources almost worldwide [5–7]. Although, stronger regulations by governments of various countries have been implemented to curb the unruly contamination of water bodies but recalcitrant nature of pollutants towards treatment in conventional wastewater treatment plants (WWTPs) has necessitated us to approach this grave problem from a new perspective [8, 9].
Widespread occurrence of water soluble pollutants, such as heavy metal ions [Cr(VI), Al(III), Hg(II), Ag(I), Pb(II), Fe(III), As(III) and Co(II)], synthetic organic contaminants like textile dyes, new emerging contaminants such as pharmaceutical and personal care products (PPCPs), microplastic pesticides, endocrine disruptors, nanomaterials textile dyes, and synthetic and natural organic contaminants, have threatens the balance of nature and causing concerns and research interests worldwide [10, 11]. Even these compounds are present at trace levels but could result in adverse effects over human health and aquatic life because of high toxicity and carcinogenic nature. Their resistant nature towards the bio-decomposition led to their gradual accumulation over a period of time in water bodies and their concentration may rise well above the safer limits [12]. Conventional techniques including primary processes like sedimentation, chemical precipitation filtration along with biological treatment as secondary process have been used for the removal of these contaminants. Advance processes for tertiary treatment like adsorption, micro and ultra-filtrations, catalytic wet air oxidation, photocatalysis, and electrocatalysis can be used to improve the efficacy of the treatment processes [13] (Figure 1.1). Researchers’ concern is to investigate and develop new class of materials for the advanced wastewater treatment while addressing other important aspects like preventing secondary pollution, reusability, chemical stability, physical integrity, and the cost of the materials [14].
Figure 1.1 A schematic representation for the different process of water remediation technologies.
Reprinted with permission [13].
Carbon being one of the most versatile elements on the earth provides an opportunity to fabricate materials with unconventional architectures. The narrow energy band gap and the electron transfer between 2s and 2p orbitals of carbon allows it to exist in different hybridization states. These stable states facilitate formation of diverse organic species with carbon as well as different bulk configuration of itself (Figure 1.2) [15]. Formation of flexible configurations results in varying strength of carbonaceous materials even at stable structures at nanoscale. Formation of nanomaterials enhances the surface area due to shrink in the diameter with bulk being maintained at the same density. Smaller size provides higher mobility which enables fast movement of nanoparticles (NPs) in the solution helping it to increase the coverage over a larger surface with relatively lesser amount of the material. The enhancement in aspect ratio also creates exposure of high number of low-coordinated atoms at the surface, edges, and vortices which increases the reactivity of these nanomaterials. These phenomenal properties enhance the ability of these nanomaterials to scavenge pollutants in aqueous medium [16]. Tunable physico-chemical properties of carbon have inspired an innovative approach towards fabrication of carbon-based nanocomposites.
Figure 1.2 Hybridization states of carbon-based nanomaterials.
Reprinted with permission [15].
Low-dimensional carbon-based nanomaterials like graphene, graphene oxide, and carbon nanotubes (CNTs) have gained significant attention for various applications over the past three decades [17]. Owing to extraordinary physiochemical properties nano-carbons have been extensively studies for application in energy, electronics, sensors, biomedical, thermal devices, and environmental remediation [15, 16, 18–20]. Graphene exhibits fascinating physical properties like tunable band gap, high electron mobility, high surface area, and enhanced active sites, which render it suitable candidate for applications related to catalysis [21, 22]. Graphene oxide (GO), derived from graphite via strong oxidation, can be thought as functionalized graphene with various oxygenated groups attached to its surface [23, 24]. GO has excellent surface functionality, aqueous processability, and amphiphilicity, providing an advantage for the removal of pollutants compare to conventional adsorbent materials [25, 26]. Due to difficult production protocols of pristine graphene via top down process, it is generally derived from reduction of GO, termed as reduced graphene oxide (rGO). Since graphene suffers from low dispersibility, hydrophobicity, and tendency to from agglomerate, arising from their low entropy gain for mixing, rGO can offset this disadvantage by stable aqueous colloids formation through electrostatic stabilization [27, 28]. CNTs are cylindrical form of graphite sheets. Recent developments have increased the utilization of CNTs in environmental remediation applications due to their highly available active surface area, catalytic sites, easily modifiable surface, enhanced chemical reactivity, and less impact on the environment [29–31]. Other carbon-based nanomaterials like carbon nanofibers, carbon beads, and nano-porous carbon has also been explored for their application in the field of wastewater treatment [32–34].
The efficiency of carbon-based nanomaterials towards application perspective can be further enhanced by various modifications. Component manipulation can be done by doping foreign element, whereas morphological control can be gained by encapsulation facilitating NPs to grow in a desired fashion, structural engineering and functionalization can also enhance various physical properties useful for adsorption activity towards wastewater treatment [35]. In this chapter, low-dimensional materials like GO and CNTs are focused due to their extensive contribution in the wastewater remediation.
1.2 Graphene Oxide
GO is one of the most fascinating macroscopic forms of graphene and exists in a non-stoichiometric form of molecules. It is a two-dimensional (2D) layered structure with oxygen functionalities including hydroxyls (OH), carboxylic (COOH) carbonyl (C=O), and alkoxy groups (C–O–C) [36, 37]. As shown in Figure 1.3, these functional groups make GO amphiphilic and enhancing its mono-dispersibility in contrary to graphene. The structural characteristic of GO helps it to interact with other molecules and ions via electrostatic forces, π-π interactions, hydrogen bonding, and hydrophilic interactions [38]. GO can be easily synthesized in both dry and wet medium. The former approach involves oxidation of graphene layers in ultra-high vacuum and subsequent treatment with ozone in ultra violet light; while, the later approach involves strong oxidation of graphite in an aqueous medium and subsequent exfoliation. Wet method is preferred due to abundance of graphite and low cost associated with the synthesis [24, 39, 40].
Figure 1.3 Functional groups attached on basal plane of GO.
Reprinted with permission [41].
1.2.1 GO and GO-Nanocomposite for Water Remediation via Adsorption
GO and its composite have attracted tremendous attention as a most potential adsorbent for water remediation due to highly exposed surface structure, abundant surface functionalities and active surface sites [42]. Nanocomposites of GO are promising because of their versatile properties and diverse variables available for fine-tuning. The GO-based nanocomposites have been widely explored for the adsorbative removal of various contaminants from water including heavy metal ions and synthetic dyes [43]. The adsorption can be controlled by various factors including physiochemical properties of adsorbent, adsorbent doses, as well as the background of contaminants chemistry. The fate, transformation, and toxicity of GO-based nanocomposite towards aquatic life have also been explored. One recent review by Asghar et al. documented the fate of magnetic GO nanocomposite and adsorption mechanisms for the adsorptive removal of heavy metal ions [44].
Dyes have shown adverse effects on human health, aquatic environment and lethal to plants. Since they have been proven to be mutagenic, they should be treated prior to discharge from industrial sources [45]. Since most of the dyes exhibit organic backbone and cationic groups, they are favorable for adsorption on GO because of π−π stacking and ionic interactions [46]. A number of dyes, like methylene blue (MB), crystal violet (CV), malachite green (MG), basic green (BG), Rhodamine B (RhB), have been chosen for this purpose to show removal efficiency of GO synthesized via different routes. Table 1.1 comprises the removal efficiency of dyes with their maximum adsorption capacity on GO as suspension and sponge form. Most of the time, GO is prepared via Hummer’s method and its modification [24, 47–49]. In general, oxidized graphite is subjected to sonication to exfoliate quasi-stacked GO sheets, which afterwards are differentially centrifuged and recovered with the supernatant. MB is one of the most studied dyes for adsorption as a model compound. Most of the studies had shown GO to follow Langmuir adsorption isotherm and well fitted with pseudo second order kinetics.
Bradder et al. [50] have shown that adsorption capacity of GO does not depends upon the surface area, rather than surface chemistry of GO plays an important role where electrostatic attractions are responsible for increased adsorption capacity. He et al. [51] found that properties of GO can be significantly altered by the method of its synthesis. GO prepared from Hummers and modified Hummers method (HGO and HmGO, respectively), GO obtained from exfoliation of HGO and HmGO (HGeO and HmGeO, respectively) were compared for adsorption of MB. A surprising trend as HmGO>HGO>HmGeO>HGeO was obtained for the adsorption. The reason for adsorption trend favoring high adsorption of MB on graphite oxide was attributed to smaller sheets of single or few layered GO. This would decrease the number of MB molecules intercalated in the lamellar space of GO, which is not favorable for flocculation. The increased adsorption efficiency for HmGO and HmGeO when compared to HGO and HGeO, respectively, was attributed to modification in the Hummers method causing higher oxidation degree which induces more negative charge favorable for adsorption of cation MB. Liu et al. [52] prepared a lightweight GO sponge using centrifugal vacuum evaporation technique. Due to hydrophilic nature and condensed phase of GO the sponge was dispersed in the aqueous phase and adsorbed dyes efficiently. Dispersed GO was in millimeter sized which is easy to recover by vacuum filtration, contrary to nanosized GO sheets, which requires ultrahigh centrifugation and can also act as secondary pollutant. Adsorption was accredited to π–π stacking and ionic interaction between GO and dyes rich in aromatic rings and cationic atoms.
Table 1.1 Dye adsorption on GO-based materials.
Dye
Catalyst
BET surface area (m
2
g
−1
)
Adsorption capacity (mg g
−1
)
Adsorption kinetics
Adsorption isotherm
Reference
Methylene Blue
GO
28
351.1
Pseudo second order
Langmuir
[
50
]
HmGeO
–
597.0
Pseudo second order
Freundlich
[
51
]
HGeO[
51
]
–
549.5
Pseudo second order
Freundlich
[
51
]
GO sponge
–
389.8
–
–
[
53
]
GO sponge
48.4
396.9
Pseudo second order
–
[
52
]
GO
–
286.9
Pseudo second order
Sips
[
54
]
Congo Red
GO
124
12.56
Pseudo second order
Langmuir
[
55
]
Acridine Orange
GO
–
1,328
–
Langmuir
[
38
]
Congo Red
SRGO
–
2,158
–
Langmuir
[
55
]
Acid Orange 8
GO
–
25.6
Pseudo second order
Langmuir
[
56
]
Direct Red 23
GO
–
14.0
Pseudo second order
Langmuir
[
56
]
Basic Red 12
GO
133
63.7
Pseudo second order
Langmuir
[
57
]
Methylene Orange
GO
133
16.8
Pseudo second order
Langmuir
[
57
]
Malachite Green
GO
17
248.1
Pseudo second order
Langmuir
[
50
]
Methyl Violet
GO Sponge
48.4
402.7
Pseudo second order
–
[
52
]
Xiao et al. showed that rGO synthesized by using L-Cysteine have the ability to remove a large number of both cationic and anionic dyes [58]. In another study by Guo et al., hierarchical sandwiched nanocomposites of GO and Fe3O4 NPs synthesized by layer-by-layer assembly was utilized for the effective removal of dyes from wastewater as shown in Figure 1.4 [59]. In an interesting study, the dimensions and geometries of Fe3O4 NPs was tuned by taking the advantage of physical interactions attributed to surficial functionalities of GO as sulphonated GO to decrease the contact area of NPs. Such fabricated nanocomposites exhibited high regeneration capability [60]. Although GO and hybrid of GO-based material demonstrated high adsorptive removal of dyes but facile separation of adsorbent from aqueous environment is still a major issue due to the contamination of water with adsorbent as secondary pollutant and toxicity issues. To overcome the issues related with separation of adsorbent after water remediation magnetic composite of GO and hydrophobic GO, aerogels have been explored [61, 62].
Cheng et al. reported a facile synthesis of composite magnetic gel using GO and poly(vinyl alcohol)(PVA) (mGO/PVA CGs) showing high adsorption capacity of cationic dyes as MB and MV along with convenient magnetic separation capability [63]. The synthetic process of composite aerogel and magnetic capability for convenient separation is shown in Figure 1.5. A bioinspired nanocomposite material of PVA/poly(acrylic acid)/GO@polydopamine (PVA/PAA/GO-COOH@PDA) with high regeneration ability was also utilized for the removal of CR, RhB, and MB [64]. Polyacrylamide composite hydrogels of GO with self-healing capacity was utilized for the acceleration of adsorption of toxic dyes. The most significant capacity of such hydrogels was to rapid removal of dyes from hydrogels just by simple heating, which could be beneficial for regeneration [65].
Figure 1.4 Removal of organic dyes from water using hierarchical sandwiched nanocomposites of GO and Fe3O4.
Reprinted with permission [59].
Figure 1.5 Schematic illustration of the synthetic route to mGO/PVA CG.
Reprinted with permission [63].
Myung et al. reported a green synthesis of highly efficient aerogel composed of graphene nanosheets using pear as a raw material [68]. Such synthesized aerogels showed a significant potential for the the removal of a number of cationic and anionic dyes as shown in Figure 1.6, theses GO nanosheets exhibits metal ion removal capacity comparable to earlier reported metal organic framework (MOF), copper terephthalate and zeolite. Metal removal from water bodies has always been a crucial task due to the toxicity issues associated with heavy metal ions induce various harmful effects on both human and animals like neurological and immunological disorders, carcinogenicity, bio-accumulation, renal dysfunction, bone degradation, and liver and blood damage [66, 67]. Zhao et al. [69] synthesized few layered GO nanosheets (FGO) for the pH dependent and ionic strength independent removal of Pb(II). At low pH values dominating species is Pb(OH)+ which is easy to get adsorbed on FGO surface, whereas at higher pH values, Pb2+ exists in Pb(OH)3− ions, which cannot be adsorbed due to electrostatic repulsion with negatively charged FGO. Removal efficiency was reported to be increased with increase in temperature from 842 mg/g (293 K), 1,150 mg/g (313 K), and 1,850 mg/g (333K), denoting the adsorption process to be endothermic for Pb2+ ions. Sun et al. [70] studied the highly efficient adsorption of Eu3+ using GO nanosheets, which was reported due to the formation of surface complex between Eu3+ and GO. Li et al. [71] used GO single layered NS for adsorption of U6+. High adsorption of on GO NS was attributed to formation of inner complexes of U6+ on GO. Tan et al. [72] studied adsorption of Cu2+, Cd2+, and Ni2+ on GO membrane and found high adsorption attributed to Lewis base and Lewis acid interaction between surface functionalized GO and metal ions. The adsorption reached quickly at equilibrium due to large inter layer spacing of GO sheets and strong attraction forces between substrate and metal ions. Henriques et al. [73] synthesized GO foam and carried out Hg2+ adsorption. GO foam was functionalized with nitrogen and sulfur, where an increase in removal efficiency with nitrogen functionalization was observed.
Figure 1.6 Adsorption behavior of GAs toward different dyes; adsorption spectra of (a) MB, (b) Rh B, (c) MO, and (d) BG1 before and after 12 hof adsorption; inset show corresponding digital photographs. (e) Adsorption efficiency of GAs toward MB, Rh B, MO, and BG1 after 12 h ofadsorption. (f) Demonstration of the reusability of GAs toward adsorption of MB, Rh B, MO, and BG1.
Reprinted with permission [68].
Composite fabrication and surface functionalization are well known to introduce selectivity towards particular metal ions. For instance, chitosan/Sulfydryl-functionalized of GO was done for selective removal of Cu2+, Pb2+, and Cd2+ from single and multi-metal ions system [76]. MOF functionalized GO (IRMOF-3/GO) exhibits high selectivity towards Cu2+ with an absorption capacity of ~254.14 mg/g (Figure 1.7). Further, the IRMOF-3/GO membrane was fabricated using nano-filtration, which showed up to ~90% rejection of Cu2+ and high stability up to 2,000 min [77]. Alginate/rGO hydrogels is also reported for adsorptive removal of Cu2+ [78]. GO-chitosan and PVA composite hydrogel was fabricated via a freeze-draw physical cross-linking process to reduce the synthesis cost. This hydrogel was further applied for the removal of Cd2+ and Ni2+ [79]. Removal of Hg2+ was achieved by the functionalization of GO with 2-pyridinecarboxaldehyde thiosemicarbazone [80]. GO-MnO2 nanocomposite was explored for the simultaneous adsorptive removal of Th4+ and U6+ with the adsorption capacity of 497.5 mg/g and 185.2 mg/g, respectively [81]. Adsorption capacity and model kinetics of different metal ions on Go based materials is tabulated at Table 1.2.
Figure 1.7 Schematic diagram of the preparation of IRMOF-3/GO and the adsorption of Cu2+ on IRMOF-3/GO.
Reprinted with permission [77].
Other organic pollutants can also be removed from water bodies using GO and their composites as adsorbent material. Increasing contamination of PPCPs in water bodies has been a major concern as next-generation pollutants due to their significant activity at even lower concentrations [82]. Agricultural and industrial waste also contains pollutant compounds with notably unsaturated aromatic rings and oxygen rich functionalities that are difficult to degrade. Jiang et al. [83] carried out adsorption of 17β-estradiol (E2) on GO NS. Kyzas et al. [84] adsorbed Atenolol (ATL) and Propranolol (PRO). Adsorption was found to be of endothermic nature and high adsorption was attributed to the electrostatic interactions between GO and pollutants. Nam et al. [85] studied adsorption of diclofenac (DCF) and sulfamethoxazole (SMX) on GO. Wang et al. [86] tested naphthalene, phenanthrene, and pyrene adsorption on GONS. Unusual low adsorption of the pollutants on GO may result from interaction between hydrophobic pollutants and hydrophilic GO partially neutralizing the negative charge, increasing the aggregation tendencies, which may reduce adsorption affinity for high concentration of pollutants. Apul et al. [87] selected Phenanthrene (PNT) and biphenyl (BP) for adsorption over GO. GO has good adsorption capacity but when compared to graphene NSs uptake of the pollutants was lesser due to possibility of functional group present on GO surface making water clusters on surface, which could decrease the number of adsorption sites. Table 1.3 shows adsorption capacity and rate kinetics of different organic pollutants on GO base materials.
Table 1.2 Metal ion adsorption on GO materials.
Catalyst
Metal ion
Adsorption capacity (mg/g)
Model used
Reference
Few layered GO
Pb
2+
842 (293 K)
Langmuir
[
69
]
1,150 (313 K)
1,850 (333 K)
GO NSs
Eu
3+
175
Langmuir
[
70
]
GO single layered NS
Th
4+
411
Langmuir
[
74
]
GO single layered NS
U
6+
299
Langmuir
[
71
]
GO aerogel
Cu
2+
17.7 (283 K)
Langmuir
[
75
]
19.6 (298 K)
29.6 (313 K)
GO foam
Hg
2+
35
Langmuir
[
73
]
GO membrane
Cd
2+
83.8
Langmuir
[
72
]
Cu
2+
72.6
Ni
2+
62.3
Table 1.3 Organic pollutants’ adsorption on GO base materials.
Catalyst
Organic pollutant
Adsorption capacity (mg/g)
Model used
Rate kinetics
Reference
GONS
17β-estradiol
149.4
Langmuir
Pseudo second order
[
83
]
Few layered GO
Atenolol
67
Langmuir–Freundlich
Pseudo second order
[
84
]
Propranolol
116
GO
Diclofenac
43.9
Freundlich
–
[
85
]
Sulfamethoxazole
1.19
GO NS
Naphthalene
2.62
Langmuir
Pseudo second order
[
86
]
Phenanthrene
5.90
Pyrene
6.12
GO
Phenanthrene
174.6
Freundlich
–
[
87
]
Biphenyl
59.0
Highly porous GO-MOF composite was applied to remove anti-inflammatory drugs from water [88]. Yang et al. targeted the adsorption of a series of emerging contaminants including di-n-butyl phthalate (DnBP), cephalexin (CLX), di(2-ethylhexyl) phthalate (DEHP), caffeine (CAF), and sulfamethoxazole (SMX) by using graphene ceremics composite [89].
1.3 Carbon Nanotube
CNT is an attractive member of carbon family, which gained a huge interest in nanotechnology due to its unique structural and optoelectrical properties [90–94]. CNTs was first discovered by Iijima in 1991 [95]. CNTs are considered a tubular form of single graphite sheet and are classified as single walled CNTs (SWCNTs) and multi-walled CNTs (MWCNTs) depending on the number of layers sheet of graphite that has been rolled into a tube with single, double, or multiple walls (Figure 1.8) [96]. CNTs usually have a diameter varied from 0.1 nm to 10 nm and lenght can be varied upto few hundreds centimeters. CNT network generally consists of a hexagonal network of sp2 hybridized carbons. CNTs can be classified into three varieties of tubule structures (armchair, zigzag, and chiral) depending on the rolling up direction of the graphene sheet [97]. The difference in orientation controls electrical properties of the CNTs have direct impact on their electrical properties [90].
CNTs are highly studied for their excellent adsorption properties owing to high surface area, chemical interness and excellent stability [98]. Adsorption on CNT is dependent on its various physical and chemical properties like surface area, hydrophobic interactions, functionalization of basal structure, π−π bonds, electrostatic interactions, surface, and capillary condensation. Physio-chemical properties of adsorbing species like polarity, size and structure of the molecule, charge, pH, and ionization strength of the solution may also affect their extent and affinity for adsorption on CNTs. Though pristine CNT exhibits a hydrophobic nature, it can well adsorb non-polar molecule. Tuning the hydrophilicity by functionalizing the CNTs can increase the adsorption capacity for polar molecules [99]. Figure 1.9 shows change in affinity of CNT towards adsorption of polar and non-polar molecules on the basis of functionality. CNTs can be engineered into different structures with controlled orientation and configuration, which gives them further advantage to be used as a versatile adsorbent [99].
Figure 1.8 Diagrams of (a) single-walled CNTs (SWCNTs) and (b) multi-walled CNTs (MWCNTs).
Reprinted with permission [90].
Adsorption of polar molecules increases with the functionalization of CNT, whereas for non-polar molecules pristine CNTs were best adsorbents [100].
1.3.1 CNTs as Adsorbent
CNTs showed considerable potential for the removal of diverse metal ions and a range of toxic dyes from water owing to unique surface properties and tubular structure [101–104]. Mohammadi et al. observed the adsorption of toxic metal ions especially divalent heavy metal ions (Pb2+, Cd2+, Co2+, Cu2+, Zn2+) from water using CNT sheets [105]. The adsorption capability of CNT sheets were observed in the order of Pb2+ > Cd2+ > Co2+ > Zn2+ > Cu2+ due to the electrostatic interactions between negatively charged acidic functional groups on CNTs surface and posively charged metal ions. Another report by Pyrzynska et al. demonstrated the different affinity for the adsorptive removal of toxic metal ions using CNTs and it follow the order of Cu2+ > Pb2+ > Co2+ at pH 9 [106]. Mao et al. observed adsorption of MB onto CNTs because of attribute to interactions of MB with SWNTs [107]. Gong et al. studied the adsorption of cationic dyes including brilliant CB, MB and neutral red by magnetic MMWCNTs nanocomposite and adsorption capacity follow the order of MB > neutral red > brilliant CB [108]. Yao et al. reported a high adsorption capacity up to 35 mg/g at 298 K for the removal of MB onto CNTs [109]. Adsorption capacity by CNTs for different dyes was tabulated in Table 1.4.
Figure 1.9 Effect of functionalization of CNTs on adsorption of polar and non-polar molecules [99].
Reprinted with permission [99].
It is observed that oxidation or surface functionalization of CNTs significantly improved the adsorption capacity [115]. Several factors, such as pH of solution, ionic strength, dose of catalyst, temperature, concentration of toxic metal ions in wastewater, and other factors have considerable impact towards the removal of contaminants from wastewater. The adsorption of cobalt over CNTs were varied with pH from 3 to 9; sharp increase in adsorption was observed with increase in pH [106]. Low adsorption at low pH due to competition between H+ and Co2+, while pH attributed to the surface negative charge which facilitates more adsorption of metal ions. M. Ghaedi et al. observed that adsorption capacity of both morin and ARS have inversely depended on pH over range 1 to 5 [116]. Increased adsorption at low pH due to enhanced electrostatic interaction between anionic dye and protonated surface functional groups. Presence of other ions adversely affected the adsorption of targeted metal ions [115]. Decrease in adsorption was reported for Ni2+, Cd2+, Cu2+, and Pb2+ by various research groups observed in presence of high ionic strength [117, 118]. Amount of adsorption for the metal ions like Pb2+, Ni2+, Cd2+, and Cu2+ were observed with increase the loading of CNTs due to increase in surface active sites, which facilitates better interaction between surface functional groups with toxic metal ions [114, 119]. Similar phenomenon were observed for dyes where enhancement of adsorption capacity with increasing adsorbent dosage was attributed to increase in surface adsorption sites along with enhanced surface area of CNTs [116]. From the available literature, it was observed that the adsorption efficiency of CNTs increases with temperature because of efficient mobility of the metal ions, dyes towards catalytic surface, and easily overcome lower activation energy barrier during adsorption processes [110, 111, 116]. Generally, adsorption of metals, dyes over CNTs were preferably follow Langmuir or the Freundlich model. Langmuir isotherm preferably useful for uniform surface coverage, where there is no interaction between adsorbate molecule [111, 115]. On the other hand, Freundlich isotherm for the heterogeneous surfaces where interaction between molecules takes place. Adsorption of toxic Cr6+via MWNTs-poly(acrylic acid) (PAA)–poly(4-amino diphenyl amine) (PADPA) preferably follow by Freundlich isotherm as reported by Kim et al. [120]. In another report, adsorption of Ni(II) over MWCNTs preferably follow Langmuir adsorption isotherm because of no observed interactions between Ni2+ and MWCNTs along with high active surface area [121]. Wu et al. reported adsorption efficiency of CNTs for Procion Red and MX-5B follow Freundlich isotherms [110].
Table 1.4 Maximum adsorption capacities for different dyes with CNTs.
Adsorbates
Adsorbents
Adsorption capacity, Q (mg/g)
Model used
Reference
MWCNTs
Procion red MX-5B
44.68
Langmuir
[
110
]
MWCNTs
Sufranine O
43.48
Langmuir
[
111
]
MWCNTs
Acid red 18
166.67
Langmuir
[
112
]
Oxidized MWCNTs
Bromothymol blue
55
Langmuir
[
113
]
MWCNTs
Methyl violet
71.76
Langmuir
[
114
]
CNTs
Methylene blue
64.7
Langmuir
[
109
]
SWCNT and MWCNT composite membrane was fabricated for the removal of PPCPs including triclosan (TCS), ibuprofen (IBU), and acetaminophen (AAP) having the removal efficiency from 10%–95% in the order of AAP≈IBU<TCS [122]. Zhu et al. reported a simple process for the synthesis of magnetic CNTs composite, which was further used for the removal of triclosan from water [123].
1.4 Conclusion
Carbon-based nanomaterials such as CNTs, graphene, and GO are emergently spotlighted for the fabrication of adsorbent material due to their excellent physical and chemical properties and surface characteristic. Nanocomposites of CNTs and GO with diverse materials are of great interest for water remediation attributable to the simultaneously enhance a variety of properties without sacrificing any material properties. Nanocomposites of CNTs and GO offer a significant advantage of excellent adsorption capacity for a range of contaminants including toxic dyes, heavy metal ions PPCPs, and many more. On the other hand, proper functionalization of CNTs allows its easy removal of toxic and carcinogenic pollutants such as metal ions, complex organic dyes and other next-generation pollutants. Key tools like kinetics, thermodynamics, and adsorption isotherm are successfully explained along with overall adsorption mechanism for both GO and CNTs. In spite of being extensively studied for their preparation and application in practical use, it is still required to reduce gap between a laboratory scale experiment and their use in actual WWTPs. This can be the focus to conduct further study for remediation of water resources.
Acknowledgements
RKG acknowledges financial assistance from Department of Science and Technology (DST), India, through the INSPIRE Faculty Award (Project No. IFA-13 ENG-57) and Grant No. DST/TM/WTI/2K16/23(G). KMT acknowledges financial assistance from National Research Foundation of Korea (Grant No. 2019R1G1A1008879).
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