graphite figure_01         Here we go again. After intercalated compounds of graphite (1974), fullerenes (1985), and carbon nanotubes (1991), it is time for another allotrope of elemental carbon to be at the forefront of scientific curiosity (Boehm 2010). The allotrope is: “graphene”. By graphene, we mean the basal plane of graphite, a one atom thick two dimensional honeycomb layer of sp2 bonded carbon. Conversely, when many graphene layers are stacked regularly in three dimensions, graphite is created.


In the introductory chapter of the book, Graphite, Graphene, and Their Polymer Nanocomposites; editors have laid out their vision for this nascent and exciting area of research. They have also briefly described the contents of the each of the chapters and explained the logic that binds them into a compelling book. This allows the readers to derive the maximum benefit from the developing story of the most sought after carbonaceous nanomaterial, graphene. Clearly, there are a very large number of both challenges and opportunities in the area of graphene research. Plasticstrends is pleased to provide to its readers a revealing look at the contents of this book. 




Why such an interest in graphene? It’s all about the digital world, and the search for materials which will make integrated circuits smaller, faster and cheaper! Graphene is a semiconductor with a zero band gap and an exceptionally-high charge mobility. In fact, electron mobilities in graphene could reach values that are more than an order of magnitude higher than those encountered in a Si transistor. This opens up the tantalizing possibility that one day graphene might replace silicon as the building block of the electronic industry and revolutionize nanoelectronics. Although the existence of graphene
had been known for a long time, the material had never been actually synthesized. This had to await the work of Andre K. Geim and Konstantin S. Novoselov of the University of Manchester, UK who were awarded the 2010 Nobel Prize in Physics for their ability to isolate a defect free, single sheet of carbon atoms through micromechanical cleavage of graphite whereby monolayers are peeled from graphite crystals (Novoselov 2004). This method, however, produces a very small amount of pristine graphene which makes it unsuitable for efficient and scalable high volume manufacturing. Nevertheless, this pioneering work paved the way to the rise of intense graphene research. Important characteristics of graphene are that it is nano-scale in dimension, and it is derived from graphite, an inexpensive precursor. Consequently, a key goal of world-wide research has been to produce a large enough volume of pristine graphene safely and in a cost efficient manner. Other researchers are seeking practical
applications of graphene that will benefit society, especially in the electronics area.


In the technical literature, a number of methods have been described for producing graphene. These can broadly be classified as 1) micro-mechanical exfoliation, 2) epitaxial growth of graphene films, 3) chemical vapor deposition, 4) Unzipping of carbon nanotubes, and 5) reduction of graphene oxides. Each method has its own benefits and related drawbacks. A “bottom-up” approach using chemical synthesis is an interesting strategy (Choucair 2009, Cai 2010). However, scaling-up to produce large quantities remains a formidable challenge. Research efforts have, so far, established that an easier route to
manufacture large amounts of graphene is via the chemical exfoliation strategy. During chemical exfoliation, such as oxidation and subsequent reduction of graphite oxides, one produces partially or highly reduced graphene oxides. From a chemical viewpoint, these graphene sheets contain various types of residual oxygen-containing species. From a physical viewpoint, graphene sheets become
corrugated, and the graphene platelets can contain a variety of defects such as topological, adatoms, edges/cracks, vacancies, loops, adsorbed impurities and so on within the graphene-like structures (Terrones 2010). When the dimensions of these platelets fall in the nano-scale range, they are commonly termed “graphene nano-platelets” (GNPs). One of the most technologically promising
applications of nano-graphene materials is in polymer reinforcement. Studies have shown that stress transfer takes place from the polymer matrix to mono-layer graphene, indicating that graphene acts as a reinforcing phase (Gong 2010).


Polymers have been combined with other polymers to form blends and copolymers, mixed with talc, calcium carbonates and clays to give filled systems and extruded and molded with fibers and other anisotropic reinforcements to yield composites and hybrid materials. This simple “mix and match” approach has allowed the polymer scientists and engineers to utilize a small library of polymers to produce a bewildering array of useful products capable of possessing extremes of property values. Traditional filled-polymer composites typically utilize high loadings of micron sized filler particles to obtain desired properties. If the filler particle size is reduced to its nano-scale dimension from its micron size, similar properties are achieved but with a drastically reduced filler loading level to achieve percolation.
Primarily, this is due to the surface area to volume ratio of the nanoparticles which is several orders of magnitude larger than that of micron-sized fillers. To qualify to be called a “nanoparticle”, the particle has to have at least one dimension in the nanometer range. Therefore, when nanometer particles are dispersed in a polymer matrix the result is termed as “Polymer nanocomposite” (PNC); the matrix itself can be single or multiphase. The critical reinforcing effects of nanosized particles come from its aspect ratio, very large specific surface area, and the particle-matrix interactions. The original concepts for PNCs owe their origin to the invention of polyamide-clay composites in the Toyota Research Corporation in 1985 (Okada 1988). At that time, the objective was to make plastics used in under-the-hood applications be heat resistant and lighter than metal. Since then, the list of nano-particles has grown and PNCs have seen numerous commercial applications ranging from auto parts to packaging to coatings (Ashton 2010).


The latest addition to this palette of nanomaterials is graphene. Graphene layers could be stacked, functionalized, and modified to provide numerous types of graphene-based nano-scale materials. Rolled-up graphene, known as carbon nanotubes (CNTs) also has some structural flexibility. However, the performance and cost advantages of graphene challenge CNTs in nanocomposites, coatings, sensors, and energy storage device applications. For instance, the quality of graphene’s crystal and band structures yields uniquely low noise levels, increasing the sensitivity of the sensors (Yang 2010). While incorporation of CNTs in large scale integrated electronic architectures is a daunting task, graphene is highly amenable to microfabrication (de Heer 2007).  On the other hand, the cost advantage of graphene, graphene oxides or its nanoplatelets over CNTs stems from easy access to the graphitic precursor material, the cost, and the scalable method. In addition, due to its structure, graphene raises fewer toxicity issues as compared to carbon nanotubes.


This book attempts to compile, unify and present the emerging research trends in graphene-based polymer nanocomposites (GPNC). Researchers from several disciplines across the continents share their expertise and research knowledge about graphene, its properties, and the behavior of graphene-based composites. To the best of our knowledge, there is no other published monograph that provides this kind of a comprehensive snapshot of graphite, graphene, and their polymer nanocomposites. Without a broad perspective of the underlying physics and the chemistry of graphene, the full story of GPNC
remains untold. That is indeed our premise, and this is where the story begins.


Organization of the chapters


In chapter 1, John Zondlo from West Virginia University (USA) introduces us to natural and synthetic graphite, their properties and characterization techniques; graphite, after all, is the precursor to graphene.
The chapter lucidly describes where natural graphite is found and how synthetic graphite is manufactured. The author lists the prominent commercial applications of graphite in this chapter.


graphite figure 1 graphite figure 2

A graphite replacement heart valve (left), and graphite piston for a high-performance racing
engine (right). (Reproduced with permission from CRC Press)


It is evident that societal growth would be impeded without the use of graphite. Applications range from graphite electrodes in the electric arc furnace to graphite refractories in the steel and aluminum industries to nuclear reactors as both a moderator and a reflector.


graphite figure 3

Prismatic graphite structures in the core of a high-temperature nuclear reactor. (Reproduced with
permission from CRC Press)



A description of the importance of the different forms of graphite provides the link to the next few chapters.


Chapters 2 and 3 prepare us about graphene and its unique characteristics. Pierre Carmier of CEA-INAC / Université Joseph Fourier, Grenoble (France) elaborates in chapter 2 as to what has made graphene to climb to the top of the materials research chart. The author enumerates the electronic transport properties of graphene and explains how graphene's bipartite Bravais lattice and its gapless band structure make graphene so exotic! While delving into the theoretical issues of graphene, the author reminds us about the obstacles that have to be overcome for real carbon-based electronics. Most of us will agree that characterization of graphene is one of the most critical tasks in graphene research. Once graphene is synthesized, there are numerous techniques for its characterization. However, some of these are still evolving as technology advances. In chapter 3, Viera Skakalova and Dong Su of Max-Planck Institute, Stuttgart (Germany) and Alan B. Kaiser of Victoria University of Wellington (New Zealand) address this critical task. Not only do the authors summarize different characterization techniques available in microscopy (AFM, SEM, TEM, STM), and in spectroscopy (Raman, Augur, ARUPS, XPS) but they also discuss unique features of electrical conduction properties depending on the degree and the nature of defects in graphene.


graphite figure 4


SEM image of a CVD-grown graphene sheet on a nickel-coated SiO2/Si substrate (a) for 30
seconds and (b) for 7 minutes, and (c) Raman spectra of a CVD-grown graphene sheet on a
nickel-coated SiO2/Si obtained from different positions on the sample (scale bar: 1?m). (From
Park, H.J. et al., Carbon, 48, 1088-94, 2010. With permission)


The authors conclude this chapter by highlighting thermal conduction properties of graphene and how the thermoelectric power of graphene could aid in thermoelectric conversion of heat to electrical energy.


In the “top-down” approach, exfoliation of graphite is the key to the preparation of single or multiple graphene nanosheets. The quality of graphene materials can vary depending on the preparative methods. In reality, only cost-effective approaches to produce graphene sheets in large quantities would have commercial importance. In chapter 4, Martin Matis, Urszula Kosidlo, Friedemann Tonner, Carsten Glanz, and Ivica Kolaric of Fraunhofer Institute for Manufacturing Engineering and Automation, Stuttgart (Germany) detail electrochemical exfoliation of graphite and recent advances in the process. In addition to low cost, this exfoliation process has the advantage of producing functionalized graphene nano-platelets (GNP) in bulk quantities which is crucial to graphene-based nanocomposites manufacturing. In chapter 5, Weifeng Zhao and Guohua Chen of Huaqiao University (China) discuss different exfoliation routes to producing graphene and graphite nano-platelets for their use in polymer composites.



graphite figure 5


Dispersion properties of electrochemically derived graphite oxides before and after organic
modification with CTAB. Reproduced from H.W. Hu, G. Chen et al. Synthetic Met. 2009,


Numerous studies on polymer based graphene nanocomposites are discussed. Ways to bring graphene nanomaterials into the real world of polymer processing were critically examined. The chapter authors propose the use of the wet ball-milling method to further exfoliate graphite nano-platelets into graphenes. Both chapters 4 and 5 describe possible routes to bringing graphene in bulk quantities to the market.


Chapters 6 through 9 showcase how graphene as the newest nano-materials can be used in numerous applications of commercial interest. Most of us will agree that clean energy is essential for securing the future of our planet. Chapter 6 deals with emerging clean energy applications of graphene-based materials in solar cells, lithium ion batteries, supercapacitors, and catalysis. Bin Luo, Minghui Liang, Michael Giersig, and Linjie Zhi of the National Center for Nanoscience and Technology, Beijing (China) discuss each of the clean energy applications in depth and provide a glimpse of graphene’s applications in the domain of clean energy technology.



graphite figure 5 a


Schematic illustration of the synthesis and structure of SnO2/GNS. (Reprinted with permission
from S.M. Paek, E. Yoo, et al. Nano Letters. 2009. 9(1): 72-75. Copyright 2009 American
Chemical Society)


These authors cite an impressive number of studies available in the current literature to capture the progress and future directions of each of these technologies. Because of its versatile application potential, the authors surmise that graphene could be used as a base material for various optoelectronic devices in the future. Martin Pumera of Nanyang Technological University (Singapore) delves into the electrochemistry of graphene-based nano-materials in chapter 7. It is known that chemical activity drastically changes at the edges of graphene depending on their carbon termination.  However, the author argues that there is no significant difference between the electrochemical response of single-, few-, and multi-layer graphene sheets. He discusses the importance of electrochemical performance of graphene
nano-structures in applications such as sensing and bio-sensing, supercapacitors and batteries.


Chapter 8 examines the fabrication of graphene-polymer nanocomposites and their applications as saturable absorbers for pulse lasers. Both graphene-based Q-switched lasers and mode-locked laser are examined. In this chapter, Kian Ping Loh, Qiaoliang Bao, Dingyan Tang, and Han Zhang of Nanyang Technological University (Singapore) show that the functionalization of graphene via covalent linking of a dye to the basal plane, and non-covalent attachment of aromatic molecules, aids in tuning the optical properties. The authors believe that electrospun graphene-polymer nanocomposites are promising candidates for practical and efficient photonic materials in the generation of high energy or ultrashort pulses.


graphite figure 6

Schematic illustration of the fabrication of graphene-polymer nanofiber composite by
electrospinning. (From Bao, Q. et al., Adv. Funct. Mater., 20, 782-791, 2010. With permission.) 


Epoxies are a class of thermoset polymers utilized extensively in products ranging from floor coatings to aircraft fuselages. Chapter 9 written by Iti Srivastava, Mohammad A. Rafiee, Fazel Yavari, Javed Rafiee, and Nikhil Koratkar of Rensselaer Polytechnic Institute, New York (USA) discusses the potential of graphene as a nanofiller in epoxy-based composite materials technology. The practical relevance of the nanocomposites’ mechanical properties such as tensile strength, Young’s modulus, buckling resistance, and ductility to material properties including fracture toughness and fatigue resistance are examined. The authors demonstrate that the graphene content required to significantly boost the mechanical properties of epoxy systems is 1-2 orders of magnitude lower than with the use of other competing nanofillers such as carbon nanotubes, nano-clays as well as silica/aluminum/titania nano-particles. The process of making hierarchical graphene/epoxy/E-glass fiber composites and their properties is also discussed. Finally, the authors have summarized technical issues that require attention in order to realize the full potential of graphene-based epoxy nanocomposites.


Nanoparticles come in different shapes and sizes. Chapter 10 provides an overview of the various types of nanofillers (ranging from metallic nanoparticles to silicates to bio-source nanoparticles to CNTs and graphenes) and reviews issues related to their polymer nanocomposites. This chapter authored by Musa R. Kamal and Jorge Uribe-Calderon of McGill University, Montreal (Canada) discusses challenges during the preparation of polymer nanocomposites. Chapters 11 and 12 address two distinctly different methods of GPNC preparation. Instead of employing the conventional route to polymer nanocomposites preparation, such as solution or melt mixing, Chapter 11 reveals how a robust and yet a simple technique for controlled polymerization, namely Atom Transfer Radical Polymerization (ATRP), is utilized to produce graphene-based polymer nanocomposites. Chapter 11 written by Arun K. Nandi, Rama K. Layek, Sanjoy Samanta, and Dhruba P. Chatterjee of the Indian Institute
for the Cultivation of Science, Kolkata (India) discusses the work of these authors and suggests that the ATRP method has the potential to fine tuning various properties of graphene-based polymer nanocomposites. Chapter 12 deals with the synthesis of GPNCs in a biodegradable polymer matrix and utilizes a solution mixing procedure. In this chapter, Gui Lin and James E. Mark of the
University of Cincinnati (USA) and Isao Noda of The Procter & Gamble Company, Ohio (USA) report on the structure-mechanical properties relationships of PHBHx reinforced by expanded graphite, graphene oxide and reduced graphene oxide.


Chapters 13 through 15 are devoted to the specialized properties of graphene-based polymer nanocomposites.


In chapter 13, Olga Shepelev and Samuel Kenig of Shenkar College of Engineering & Design, Ramat Gan (Israel), explore the opportunities to modify graphene nanoplatelets via surface treatment.



graphite figure 7


SEM image of PP / GNP nanocomposites containing modified GNP with polyol/silica
combination. (Reproduced with permission from CRC Press)


The authors compounded treated graphene into a polypropylene matrix to prepare polymer nanocomposites and showed that the treatments improved nanocomposite properties. Chapter 14 deals with water vapour barrier properties of GPNCs. In this chapter, Mathew Thompson, Sushant Agarwal, Rakesh K. Gupta of West Virginia University (USA), and Prithu Mukhopadhyay of IPEX Technologies Inc., Verdun (Canada) describe the process of molecular diffusion through polymers and show that graphene based PNCs have similar barrier behavior to clay-based PNCs, but the loading level of graphene needed is much lower. However, the authors question if the permeability reduction in the nanocomposite is due to diminished diffusion coefficients or lowered solubility of the diffusing molecule! These results
make out a case for the development of an appropriate theory for diffusion through PNCs. Chapter 15, authored by J.S. van der wal of Composite Agency, Amsterdam (The Netherlands), addresses chemically driven expansion of polymers within a composite structure, another important issue for long term service life of a product. Using methanol as a diffusing molecule, the author shows how a small amount of functionalized graphene sheets enhances the interfacial robustness of an epoxy composite.


In chapter 16, a review of graphene/polymer nanocomposites is reproduced. Here, Hyunwoo Kim, Ahmed A. Abdala (The Petroleum Institute, Abu Dhabi, UAE), and Christopher W. Macosko of the University of Minnesota, Minneapolis (USA) provide a lucid perspective of graphene based polymer nanocomposites research. Chapter 17 is concerned with preparation, properties and limitations of highly filled graphite-polymer composites. Improved electrical conductivity of graphite is attractive for the preparation of bipolar plates for the proton exchange membrane (PEM) used in fuel cells. This chapter coauthored by Sadhan C. Jana and Ling Du of University of Akron, Ohio (USA) employed a synergistic combination of expanded graphite and electrically conductive carbon black in epoxies to examine both in-plane and through-plane electrical conductivity.


The Opportunities and the Challenges


Graphene research has caught the world’s attention. Start-upcompanies that supply graphene materials are emerging in different parts of the world, and nanomaterials providers are adding graphene into their
product portfolio. Market research entities are totaling graphene sales numbers and projecting encouraging future sales volumes. Even governments are allocating money for funding graphene research. From a commercial standpoint, this is indeed good news for graphene-based polymer nanocomposites. This new material is entering a crucial segment in its product lifecycle from innovation to applications. But challenges still need to be overcome in order to bring about synergy between graphene research and its myriad anticipated applications.


The chemistry part of graphene and its derivatives has, however, begun to unfold. Graphene sheets are individually very strong, but, in graphite, sheets slide past one another making the material soft as is the case with pencil lead. Likewise, the thermal conductivity of suspended graphene differs considerably from graphene grown via chemical vapor deposition (CVD). Although composed of identical atoms, only differently arranged, the material properties are drastically different. Can the basal surface of graphene be made reactive? A knowledge of the interactions at the liquid-graphene interfaces is crucial to the application of graphene in electrochemical energy storage systems. So is the understanding and control of hydrophobic interactions in the field of protein folding and self-assembly. Studies are being conducted to examine the controllable interaction of water with epitaxial graphene films of different thickness values (Zhou 2012). Indeed, graphene’s wetting transparency comes from its extreme thinness. How one can exploit the wetting response in the design of conducting, conformal, and impermeable surface coatings (Rafiee 2012)? Only future studies will tell! Curiosity will find one day what happens to graphene when it is subjected to high compression. These new pieces of information will allow researchers to continue to address fundamental questions that go to the very core of our understanding of chemical interactions in
materials while simultaneously opening the doors to innovative applications.


The synthesis and properties of graphene nanoplatelets, its oxides, and the control of type and quantity of oxygen containing species have been the research foci of the graphene-based nanocomposites community (Terrones 2011, Mukhopadhyay 2011, Potts 2011). Strategies such as electrolytic exfoliation, ball milling or microwave heating are being advanced as the means of obtaining single, few and multi-layered graphene flakes in bulk quantities. Spectroscopic techniques (Raman, SEM, TEM, AFM, XPS, Auger, ARUPS) are being used to understand surface and edge chemistry of graphene. The various techniques are needed since the morphology of graphene sheets changes when they are derived from different synthetic routes. A proper characterization of graphene is critical to understanding and exploiting GPNC properties. To tailor polymer chain length and molecular weight, modern synthetic tools (ATRP, RAFT, NMRP) could be used to develop application-specific GPNCs.


Graphene-based composites could be used in well-established technologies (cars, aircrafts, fuel cells etc.) as well as in emerging green-technologies (solar cells, batteries, catalysis). For instance,
transparent and conducting GPNCs could replace indium tin oxide one day. While not necessarily transparent, highly-conducting GPNCs could find applications in nano-electromechanical systems. In structural applications, the buckling resistance of a composite material is of immense practical interest. So is the load transfer and understanding of fatigue life. Studies are piling up to develop engineering data and design guidelines for GPNCs. Then there are applications that can only be dreamed about.


One of the major obstacles in the path to progress is to understand the detailed evolution of chemical structures during oxidation/reduction and controlled functionalization of graphene. A range of defects in a graphene-like structure can influence the physico-chemical properties of graphene. The path forward is then to accurately identify the defects and to systematically quantify them. Essentially, these defects pose challenges but also afford opportunities to anchor polymer chains to the surface and thereby maximize the application potential of synthesized GPNCs. Although CNTs and graphene appear
to provide comparable mechanical and electrical properties, graphene-based composites potentially provide larger thermal conductivity enhancements and superior barrier properties than CNT-based composites. Graphene nanocomposites, when used as thermal interface materials, outperform those containing CNT or metal nano-particles due to graphene’s aspect ratio and lower Kapitza
resistance at the composites interface (Khan 2012). The problem with barrier studies, however, is the lack of comprehensive data and a suitable model to better understand barrier properties of GPNCs.


Nonetheless, the main challenge that remains: how to produce a large enough volume of graphene safely and in a cost efficient manner. That’s where the stage is set and the race is on.


The study of graphene-based polymer nanocomposites is a multi-disciplinary research field. Latest breakthroughs can emerge only when convergent thinking of various fields meet and learn from one another’s work. The tree of knowledge of several branches such as chemistry, physics, and biology to chemical, mechanical, electrical, and civil engineering can allow the rise of graphene to attain its true potential. Meaningful advancements to bridge the gap between GPNC research and its applications are likely to occur only if a broader scientific and engineering perspective is in view. This is what each of the chapter authors, who is a specialist in his or her own field, brings to the fore in the story of Graphite,Graphene, and Their Polymer Nanocomposites. We hope that this book will contribute to the advancement of both science and technology in this exciting area.




One of the editors, Prithu Mukhopadhyay, would like to thank IPEX Technologies Inc. for allowing him to dabble in polymer science and technology with a keen eye for commercial
development of products.

Plasticstrends appreciates the permission granted by CRC press, to publish the introductory chapter from the book “Graphite, Graphene, and Their Polymer Nanocomposites”.  To learn more about the book, please visit





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Prithu Mukhopadhyay

Prithu Mukhopadhyay is a Scientist with IPEX Technologies Inc. in Montreal, Canada. Since 1997, he has been engaged in R&D as well as manufacturing and quality management for
injection molding and extrusion. He earned his master’s degree in organic chemistry and his Ph.D. in polymer chemistry from the Indian Institute of Technology, Kharagpur. He came to
Montreal, Canada in 1991 as a post-Doctoral fellow in chemical engineering at Ecole Polytechnique after having worked as a chemist for the Oil and Natural Gas Commission of
India. Prithu is passionate about new plastics technologies, and he has been a member of the New Technology Committee of the Society of Plastics Engineers since 1998. He has chaired the
committee in the past, and he has been active in developing New Technology Forums at the Annual Technical Conference of the Society since 2000. He is an expert on plastics piping
materials, and he has published and spoken extensively on this and a variety of polymer topics. He is the founding editor of Plasticstrends, an educational web site that was established in 2000.

Rakesh K. Gupta

Rakesh K. Gupta is George B. and Carolyn A. Berry Professor and Department Chairman of Chemical Engineering at West Virginia University where he has been teaching since 1992. He
holds B. Tech. and Ph.D., degrees in chemical engineering from the Indian Institute of Technology, Kanpur, and the University of Delaware, respectively. Before coming to WVU, he
taught at the State University of New York at Buffalo for 11 years. He has also worked briefly for the Monsanto and DuPont Companies. His research focuses on polymer rheology, polymer
processing, and polymer composites. He has published more than 100 journal papers, 65 conference papers and 12 book chapters on these topics. He also holds three U.S. patents. He is
the author of Polymer and Composite Rheology, the coauthor of Fundamentals of Polymer Engineering and the coeditor of Polymer Nanocomposites Handbook.