Graphene’s success has shown that it is possible to create stable, single and few-atom-thick layers of van der Waals materials, and also that these materials can exhibit fascinating and technologically useful properties. Here we review the state-of-the-art of 2D materials beyond graphene. Initially, we will outline the different chemical classes of 2D materials and discuss the various strategies to prepare single-layer, few-layer, and multilayer assembly materials in solution, on substrates, and on the wafer scale. Additionally, we present an experimental guide for identifying and characterizing single-layer-thick materials, as well as outlining emerging techniques that yield both local and global information. We describe the differences that occur in the electronic structure between the bulk and the single layer and discuss various methods of tuning their electronic properties by manipulating the surface. Finally, we highlight the properties and advantages of single-, few-, and many-layer 2D materials in...

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Progress, Challenges, and Opportunities in Two-Dimensional Materials Beyond Graphene

Nitrogen-doped graphene (N-graphene) was synthesized by chemical vapor deposition of methane in the presence of ammonia. The resultant N-graphene was demonstrated to act as a metal-free electrode with a much better electrocatalytic activity, long-term operation stability, and tolerance to crossover effect than platinum for oxygen reduction via a four-electron pathway in alkaline fuel cells. To the best of our knowledge, this is the first report on the use of graphene and its derivatives as metal-free catalysts for oxygen reduction. The important role of N-doping to oxygen reduction reaction (ORR) can be applied to various carbon materials for the development of other metal-free efficient ORR catalysts for fuel cell applications, even new catalytic materials for applications beyond fuel cells.

/pdf/nitrogen-doped-graphene-as-efficient-metal-free-2c5sl934bm.pdf

Nitrogen-Doped Graphene as Efficient Metal-Free Electrocatalyst for Oxygen Reduction in Fuel Cells

Approaches, Derivatives and Applications Vasilios Georgakilas,† Michal Otyepka,‡ Athanasios B. Bourlinos,‡ Vimlesh Chandra, Namdong Kim, K. Christian Kemp, Pavel Hobza,‡,§,⊥ Radek Zboril,*,‡ and Kwang S. Kim* †Institute of Materials Science, NCSR “Demokritos”, Ag. Paraskevi Attikis, 15310 Athens, Greece ‡Regional Centre of Advanced Technologies and Materials, Department of Physical Chemistry, Faculty of Science, Palacky University Olomouc, 17. listopadu 12, 771 46 Olomouc, Czech Republic Center for Superfunctional Materials, Department of Chemistry, Pohang University of Science and Technology, San 31, Hyojadong, Namgu, Pohang 790-784, Korea Institute of Organic Chemistry and Biochemistry, Academy of Sciences of the Czech Republic, v.v.i., Flemingovo naḿ. 2, 166 10 Prague 6, Czech Republic

Functionalization of Graphene: Covalent and Non-Covalent Approaches, Derivatives and Applications

Graphene based materials: Past, present and future

Nitrogen doping has been an effective way to tailor the properties of graphene and render its potential use for various applications. Three common bonding configurations are normally obtained when doping nitrogen into the graphene: pyridinic N, pyrrolic N, and graphitic N. This paper reviews nitrogen-doped graphene, including various synthesis methods to introduce N doping and various characterization techniques for the examination of various N bonding configurations. Potential applications of N-graphene are also reviewed on the basis of experimental and theoretical studies.

https://s3-eu-west-1.amazonaws.com/pfigshare-u-files/1431849/NitrogenReviewonRecentProgressinNitrogenDopedGrapheneSynthesisCharacterizationandItsPotentialApplications.pdf

Review on Recent Progress in Nitrogen-Doped Graphene: Synthesis, Characterization, and Its Potential Applications

To realize graphene-based electronics, various types of graphene are required; thus, modulation of its electrical properties is of great importance. Theoretic studies show that intentional doping is a promising route for this goal, and the doped graphene might promise fascinating properties and widespread applications. However, there is no experimental example and electrical testing of the substitutionally doped graphene up to date. Here, we synthesize the N-doped graphene by a chemical vapor deposition (CVD) method. We find that most of them are few-layer graphene, although single-layer graphene can be occasionally detected. As doping accompanies with the recombination of carbon atoms into graphene in the CVD process, N atoms can be substitutionally doped into the graphene lattice, which is hard to realize by other synthetic methods. Electrical measurements show that the N-doped graphene exhibits an n-type behavior, indicating substitutional doping can effectively modulate the electrical properties of graphene. Our finding provides a new experimental instance of graphene and would promote the research and applications of graphene.

Synthesis of N-Doped Graphene by Chemical Vapor Deposition and Its Electrical Properties

Unresolved problems associated with the production of graphene materials include the need for greater control over layer number, crystallinity, size, edge structure and spatial orientation, and a better understanding of the underlying mechanisms. Here we report a chemical vapor deposition approach that allows the direct synthesis of uniform single-layered, large-size (up to 10,000 μm2), spatially self-aligned, and single-crystalline hexagonal graphene flakes (HGFs) and their continuous films on liquid Cu surfaces. Employing a liquid Cu surface completely eliminates the grain boundaries in solid polycrystalline Cu, resulting in a uniform nucleation distribution and low graphene nucleation density, but also enables self-assembly of HGFs into compact and ordered structures. These HGFs show an average two-dimensional resistivity of 609 ± 200 Ω and saturation current density of 0.96 ± 0.15 mA/μm, demonstrating their good conductivity and capability for carrying high current density.

https://www.pnas.org/content/pnas/109/21/7992.full.pdf

Uniform hexagonal graphene flakes and films grown on liquid copper surface

We report the metal-catalyst-free synthesis of high-quality polycrystalline graphene on dielectric substrates [silicon dioxide (SiO2) or quartz] using an oxygen-aided chemical vapor deposition (CVD) process The growth was carried out using a CVD system at atmospheric pressure After high-temperature activation of the growth substrates in air, high-quality polycrystalline graphene is subsequently grown on SiO2 by utilizing the oxygen-based nucleation sites The growth mechanism is analogous to that of growth for single-walled carbon nanotubes Graphene-modified SiO2 substrates can be directly used in transparent conducting films and field-effect devices The carrier mobilities are about 531 cm2 V–1 s–1 in air and 472 cm2 V–1 s–1 in N2, which are close to that of metal-catalyzed polycrystalline graphene The method avoids the need for either a metal catalyst or a complicated and skilled postgrowth transfer process and is compatible with current silicon processing techniques

Oxygen-Aided Synthesis of Polycrystalline Graphene on Silicon Dioxide Substrates

The ability to dope graphene is highly important for modulating electrical properties of graphene. However, the current route for the synthesis of N-doped graphene by chemical vapor deposition (CVD) method mainly involves high growth temperature using ammonia gas or solid reagent melamine as nitrogen sources, leading to graphene with low doping level, polycrystalline nature, high defect density and low carrier mobility. Here, we demonstrate a self-assembly approach that allows the synthesis of single-layer, single crystal and highly nitrogen-doped graphene domain arrays by self-organization of pyridine molecules on Cu surface at temperature as low as 300 °C. These N-doped graphene domains have a dominated geometric structure of tetragonal-shape, reflecting the single crystal nature confirmed by electron-diffraction measurements. The electrical measurements of these graphene domains showed their high carrier mobility, high doping level, and reliable N-doped behavior in both air and vacuum.

Low temperature growth of highly nitrogen-doped single crystal graphene arrays by chemical vapor deposition.

By using near-equilibrium chemical vapor deposition, it is demonstrated that high-quality single-crystal graphene can be grown on dielectric substrates. The maximum size is about 11 μm. The carrier mobility can reach about 5650 cm(2) V(-1) s(-1) , which is comparable to those of some metal-catalyzed graphene crystals, reflecting the good quality of the graphene lattice.

Gui Yu

Papers

Synthesis of N-Doped Graphene by Chemical Vapor Deposition and Its Electrical Properties

Uniform hexagonal graphene flakes and films grown on liquid copper surface

Oxygen-Aided Synthesis of Polycrystalline Graphene on Silicon Dioxide Substrates

Low temperature growth of highly nitrogen-doped single crystal graphene arrays by chemical vapor deposition.

Near-equilibrium chemical vapor deposition of high-quality single-crystal graphene directly on various dielectric substrates.