Self-assembled organic layers containing various functional groups between graphene layers were examined as gas barrier films. The formation of well-defined self-assembled layers of functionalized alkane molecules on graphene was confirmed by scanning tunneling microscopy (STM). The roles of these organic layers as gas barrier films could be quantitatively deduced by comparing their water vapor transmission rate (WVTR). The formation of self-assembled layers dramatically improved gas barrier properties by primarily blocking defects and gas molecule pathways. For functionalized alkanes containing hydrophilic groups, more enhanced gas barrier properties were observed compared to those with hydrophobic groups. These results clearly indicate that the primary role of the organic layers in gas barrier films is to block defects and the pathways of water molecules, with a secondary role of delaying the movement of water molecules through hydrogen bonding interactions.

Large-area graphene of the order of centimeters was deposited on copper substrates by low-pressure chemical vapor deposition (LPCVD) using hexane as the carbon source. The effect of temperature and the carrier gas flowrates on the quality and uniformity of the as-deposited graphene was investigated using the Raman analysis. The film deposited at 870 °C with a total carrier gas flowrate of 50 sccm is predominantly single-layer with very low defects according to the Raman spectra. The 2D/G peak intensity ratios obtained from the Raman spectra of samples from three different locations of graphene deposited on a whole copper catalyst was used to calculate the large-area uniformity. Based on the results, a very high uniformity of 89.6% was calculated for the graphene deposited at 870 °C. The uniformity was observed to decrease with increasing temperature. Similar to the thickness uniformity, the electrical conductivity values obtained as a result of I–V measurements and water contact angle measurements were found to be close to each other for the graphene deposited under the same deposition conditions.

In this study, graphene was rapidly grown by chemical vapor deposition using a liquid cell for supplying methanol as a carbon source of graphene. To realize the rapid growth, methanol which is carbon-contained organic solvent was used instead of methane gas, a widely used carbon source for graphene growth. The graphene grown with the growth time as a variable was transferred to a SiO2/ Si substrate with an oxide thickness of 300 nm to confirm whether it was grown with full coverage with an optical microscope. The results confirmed a full coverage in 0.5 min of growth. The Raman spectra also confirmed the G-peak position at 1585.0 cm−1 and an intensity ratio of 2D/G at 2.3 or higher. Concerning electrical transport characteristics, at an induced carrier density of 1 × 1012 cm−2, the hole (μh) and electron (μe) mobilities were 1524 cm2 V−1 s−1 and 1528 cm2 V−1 s−1, respectively. Thus, our study confirmed that high-quality, large-area graphene can be grown within 0.5 min.

The study presented in the article is focused on use of graphene obtained by novel microwave-enhanced chemical vapor deposition (MECVD) method as a construction material for 3D porous structures—aerogels and sponges. MECVD graphene nanoplatelets-based aerogels were obtained by mixing MECVD graphene nanoplatelets and chitosan, dissolved in 3% acetic acid followed by its freeze drying and carbonization at 800° in inert medium. Surface morphology of aerogels was characterized by SEM. MECVD graphene nanoplatelets-based aerogels are characterized by a porous structure; they are superhydrophobic and possess high sorption capacity with regard to organic liquids of different densities. Polyurethane sponges coated with MECVD graphene can serve as an alternative to aerogels. The process of their obtaining is cheaper and less complicated. They were obtained by facile “dip-coating” method, modifying its surface to increase its hydrophobicity. The resulting sponges are superhydrophobic and superoleophilic, and demonstrate high rate of sorption of organic liquids and can be easily regenerated by squeezing. In addition, they can be used as a separating material in conjunction with vacuum system for continuous and selective collection of organic liquids from the surface of water.

Cobalt was electrodeposited onto chemical vapor deposition (CVD) graphene/Si/SiO2 substrates, during different time intervals, using an electrolyte solution containing a low concentration of cobalt sulfate. The intention was to investigate the details of the deposition process (and the dissolution process) and the resulting magnetic properties of the Co deposits on graphene. During and after electrodeposition, in-situ magnetic measurements were performed using an (AGFM). These were followed by ex situ morphological analysis of the samples with ΔtDEP 30 and 100 s by atomic force microscopy in the non-contact mode on pristine CVD graphene/SiO2/Si. We demonstrate that it is possible to electrodeposit Co onto graphene, and that in-situ magnetic measurements can also help in understanding details of the deposition process itself. The results show that the Co deposits are ferromagnetic with decreasing coercivity (HC) and demonstrate increasing magnetization on saturation (MSAT) and electric signal proportional to remanence (Mr), as a function of the amount of the electrodeposited Co. It was also found that, after the end of the dissolution process, a certain amount of cobalt remains on the graphene in oxide form (this was confirmed by X-ray photoelectron spectroscopy), as suggested by the magnetic measurements. This oxide tends to exhibit a limited asymptotic amount when cycling through the deposition/dissolution process for increasing deposition times, possibly indicating that the oxidation process is similar to the graphene surface chemistry.

Graphene was grown on molybdenum (Mo) foil by a chemical vapor deposition method at different growth temperatures (1000°C, 1100°C, and 1200°C). The properties of graphene were investigated by X-ray diffraction (XRD), X-ray photoelectron spectroscopy, and Raman spectroscopy. The results showed that the quality of the deposited graphene layer was affected by the growth temperature. XRD results showed the presence of a carbide phase on the Mo surface; the presence of carbide was more intense at 1200°C. Additionally, a higher I2D/IG ratio (0.418) was observed at 1200°C, which implies that there are fewer graphene layers at this temperature. The lowest ID/IG ratio (0.908) for the graphene layers was obtained at 1200°C, suggesting that graphene had fewer defects at this temperature. The size of the graphene domains was also calculated. We found that by increasing the growth temperature, the graphene domain size also increased.

Exceptional progress has been made with chemical vapor deposition (CVD) of graphene in the past few years. Not only has good monolayer growth of graphene been achieved, but large-area synthesis of graphene sheets has been successful too. However, the polycrystalline nature of CVD graphene is hampering further progress as graphene property degrades due to presence of grain boundaries. This review will cover factors that affect nucleation of graphene and how other scientists sought to obtain large graphene domains. In addition, the limitation of the current research trend will be touched upon as well.

We report a highly sensitive NO2 gas sensor based on multi-layer graphene (MLG) films synthesized by a chemical vapor deposition method on a microheater-embedded flexible substrate. The MLG could detect low-concentration NO2 even at sub-ppm (<200 ppb) levels. It also exhibited a high resistance change of ~6% when it was exposed to 1 ppm NO2 gas at room temperature for 1 min. The exceptionally high sensitivity could be attributed to the large number of NO2 molecule adsorption sites on the MLG due to its a large surface area and various defect-sites, and to the high mobility of carriers transferred between the MLG films and the adsorbed gas molecules. Although desorption of the NO2 molecules was slow, it could be enhanced by an additional annealing process using an embedded Au microheater. The outstanding mechanical flexibility of the graphene film ensures the stable sensing response of the device under extreme bending stress. Our large-scale and easily reproducible MLG films can provide a proof-of-concept for future flexible NO2 gas sensor devices.

Graphene has been synthesized on 100- and 300-nm-thick Ni/SiO2/Si substrates with CH4 gas (1 SCCM) diluted in mixed gases of 10% H2 and 90% Ar (99 SCCM) at 900˚C by using inductively-coupled plasma chemical vapor deposition (ICP-CVD). The film morphology of 100-nm-thick Ni changed to islands on SiO2/Si substrate after heat treatment at 900˚C for 2 min because of grain growth, whereas 300-nm-thick Ni still maintained a film morphology. Interestingly, suspended graphene was formed among Ni islands on 100-nm-thick Ni/SiO2/Si substrate for the very short growth of 1 sec. In addition, the size of the graphene domains was much larger than that of Ni grains of 300-nm-thick Ni/SiO2/Si substrate. These results suggest that graphene growth is strongly governed by the direct formation of graphene on the Ni surface due to reactive carbon radicals highly activated by ICP, rather than to well-known carbon precipitation from carbon-containing Ni. The D peak intensity of the Raman spectrum of graphene on 300-nm-thick Ni/SiO2/Si was negligible, suggesting that high-quality graphene was formed. The 2D to G peak intensity ratio and the full-width at half maximum of the 2D peak were approximately 2.6 and 47cm-1, respectively. The several-layer graphene showed a low sheet resistance value of 718Ω/sq and a high light transmittance of 87% at 550 nm.

Methanol as a carbon source in chemical vapor deposition (CVD) graphene has an advantage over methane and hydrogen in that we can avoid optimizing an etching reagent condition. Since methanol itself can easily decompose into hydrocarbon and water (an etching reagent) at high temperatures [1], the pressure and the temperature of methanol are the only parameters we have to handle. In this study, synthetic conditions for highly crystalline and large area graphene have been optimized by adjusting pressure and temperature; the effect of each parameter was analyzed systematically by Raman, scanning electron microscope, transmission electron microscope, atomic force microscope, four-point-probe measurement, and UV-Vis. Defect density of graphene, represented by D/G ratio in Raman, decreased with increasing temperature and decreasing pressure; it negatively affected electrical conductivity. From our process and various analyses, methanol CVD growth for graphene has been found to be a safe, cheap, easy, and simple method to produce high quality, large area, and continuous graphene films.

We present a method of graphene synthesis with high thickness uniformity using the thermal chemical vapor deposition (TCVD) technique; we demonstrate its application to a grid supporting membrane using transmission electron microscope (TEM) observation, particularly for nanomaterials that have smaller dimensions than the pitch of commercial grid mesh. Graphene was synthesized on electron-beam-evaporated Ni catalytic thin films. Methane and hydrogen gases were used as carbon feedstock and dilution gas, respectively. The effects of synthesis temperature and flow rate of feedstock on graphene structures have been investigated. The most effective condition for large area growth synthesis and high thickness uniformity was found to be 1000˚C and 5 sccm of methane. Among the various applications of the synthesized graphenes, their use as a supporting membrane of a TEM grid has been demonstrated; such a grid is useful for high resolution TEM imaging of nanoscale materials because it preserves the same focal plane over the whole grid mesh. After the graphene synthesis, we were able successfully to transfer the graphenes from the Ni substrates to the TEM grid without a polymeric mediator, so that we were able to preserve the clean surface of the as-synthesized graphene. Then, a drop of carbon nanotube (CNT) suspension was deposited onto the graphene-covered TEM grid. Finally, we performed high resolution TEM observation and obtained clear image of the carbon nanotubes, which were deposited on the graphene supporting membrane.

The defect sites on chemical vapor deposition grown graphene are investigated through the selective electrochemical deposition (SED) of Au nanoparticles. For SED of Au nanoparticles, an engineered potential pulse is applied to the working electrode versus the reference electrode, thereby highlighting the defect sites, which are more reactive relative to the pristine surface. Most defect sites decorated by Au nanoparticles are situated along the Cu grain boundaries, implying that the origin of the defects lies in the synthesis of uneven graphene layers on the rough Cu surface.

We analyzed the effect of etchants for metal catalysts in terms of the characteristics of resulting graphene films, such as sheet resistance, hall mobility, transmittance, and carrier concentration. We found the residue of FeCl3 etchant degraded the sheet resistance and mobility of graphene films. The residue was identified as an iron oxide containing a small amount of Cl through elemental analysis using X-ray photoelectron spectroscopy. To remove this residue, we provide an alternative etching solution by introducing acidic etching solutions and their combinations (HNO3, HCl, FeCl3 + HCl, and FeCl3+HNO3). The combination of FeCl3 and acidic solutions (HCl and HNO3) resulted in more enhanced electrical properties than pure etchants, which is attributed to the elimination of left over etching residue, and a small amount of amorphous carbon debris after the etching process.

Graphene has been effectively synthesized on Ni/SiO2/Si substrates with CH4 (1 SCCM) diluted in Ar/H2(10%) (99 SCCM) by using an inductively-coupled plasma-enhanced chemical vapor deposition. Graphene was formed on the entire surface of the 500 nm thick Ni substrate even at 700 ˚C, although CH4 and Ar/H2 gas were supplied under plasma of 600 W for 1 second. The Raman spectrum showed typical graphene features with D, G, and 2D peaks at 1356, 1584, and 2710 cm-1, respectively. With increase of growth temperature to 900 ˚C, the ratios of the D band intensity to the G band intensity and the 2D band intensity to the G band intensity were increased and decreased, respectively. The results were strongly correlated to a rougher and coarser Ni surface due to the enhanced recrystallization process at higher temperatures. In contrast, highquality graphene was synthesized at 1000 ˚C on smooth and large Ni grains, which were formed by decreasing Ni deposition thickness to 300 nm.