We investigated the effect of surfactants and their concentration (Csur) on the final graphene concentration (CG) via the liquid-phase exfoliation method. Six typical surfactants including ionic and non-ionic ones were explored and the optimized Csur for each surfactant was suggested. For ionic surfactants, CG increases with Csur before reaching its maximum and then maintains the high level. The different mechanisms of ionic and non-ionic surfactants in stabilizing graphene dispersions are explained by the theory for colloidal stability. The as-prepared graphene sheets are verified to be highly exfoliated through transmission electron microscopy and atomic force microscopy studies, while the defect-free structure was evidenced by Raman spectra and X-ray photoelectron spectroscopy.
Liquid-phase exfoliation of two-dimensional materials is very attractive for large-scale applications. Although used extensively, isolating MoS2 layers (<10) with high efficiency is reported to be extremely difficult. Further, the importance of soaking has not yet been studied, and the surfactants' role in stabilizing MoS2 nanosheets is poorly understood1. Herein, we report a novel approach to exfoliating large quantities of MoS2 via high-pressure (HP) liquid-phase exfoliation (LPE) in deionized (DI) water. 4 to 7 layers of MoS2 nanosheets were obtained from 60 days-soaked samples and they wer…
Surfactants are often used to stabilise two-dimensional (2D) materials in environmentally friendly solvents such as water. Aqueous-surfactant solutions prevent agglomeration of nanosheets through steric and electrostatic repulsion, facilitating the production of high concentration nanomaterial dispersions. Turbulent, shear-assisted liquid exfoliation of layered precursor materials produces defect-free nanosheets by promoting mixing and generating sufficiently high shear rates to overcome out-of-plane van der Waals bonds. In the presence of a liquid-gas interface, a consequence of using surfact…
Ultrasonication is widely used to exfoliate two dimensional (2D) van der Waals layered materials such as graphene. Its fundamental mechanism, inertial cavitation, is poorly understood and often ignored in ultrasonication strategies resulting in low exfoliation rates, low material yields and wide flake size distributions, making the graphene dispersions produced by ultrasonication less economically viable. Here we report that few-layer graphene yields of up to 18% in three hours without introduction of basal plane defects can be achieved by optimising inertial cavitation during ultrasonication.…
Few layer graphene (FLG) was synthesized by $μ$-wave assisted exfoliation of expanded graphite in toluene with an overall yield from c.a. 7% to 20%. A significant difference in the absorption of $μ$-waves by the expanded graphite and toluene allowed a rapid heating of the medium. The number of FLG sheets varies from 3 to 12, while the lateral size of the sheets exceeds few $μ$ms. The obtained FLG exhibits very low resistance with average value of 1.6 k$Ω$ (500 $Ω$ minimum) which is comparable to that of high quality graphenes synthesized by CVD methods, and lower than numbers of exfoliated gra…
In crystal growth, surfactants are additive molecules used in dilute amount or as dense, permeable layers to control surface morphologies. Here, we investigate the properties of a strikingly different surfactant: a two-dimensional and covalent layer with close atomic packing, graphene. Using in situ, real time electron microscopy, scanning tunneling microscopy, kinetic Monte Carlo simulations, and continuum mechanics calculations, we reveal why metallic atomic layers can grow in a two-dimensional manner below an impermeable graphene membrane. Upon metal growth, graphene dynamically opens nanoc…
Remote epitaxy is a promising approach for synthesizing exfoliatable crystalline membranes and enabling epitaxy of materials with large lattice mismatch. However, the atomic scale mechanisms for remote epitaxy remain unclear. Here we experimentally demonstrate that GaSb films grow on graphene-terminated GaSb (001) via a seeded lateral epitaxy mechanism, in which pinhole defects in the graphene serve as selective nucleation sites, followed by lateral epitaxy and coalescence into a continuous film. Remote interactions are not necessary in order to explain the growth. Importantly, the small size …
We report the use of a surfactant molecule during the epitaxy of graphene on SiC(0001) that leads to the growth in an unconventional orientation, namely $R0^\circ$ rotation with respect to the SiC lattice. It yields a very high-quality single-layer graphene with a uniform orientation with respect to the substrate, on the wafer scale. We find an increased quality and homogeneity compared to the approach based on the use of a pre-oriented template to induce the unconventional orientation. Using spot profile analysis low energy electron diffraction, angle-resolved photoelectron spectroscopy, and …
In this work, linear polystyrene-poly(2-vinylpyridine) (PS-b-P2VP) and heteroarm star PS_22P2VP_22 ionizable block copolymers were used as dispersing agents for the liquid-phase exfoliation of pristine graphene. Various strategies such as direct exfoliation, film hydration and phase transfer have been employed and compared. The best strategy involved a two-step process, namely, pre-exfoliation of graphite in polymer/CHCl3 solutions followed by phase transfer to acidified water. High concentrations of stable aqueous suspensions of graphene flakes, highly enriched in monolayer structures, were t…
Single-crystalline membranes of functional materials enable the tuning of properties via extreme strain states; however, conventional routes for producing membranes require the use of sacrificial layers and chemical etchants, which can both damage the membrane and limit the ability to make them ultrathin. Here we demonstrate the epitaxial growth of the cubic Heusler compound GdPtSb on graphene-terminated Al$_2$O$_3$ substrates. Despite the presence of the graphene interlayer, the Heusler films have epitaxial registry to the underlying sapphire, as revealed by x-ray diffraction, reflection high…
Electrochemical exfoliation is one of the most promising methods for scalable production of graphene. However, limited understanding of its Raman spectrum as well as lack of measurement standards for graphene strongly limit its industrial applications. In this work we show a systematic study of the Raman spectrum of electrochemically exfoliated graphene, produced using different electrolytes and different types of solvents in varying amounts. We demonstrate that no information on the thickness can be extracted from the shape of the 2D peak as this type of graphene is defective. Furthermore, th…
We present a high scale method to produce few layer graphene (FLG) based on the mechanical exfoliation of graphite and compare the obtained FLG with the one reported earlier arising from pencil lead ablation. Several things are modified and improved in the new approach. The purification and the ablation set_up are simplified, and the morphology of the FLG is modified and improved in view of some applications. The morphology dependent properties of FLGs, lead FLG and graphite FLG, are investigated as conductive layers and in nanocomposites. Newly obtained FLG has higher aspect ratio (high later…
Functional composite thin films have a wide variety of applications in flexible and/or electronic devices, telecommunications and multifunctional emerging coatings. Rapid screening of their properties is a challenging task, especially with multiple components defining the targeted properties. In this work we present a manifold for accelerated automated screening of viscous graphene suspensions for optimal electrical conductivity. Using Opentrons OT2 robotic auto-pipettor, we tested 3 most industrially significant surfactants - PVP, SDS and T80 - by fabricating 288 samples of graphene suspensio…
Herein, we report an easy, straight forward, and versatile approach to build 0D/2D hybrid nanoparticle/graphene architectures by means of non-covalent chemistry and a modified Layer-by-Layer assembly. Three water soluble perylene diimides were employed to efficiently exfoliate pristine graphite into positively charged few- and multilayer graphene flakes. Further combination of these cationic building blocks with anionic zinc oxide nanoparticles led to the formation of tailor-made hybrid films via electrostatic and van der Waals interactions. These supramolecular hybrid nano-structures were tho…
The surfactant assisted exfoliation and non-covalent functionalization of two-dimensional layered materials, like graphene, transition metal dichalcogenides, etc., has extraordinarily been propelled forward within the last 5 years. Numerous molecules have been designed and attached to the exfoliated layers, and based on their outstanding properties, perylene based dyes have become one of the most frequently used π-detergents. Therefore, the prospect of this micro review is to summarize the most prominent achievements in this rapidly progressing field of research.
The past decade has seen rapid growth in the research area of graphene and its application to novel electronics. With Moore's law beginning to plateau, the need for post-silicon technology in industry is becoming more apparent. Moreover, existing technology is insufficient for implementing terahertz detectors and receivers, which are required for a number of applications including medical imaging and security scanning. Graphene is considered to be a key potential candidate for replacing silicon in existing CMOS technology as well as realizing field effect transistors for terahertz detection, d…
Humidity sensing is important to a variety of technologies and industries, ranging from environmental and industrial monitoring to medical applications. Although humidity sensors abound, few available solutions are thin, transparent, compatible with large-area sensor production and flexible, and almost none are fast enough to perform human respiration monitoring through breath detection or real-time finger proximity monitoring via skin humidity sensing. This work describes chemiresistive graphene-based humidity sensors produced in few steps with facile liquid phase exfoliation (LPE) followed b…
Development of the next generation thermal interface materials with high thermal conductivity is important for thermal management and packaging of electronic devices. We report on the synthesis and thermal conductivity measurements of non-curing thermal paste, i.e. grease, based on mineral oil with the mixture of graphene and few-layer graphene flakes as the fillers. It was found that graphene thermal paste exhibits a distinctive thermal percolation threshold with the thermal conductivity revealing a sublinear dependence on the filler loading. This behavior contrasts with the thermal conductiv…
