ABSTRACT
In this work, we implement a dual frequency (24 kHz and 1174 kHz) ultrasonic assisted liquid phase exfoliation (ULPE) technique in deionized water (DIW) and other eco-friendly solvents, to produce a variety of high-quality few-layer graphene (FLG) solutions under controlled ultrasonication conditions. The resulting FLG dispersions of variable sizes (â¼0.2-1.5 µm2) confirmed by characterisation techniques comprising UV-Vis spectroscopy, Raman spectroscopy and high-resolution transmission electron microscopy (HR-TEM). For the first time we demonstrate that high yield of FLG flakes with minimal defects, stable for 6 + months in a solution (stability â¼ 70 %), can be obtained in less than 1-hour of treatment in either water/ethanol (DIW:EtOH) or water/isopropyl alcohol (DIW:IPA) eco-friendly mixtures. We also scrutinized the underlying mechanisms of cavitation using high-speed imaging synchronized with acoustic pressure measurements. The addition of ethanol or IPA to deionized water is proposed to play a central role in exfoliation as it regulates the extend of the cavitation zone, the intensity of the ultrasonic field and, thus, the cavitation effectiveness. Our study revealed that lateral sizes of the obtained FLG depend on the choice of exfoliating media and the diameter of a sonotrode used. This variability offers flexibility in producing FLG of different sizes, applicable in a wide spectrum of size-specific applications.
ABSTRACT
Achieving a sustainable production of pristine high-quality graphene and other layered materials at a low cost is one of the bottlenecks that needs to be overcome for reaching 2D material applications at a large scale. Liquid phase exfoliation in conjunction with N-methyl-2-pyrrolidone (NMP) is recognized as the most efficient method for both the exfoliation and dispersion of graphene. Unfortunately, NMP is neither sustainable nor suitable for up-scaling production due to its adverse impact on the environment. Here, we show the real potential of green solvents by revealing the independent contributions of their exfoliation efficiency and graphene dispersibility to the graphene yield. By experimentally separating these two factors, we demonstrate that the exfoliation efficiency of a given solvent is independent of its dispersibility. Our studies revealed that isopropanol can be used to exfoliate graphite as efficiently as NMP. Our finding is corroborated by the matching ratio between the polar and dispersive energies of graphite and that of the solvent surface tension. This direct evidence of exfoliation efficiency and dispersibility of solvents paves the way to developing a deeper understanding of the real potential of sustainable graphene manufacturing at a large scale.
ABSTRACT
Graphene dispersions in water are highly desirable for a range of applications such as biomedicines, separation membranes, coatings, inkjet printing and more. Recent novel research has been focussed on developing a green approach for scalable production of graphene. However, one important parameter, which is often neglected is the bulk temperature of the processing liquid. This paper follows our earlier work where optimal sono-exfoliation parameters of graphite in aqueous solutions were determined based on the measured acoustic pressure fields at various temperatures and input powers. Here, we take the next step forward and demonstrate using systematic characterisation techniques and acoustic pressure measurements that sonication-assisted liquid phase exfoliation (LPE) of graphite powder can indeed produce high quality few layer graphene flakes in pure water at a specific temperature, i.e. 40 °C, and at an optimised input generator power of 50%, within 2-h of processing. UV-vis analysis also revealed that the exfoliation, stability and uniformity of dispersions were improved with increasing temperature. We further confirmed the successful exfoliation of graphene sheets with minimal level of defects in the optimized sample with the help of Raman microscopy and transmission electron microscopy. This study demonstrated that understanding and controlling processing temperature is one of the key parameters for graphene exfoliation in water which offers a potential pathway for its large-scale production.
ABSTRACT
The volume of fluid (VOF) and continuous surface force (CSF) methods were used to develop a bubble dynamics model for the simulation of bubble oscillation and implosion dynamics under ultrasound. The model was calibrated and validated by the X-ray image data acquired by ultrafast synchrotron X-ray. Coupled bubble interactions with bulk graphite and freely moving particles were also simulated based on the validated model. Simulation and experiments quantified the surface instability developed along the bubble surface under the influence of ultrasound pressure fields. Once the surface instability exceeds a certain amplitude, bubble implosion occurs, creating shock waves and highly deformed, irregular gas-liquid boundaries and smaller bubble fragments. Bubble implosion can produce cyclic impulsive stresses sufficient enough to cause µs fatigue exfoliation of graphite layers. Bubble-particle interaction simulations reveal the underlying mechanisms for efficient particle dispersion or particle wrapping which are all strongly related to the oscillation dynamics of the bubbles and the particle surface properties.
Subject(s)
Graphite , Surface Properties , Ultrasonics , X-RaysABSTRACT
Scaling up ultrasonic cavitation melt treatment (UST) requires effective flow management with minimised energy requirements. To this end, container dimensions leading to the resonance play a crucial role in amplifying pressure amplitude for cavitation. To quantify the importance of resonance length during the treatment of liquid aluminium, we used calibrated high-temperature cavitometers (in the range of 8-400 kHz), to measure and record the acoustic pressure profiles inside the cavitation-induced environment of liquid Al and deionized water (used as an analogue to Al) excited at 19.5 kHz. To achieve a comprehensive map of the acoustic pressure field, measurements were conducted at three different cavitometer positions relative to the vibrating sonotrode probe and for a number of resonant and non-resonant container lengths based on the speed of sound in the treated medium. The results showed that the resonance length affected the pressure magnitude in liquid Al in all cavitometer positions, while water showed no sensitivity to resonance length. An important practical application of UST in aluminium processing concerns grain refinement. For this reason, grain size analysis of UST-treated Al-Cu-Zr-Ti alloy was used as an indicator of the melt treatment efficiency. The result showed that the treatment in a resonance tank of L=λAl (the wavelength of sound in Al) gave the best structure refinement as compared to other tested lengths. The data given here contribute to the optimisation of the ultrasonic process in continuous casting, by providing an optimum value for the critical compartment (e.g. in a launder of direct-chill casting) dimension.
ABSTRACT
Ultrasonic melt processing significantly improves the properties of metallic materials. However, this promising technology has not been successfully transferred to the industry because of difficulties in treating large volumes of melt. To circumvent these difficulties, a fundamental understanding of the efficiency of ultrasonic treatment of liquid metals is required. In this endeavor, the dynamics of two interacting hydrogen bubbles in liquid aluminum are studied to determine the effect of a strong acoustic field on their behavior. It is shown that coalescence readily occurs at low frequencies in the range of 16 to 20 kHz; forcing frequencies at these values are likely to promote degassing. Emitted acoustic pressures from relatively isolated bubbles that resonate with the driving frequency are in the megapascal range and these cavitation shock waves are presumed to promote grain refinement by disrupting the growth of the solidification front.
