79 research outputs found

    Comparison of carbon materials as electrodes for enzyme electrocatalysis:hydrogenase as a case study

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    We present a study of electrocatalysis by an enzyme adsorbed on a range of carbon materials, with different size, surface area, morphology and graphitic structure, which are either commercially available or prepared via simple, established protocols. We choose as our model enzyme the hydrogenase I from E. coli (Hyd-1), which is an active catalyst for H2 oxidation, is relatively robust and has been demonstrated in H2 fuel cells and H2-driven chemical synthesis. The carbon materials were characterised according to their surface area, surface morphology and graphitic character, and we use the electrocatalytic H2 oxidation current for Hyd-1 adsorbed on these materials to evaluate their effectiveness as enzyme electrodes. Here, we show that a variety of carbon materials are suitable for adsorbing hydrogenases in an electroactive configuration. This unified study provides insight into selection and design of carbon materials for study of redox enzymes and different applications of enzyme electrocatalysis

    Unveiling the mechanism of the in situ> formation of 3d fiber macroassemblies with controlled properties

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    Electrospinning technique is well-known for the generation of different fibers. While it is a "simple" technique, it lies in the fact that the fibers are typically produced in the form of densely packed two-dimensional (2D) mats with limited thickness, shape, and porosity. The highly demanded three-dimensional (3D) fiber assemblies have been explored by time-consuming postprocessing and/or complex setup modifications. Here, we use a classic electrospinning setup to directly produce 3D fiber macrostructures only by modulating the spinning solution. Increasing solution conductivity modifies electrodynamic jet behavior and fiber assembling process; both are observed in situ using a high-speed camera. More viscous solutions render thicker fibers that own enhanced mechanical stiffness as examined by finite element analysis. We reveal the correlation between the universal solution parameters and the dimensionality of fiber assemblies, thereof, enlightening the design of more "3D spinnable" solutions that are compatible with any commercial electrospinning equipment. After a calcination step, ultralightweight ceramic fiber assemblies are generated. These inexpensive materials can clean up exceptionally large fractions of oil spillages and provide high-performance thermal insulation. This work would drive the development and scale-up production of next-generation 3D fiber materials for engineering, biomedical, and environmental applications

    Effects of green solvents and surfactants on the characteristics of few-layer graphene produced by dual-frequency ultrasonic liquid phase exfoliation technique

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    Nowadays, one of the promising methods for scalable graphene production is ultrasound-aided liquid phase exfoliation (ULPE) of graphite. Two current limiting factors of ULPE are the use of harmful solutions (such as N-Methyl-2-pyrrolidone or Dimethylformamide) and a relatively low graphene yield. In this study, we demonstrate a new dual frequency (20 kHz and 1174 kHz) ULPE approach in various eco-friendly media, which enabled us to produce various few-layer graphene (FLG) solutions of high quality. By implementing sophisticated characterisation techniques consisting of Raman spectroscopy, UV–vis spectroscopy and high-resolution electron microscopy, the final graphene flakes structure was confirmed to correlate the properties of each individual solution. The thinner (∼3 layers) and larger (∼1.5 μm2) flakes were observed while using just water, with the highest yield (11%) of smaller FLG flakes to be achieved in the mixture of water and a surfactant. In order to understand the cavitation mechanism in different solutions, the ULPE process was investigated by acoustic measurements. This study demonstrates the crucial role of ethanol (as a solvent) and surfactants as it regulates the cavitation power and intensity of the ultrasonic field and, thereby, the cavitation effectiveness. It is suggested that the mixture of water, ethanol and a surfactant is the best medium for ULPE process where a high yield of low-defective FLG flakes can be obtained in a solution stable at least for 3 months (around 80%)

    Time dependent decomposition of ammonia borane for the controlled production of 2D hexagonal boron nitride.

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    Ammonia borane (AB) is among the most promising precursors for the large-scale synthesis of hexagonal boron nitride (h-BN) by chemical vapour deposition (CVD). Its non-toxic and non-flammable properties make AB particularly attractive for industry. AB decomposition under CVD conditions, however, is complex and hence has hindered tailored h-BN production and its exploitation. To overcome this challenge, we report in-depth decomposition studies of AB under industrially safe growth conditions. In situ mass spectrometry revealed a time and temperature-dependent release of a plethora of NxBy-containing species and, as a result, significant changes of the N:B ratio during h-BN synthesis. Such fluctuations strongly influence the formation and morphology of 2D h-BN. By means of in situ gas monitoring and regulating the precursor temperature over time we achieve uniform release of volatile chemical species over many hours for the first time, paving the way towards the controlled, industrially viable production of h-BN

    Dual frequency ultrasonic cavitation in various liquids: High-speed imaging and acoustic pressure measurements

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    Ultrasonic cavitation is used in various processes and applications, utilizing powerful shock waves and high-speed liquid jets generated by the collapsing bubbles. Typically, a single frequency source is used to produce the desired effects. However, optimization of the efficiency of ultrasound reactors is necessary to improve cavitation activity in specific applications such as for the exfoliation of two dimensional materials. This research takes the next step to investigate the effect of a dual frequency transducer system on the bubble dynamics, cavitation zone, pressure fields, acoustic spectra, and induced shock waves for four liquids with a range of physical properties. Using ultra-high-speed imaging and synchronized acoustic pressure measurements, the effect of ultrasonic dual frequencies on bubble dynamics was investigated. The addition of a high frequency transducer (1174 kHz) showed that the bubble fragments and satellite bubbles induced from a low frequency transducer (24 kHz) were able to extend their lifecycle and increase spatial distribution, thus, extending the boundaries of the cavitation zone. Furthermore, this combination of ultrasonic frequencies generated higher acoustic pressures (up to 180%) and enhanced the characteristic shock wave peak, indicating more bubble collapses and the generation of additional shock waves. The dual frequency system also enlarged the cavitation cloud size under the sonotrode. These observations specifically delineated the enhancement of cavitation activity using a dual frequency system pivotal for optimization of existing cavitation-based processing technologies

    WS22D nanosheets in 3D nanoflowers

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    In this work it has been established that 3D nanoflowers of WS2 synthesized by chemical vapour deposition are composed of few layer WS2 along the edges of the petals. An experimental study to understand the evolution of these nanostructures shows the nucleation and growth along with the compositional changes they undergo

    A Graphene Surface Force Balance

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    We report a method for transferring graphene, grown by chemical vapor deposition, which produces ultraflat graphene surfaces (root-mean-square roughness of 0.19 nm) free from polymer residues over macroscopic areas (>1 cm2). The critical step in preparing such surfaces involves the use of an intermediate mica template, which itself is atomically smooth. We demonstrate the compatibility of these model surfaces with the surface force balance, opening up the possibility of measuring normal and lateral forces, including friction and adhesion, between two graphene sheets either in contact or across a liquid medium. The conductivity of the graphene surfaces allows forces to be measured while controlling the surface potential. This new apparatus, the graphene surface force balance, is expected to be of importance to the future understanding of graphene in applications from lubrication to electrochemical energy storage systems
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