Amidst these growing sustainability concerns, producing NH via electrochemical NO reduction reaction (NORR) emerges as a promising alternative to the conventional Haber-Bosch process. In a pioneering approach, this study introduces Ru incorporation into CoO lattices at the nanoscale and further couples it with electroreduction conditioning (ERC) treatment as a strategy to enhance metal oxide reducibility and induce oxygen vacancies, advancing NH production from NORR. Here, supported by a suite of ex situ and in situ characterization measurements, the findings reveal that Ru enrichment promotes Co species reduction and oxygen vacancy formation.
View Article and Find Full Text PDFLiquid metals (LMs) are electronic liquid with enigmatic interfacial chemistry and physics. These features make them promising materials for driving chemical reactions on their surfaces for designing nanoarchitectonic systems. Herein, we showed the interfacial interaction between eutectic gallium-indium (EGaIn) liquid metal and graphene oxide (GO) for the reduction of both substrate-based and free-standing GO.
View Article and Find Full Text PDFA green carbon capture and conversion technology offering scalability and economic viability for mitigating CO emissions is reported. The technology uses suspensions of gallium liquid metal to reduce CO into carbonaceous solid products and O at near room temperature. The nonpolar nature of the liquid gallium interface allows the solid products to instantaneously exfoliate, hence keeping active sites accessible.
View Article and Find Full Text PDFThe introduction of trace impurities within the doping processes of semiconductors is still a technological challenge for the electronics industries. By taking advantage of the selective enrichment of liquid metal interfaces, and harvesting the doped metal oxide semiconductor layers, the complexity of the process can be mitigated and a high degree of control over the outcomes can be achieved. Here, a mechanism of natural filtering for the preparation of doped 2D semiconducting sheets based on the different migration tendencies of metallic elements in the bulk competing for enriching the interfaces is proposed.
View Article and Find Full Text PDFAlthough it remains unexplored, the direct synthesis and expulsion of metals from alloys can offer many opportunities. Here, such a phenomenon is realized electrochemically by applying a polarizing voltage signal to liquid alloys. The signal induces an abrupt interfacial perturbation at the Ga-based liquid alloy surface and results in an unrestrained discharge of minority elements, such as Sn, In, and Zn, from the liquid alloy.
View Article and Find Full Text PDFRoom-temperature synthesis of 2D graphitic materials (2D-GMs) remains an elusive aim, especially with electrochemical means. Here, it is shown that liquid metals render this possible as they offer catalytic activity and an ultrasmooth templating interface that promotes Frank-van der Merwe regime growth, while allowing facile exfoliation due to the absence of interfacial forces as a nonpolar liquid. The 2D-GMs are formed at low onset potential and can be in situ doped depending on the choice of organic precursors and the electrochemical set-up.
View Article and Find Full Text PDFIt has become apparent that renewable energy sources are plentiful in many, often remote, parts of the world, such that storing and transporting that energy has become the key challenge. For long-distance transportation by pipeline and bulk tanker, a liquid form of energy carrier is ideal, focusing attention on liquid hydrogen and ammonia. Development of high-activity and selectivity electrocatalyst materials to produce these energy carriers by reductive electrochemistry has therefore become an important area of research.
View Article and Find Full Text PDFFreestanding flexible electrodes with high areal mass loading are required for the development of flexible high-performance lithium-ion batteries (LIBs). Currently they face the challenge of low mass loading due to the limited concentrations attainable in processable dispersions. Here, we report a simple low-temperature hydrothermal route to fabricate flexible layered molybdenum disulfide (MoS)/reduced graphene oxide (MSG) films offering high areal capacity and good lithium storage performance.
View Article and Find Full Text PDFThe original version of this Article contained errors in the author affiliations. Affiliation 1 incorrectly read 'School of Chemical Engineering, University of New South Wales (UNSW), Sydney, NSW 2031, Australia' and affiliation 4 incorrectly read 'School of Engineering, RMIT University, Melbourne, VIC 3001, Australia.' This has now been corrected in both the PDF and HTML versions of the Article.
View Article and Find Full Text PDFNegative carbon emission technologies are critical for ensuring a future stable climate. However, the gaseous state of CO does render the indefinite storage of this greenhouse gas challenging. Herein, we created a liquid metal electrocatalyst that contains metallic elemental cerium nanoparticles, which facilitates the electrochemical reduction of CO to layered solid carbonaceous species, at a low onset potential of -310 mV vs CO/C.
View Article and Find Full Text PDFFabrication of flexible and free-standing graphene-fiber- (GF-) based microelectrode arrays with a thin platinum coating, acting as a current collector, results in a structure with low impedance, high surface area, and excellent electrochemical properties. This modification results in a strong synergistic effect between these two constituents leading to a robust and superior hybrid material with better performance than either graphene electrodes or Pt electrodes. The low impedance and porous structure of the GF results in an unrivalled charge injection capacity of 10.
View Article and Find Full Text PDFSilicon-based impurities are ubiquitous in natural graphite. However, their role as a contaminant in exfoliated graphene and their influence on devices have been overlooked. Herein atomic resolution microscopy is used to highlight the existence of silicon-based contamination on various solution-processed graphene.
View Article and Find Full Text PDFThis work presents a study on a capacitively coupled contactless conductivity detector (C4D) for micron-sized fibers. Following a previous report on the qualitative application of C4D for fibers, the present study provides a thorough analysis of the signal response to fiber conductivity. Using reduced graphene oxide (RGO) fibers, the detector response as a function of fiber length, cross-sectional area and resistance has been investigated.
View Article and Find Full Text PDFHerein, we show properly engineered MoS crystals can readily form liquid crystalline dispersions in water making them ideal candidates for large-scale manufacturing processes. The guideline provided here can serve as the basis to develop practical protocols to address the long-standing goal of large-scale manufacturing of 2D materials.
View Article and Find Full Text PDFGraphene oxide (GO), the main precursor of graphene-based materials made by solution processing, is known to be very stiff. Indeed, it has a Young's modulus comparable to steel, on the order of 300 GPa. Despite its very high stiffness, we show here that GO is superflexible.
View Article and Find Full Text PDFThe efficient and selective catalytic reduction of CO2 is a highly promising process for both of the storage of renewable energy as well as the production of valuable chemical feedstocks. In this work, we show that the addition of an ionic liquid, 1-butyl-3-methylimidazolium tetrafluoroborate, in an aprotic electrolyte containing a proton source and FeTPP, promotes the in situ formation of the [Fe(0) TPP](2-) homogeneous catalyst at a less negative potential, resulting in lower overpotentials for the CO2 reduction (670 mV) and increased kinetics of electron transfer. This co-catalysis exhibits high Faradaic efficiency for CO production (93 %) and turnover number (2 740 000 after 4 hour electrolysis), with a four-fold increase in turnover frequency (TOF) when compared with the standard system without the ionic liquid.
View Article and Find Full Text PDFThe use of capacitively coupled contactless conductivity detection (C(4)D) for the characterisation of thin conductive graphene fibres, graphene composite fibres, and graphene coated fibrous materials is demonstrated for the first time. Within a few seconds, the non-destructive C(4)D detector provides a profile of the longetudinal physical homogeneity of the fibre, as well as extra information regarding fibre mophology and composition. In addition to the theoretical considerations related to the factors affect the output signal, this work evaluates the properties of graphene fibres using scanning C(4)D following the manufacturing process of wet-spinning.
View Article and Find Full Text PDFDue to excellent electrical and mechanical properties of carbon nano materials, it is of great interest to fabricate flexible, high conductive, and shape engineered carbon based fibers. As part of these approaches, hollow, twist, ribbon, and other various shapes of carbon based fibers have been researched for various functionality and application. In this paper, we suggest simple and effective method to control the fiber shape.
View Article and Find Full Text PDFAlthough great attention has been paid to wearable electronic devices in recent years, flexible lightweight batteries or supercapacitors with high performance are still not readily available due to the limitations of the flexible electrode inventory. In this work, highly flexible, bendable and conductive rGO-PEDOT/PSS films were prepared using a simple bar-coating method. The assembled device using rGO-PEDOT/PSS electrode could be bent and rolled up without any decrease in electrochemical performance.
View Article and Find Full Text PDFThe successful commercialization of smart wearable garments is hindered by the lack of fully integrated carbon-based energy storage devices into smart wearables. Since electrodes are the active components that determine the performance of energy storage systems, it is important to rationally design and engineer hierarchical architectures atboth the nano- and macroscale that can enjoy all of the necessary requirements for a perfect electrode. Here we demonstrate a large-scale flexible fabrication of highly porous high-performance multifunctional graphene oxide (GO) and rGO fibers and yarns by taking advantage of the intrinsic soft self-assembly behavior of ultralarge graphene oxide liquid crystalline dispersions.
View Article and Find Full Text PDFWith the aim of fabricating multifunctional fibers with enhanced mechanical properties, electrical conductivity and electrochemical performance, we develop wet-spinning of composite formulation based on functionalized PEG-SWNT and PEDOT:PSS. The method of addition and loading are directly correlated to the quality and the ease of spinnability of the formulation and to the mechanical and electrical properties of the resultant fibers. Both the fiber modulus (Y) and strength (σ) scaled linearly with PEG-SWNT volume fraction (Vf).
View Article and Find Full Text PDFBy controlling the SWNT-rGO electrode composition and thickness to attain the appropriate porosity and tortuosity, the electroactive surface area is maximized while rapid diffusion of the electrolyte through the electrode is maintained. This leads to an increase in exchange current density between the electrode and electrolyte which results in enhanced thermocell performance.
View Article and Find Full Text PDFWe introduce soft self-assembly of ultralarge liquid crystalline (LC) graphene oxide (GO) sheets in a wide range of organic solvents overcoming the practical limitations imposed on LC GO processing in water. This expands the number of known solvents which can support amphiphilic self-assembly to ethanol, acetone, tetrahydrofuran, N-dimethylformamide, N-cyclohexyl-2-pyrrolidone, and a number of other organic solvents, many of which were not known to afford solvophobic self-assembly prior to this report. The LC behavior of the as-prepared GO sheets in organic solvents has enabled us to disperse and organize substantial amounts of aggregate-free single-walled carbon nanotubes (SWNTs, up to 10 wt %) without compromise in LC properties.
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