SiO electrodes are promising for high-energy-density lithium-ion batteries (LIBs) due to their ability to mitigate volume expansion-induced degradation. Here, we investigate the surface dynamics of SiO thin-film electrodes cycled in different carbonate-based electrolytes using a combination of ex situ X-ray photoelectron spectroscopy (XPS) and operando synchrotron X-ray reflectivity analyses. The thin-film geometry allows us to probe the depth-dependent chemical composition and electron density from surface to current collector through the solid electrolyte interphase (SEI), the active material, and the thickness evolution during cycling.
View Article and Find Full Text PDFNew battery technologies are currently under development, and among them, all-solid-state batteries should deliver better electrochemical performance and enhanced safety. Composite solid electrolytes, combining a solid polymer electrolyte (SPE) and a ceramic electrolyte (CE), should then provide high ionic conductivity coupled to high mechanical stability. To date, this synergy has not yet been reached due to the complexity of the Li-ion transport within the hybrid solid electrolyte, especially at the SPE/CE interface currently considered the limiting step.
View Article and Find Full Text PDFRoom temperature ionic liquids (ILs) can create a strong accumulation of charges at solid interfaces by forming a very thin and dense electrical double layer (EDL). The structure of this EDL has important consequences in numerous applications involving ILs, for example, in supercapacitors, sensors, and lubricants, by impacting the interfacial capacitance, the charge carrier density of semiconductors, as well as the frictional properties of the interfaces. We have studied the interfacial structure of a long chain imidazolium-based IL (1-octyl-3-methylimidazolium dicyanamide) on several substrates: mica, silica, silicon, and molybdenum disulfide (MoS), using atomic force microscopy (AFM) experiments and molecular dynamics (MD) simulations.
View Article and Find Full Text PDFMetal-organic frameworks are a class of porous materials that show promising properties in the field of microelectronics. To reach industrial use of these materials, gas phase techniques are often preferred and were recently introduced. However, the thicknesses achieved are not sufficient, limiting further development.
View Article and Find Full Text PDFUsing Si as anode materials for Li-ion batteries remain challenging due to its morphological evolution and SEI modification upon cycling. The present work aims at developing a composite consisting of carbon-coated Si nanoparticles (Si@C NPs) intimately embedded in a three-dimensional (3D) graphene hydrogel (GHG) architecture to stabilize Si inside LiB electrodes. Instead of simply mixing both components, the novelty of the synthesis procedure lies in the in situ hydrothermal process, which was shown to successfully yield graphene oxide reduction, 3D graphene assembly production, and homogeneous distribution of Si@C NPs in the GHG matrix.
View Article and Find Full Text PDFWith the goal to improve their photostability, InP-based QDs are passivated with three types of inorganic shells, namely (i) a gradient ZnSeS shell, (ii) an additional ZnS shell on top of the gradient shell with two different thicknesses (core/shell/shell, CSS), (iii) an alumina coating on top of ZnS. All three systems have photoluminescence quantum yields (PLQY) > 50% and similar PL decay times (64-67 ns). To assess their photostability they are incorporated into a transparent poly (methyl methacrylate) (PMMA) matrix and exposed to continuous irradiation with simulated sunlight in a climate chamber.
View Article and Find Full Text PDFThe liquid-phase exfoliation of graphite is one of the most promising methods to increase production and commercial availability of graphene. Because ionic liquids can be easily obtained with chosen molecular structures and tuneable physicochemical properties, they can be use as media to optimize the exfoliation of graphite. The understanding of the interactions involved between graphite and various chemical functions in the solvent ions will be helpful to find liquids capable of dissociating and stabilizing important quantities of large graphene layers.
View Article and Find Full Text PDFHigh content nitrogen, sulfur and phosphorus heteroatoms assembled in tree-like dendrimers (DG ) are confined within the galleries of two-dimensional graphene oxide (GO). The presence of the ternary diethyl--ethyl-ammonium groups on the dendrimer peripheries ensures the exfoliation of graphene sheets thereby affording interfacially bridged, three-dimensional heteroatom-enriched graphene-based hybrid nanostructures (DG -GO). Dendrimer generation (from 1 to 4) that reflects the bulkiness of these conceived nano-trees impacts increasingly the degree of dispersion-exfoliation and sheet desordering.
View Article and Find Full Text PDFWhereas the integration of silver nanowires in functional devices has reached a fair level of maturity, the integration of copper nanowires still remains difficult, mainly due to the intrinsic instability of copper nanowires in ambient conditions. In this paper, copper nanowire based transparent electrodes with good performances (33 Ω sq associated with 88% transparency) were obtained, and their degradation in different conditions was monitored, in particular by electrical measurements, transmission electron microscopy, x-ray photoelectron spectrometry and Auger electron spectroscopy. Several routes to stabilize the random networks of copper nanowires were evaluated.
View Article and Find Full Text PDFThe linear, two-coordinate and isostructural heteroleptic [M(IPr){N(SiMe)}] (IPr = 1,3-bis(diisopropylphenyl)-imidazol-2-ylidene), formally M complexes (M = Co, 3; Fe, 4) were obtained by the reduction of [M(IPr)Cl{N(SiMe)}] with KC, or [Co(IPr){N(SiMe)}] with mes*PH, mes* = 2,4,6-tBuCH. The magnetism of 3 and 4 implies Co and Fe centres coupled to one ligand-delocalized electron, in line with XPS and XANES data; the ac susceptibility of 4 detected a pronounced frequency dependence due to slow magnetization relaxation. Reduction of [Fe(IPr)Cl{N(SiMe)}] with excess KC in toluene gave the heteronuclear 'inverse-sandwich' Fe-K complex 7, featuring η-toluene sandwiched between one Fe and one K centre.
View Article and Find Full Text PDFCopper/copper oxide (Cu/Cu O) electrodes are known to display interesting electrocatalytic performances for the reduction of CO , and thus, deserve further investigation for optimization. Here, we show that the addition of nitrogen-based organic additives greatly improves the activity of these electrodes (higher current densities, greater selectivity, and higher faradaic yields). The best effector is found to be tetramethyl cyclam.
View Article and Find Full Text PDFThe interfacing of polyoxometalates and graphene can be considered to be an innovative way to generate hybrid structures that take advantage of the properties of both components. Polyoxometalates are redox-sensitive and photosensitive compounds with high temperature stability (up to 400 °C for some), showing tunable properties depending on the metal incorporated inside the complex. Graphene has a unique electronic band structure combined with good material properties for electrical and optical applications.
View Article and Find Full Text PDFIn thin film technology, future semiconductor and display products with high performance, high density, large area, and ultra high definition with three-dimensional functionalities require high performance thin film transistors (TFTs) with high stability. Zinc oxynitride, a composite of zinc oxide and zinc nitride, has been conceded as a strong substitute to conventional semiconductor film such as silicon and indium gallium zinc oxide due to high mobility value. However, zinc oxynitride has been suffered from poor reproducibility due to relatively low binding energy of nitrogen with zinc, resulting in the instability of composition and its device performance.
View Article and Find Full Text PDFWe report the results of a VAMAS (Versailles Project on Advanced Materials and Standards) interlaboratory study on the measurement of composition in organic depth profiling. Layered samples with known binary compositions of Irganox 1010 and either Irganox 1098 or Fmoc-pentafluoro-l-phenylalanine in each layer were manufactured in a single batch and distributed to more than 20 participating laboratories. The samples were analyzed using argon cluster ion sputtering and either X-ray photoelectron spectroscopy (XPS) or time-of-flight secondary ion mass spectrometry (ToF-SIMS) to generate depth profiles.
View Article and Find Full Text PDFThe purpose of this article is to report a new method for the surface functionalization of commercially available gas diffusion layers (GDLs) by the electrochemical reduction of diazonium salt containing hydrophobic functional groups. The method results in superhydrophobic GDLs, over a large area, without pore blocking. An X-ray photoelectron spectroscopy study based on core level spectra and chemical mapping has demonstrated the successful grafting route, resulting in a homogeneous distribution of the covalently bonded hydrophobic molecules on the surface of the GDL fibers.
View Article and Find Full Text PDFThe use of mild oxidants in chemical vapor deposition (CVD) reactions has proven enormously useful. This was also true for the CVD growth of carbon nanotubes. As yet though, the use of mild oxidants in the CVD of graphene has remained unexplored.
View Article and Find Full Text PDFWe examined the ultrafast dynamics of photocarriers in nanocrystalline ZnOxNy thin films as a function of compositional variation using femtosecond differential transmittance spectroscopy. The relaxation dynamics of photogenerated carriers and electronic structures are strongly dependent on nitrogen concentration. Photocarriers of ZnOxNy films relax on two different time scales.
View Article and Find Full Text PDFInterest in oxide semiconductors stems from benefits, primarily their ease of process, relatively high mobility (0.3-10 cm(2)/vs), and wide-bandgap. However, for practical future electronic devices, the channel mobility should be further increased over 50 cm(2)/vs and wide-bandgap is not suitable for photo/image sensor applications.
View Article and Find Full Text PDFChemically bonded graphene/carbon nanotube composites as flexible supercapacitor electrode materials are synthesized by amide bonding. Carbon nanotubes attached along the edges and onto the surface of graphene act as spacers to increase the electrolyte-accessible surface area. Our lamellar structure electrodes demonstrate the largest volumetric capacitance (165 F cm(-3) ) ever shown by carbon-based electrodes.
View Article and Find Full Text PDFOur recent studies on metal-organic nanohybrids based on alkylated graphene oxide (GO), reduced alkylated graphene oxide (RGO) and InP/ZnS core/shell quantum dots (QDs) are presented. The GO alkylated by octadecylamine (ODA) and the QD bearing a dodecane thiol (DDT) ligand are soluble in toluene. The nanocomposite alkylated-GO-QD (GOQD) is readily formed from the solution mixture.
View Article and Find Full Text PDFA carbon-free Li(4)Ti(5)O(12) electrode has shown excellent electrochemical performance without any effort to enhance the electrical conductivity. Partial reduction of Ti(4+) and a metallic Li(7)Ti(5)O(12) phase are suggested to be possible origins of the exceptional behavior.
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