148 research outputs found
Controllable Synthesis of 2D Nonlayered Cr2S3 Nanosheets and Their Electrocatalytic Activity Toward Oxygen Evolution Reaction
The design of oxygen evolution reaction (OER) electrocatalysts based on Earth-abundant
materials holds great promise for realizing practically viable water-splitting systems. In this
regard, two-dimensional (2D) nonlayered materials have received considerable attention in
recent years owing to their intrinsic dangling bonds which give rise to the exposure of
unsaturated active sites. In this work, we solved the synthesis challenge in the
development of a 2D nonlayered Cr2S3 catalyst for OER application via introducing a
controllable chemical vapor deposition scheme. The as-obtained catalyst exhibits a very
good OER activity requiring overpotentials of only 230 mV and 300 mV to deliver current
densities of 10 mA cm−2 and 30 mA cm−2
, respectively, with robust stability. This study
provides a general approach to optimize the controllable growth of 2D nonlayered material
and opens up a fertile ground for studying the various strategies to enhance the water
splitting reaction
Advances in Focused Ion Beam Tomography for Three-Dimensional Characterization in Materials Science
Over the years, FIB-SEM tomography has become an extremely important technique for the three-dimensional reconstruction of microscopic structures with nanometric resolution. This paper describes in detail the steps required to perform this analysis, from the experimental setup to the data analysis and final reconstruction. To demonstrate the versatility of the technique, a comprehensive list of applications is also summarized, ranging from batteries to shale rocks and even some types of soft materials. Moreover, the continuous technological development, such as the introduction of the latest models of plasma and cryo-FIB, can open the way towards the analysis with this technique of a large class of soft materials, while the introduction of new machine learning and deep learning systems will not only improve the resolution and the quality of the final data, but also expand the degree of automation and efficiency in the dataset handling. These future developments, combined with a technique that is already reliable and widely used in various fields of research, are certain to become a routine tool in electron microscopy and material characterization
Hydrogen Desorption below 150 °c in MgH2-TiH2 Composite Nanoparticles: Equilibrium and Kinetic Properties
Reversible hydrogen sorption coupled with the MgH2 <-> Mg phase transformation was achieved in the remarkably low 340-425 K temperature range using MgH2-TiH2 composite nanoparticles obtained by reactive gas-phase condensation of Mg Ti vapors under He/H-2 atmosphere. The equilibrium pressures determined by in situ measurements at low temperature were slightly above those predicted using enthalpy Delta H and entropy Delta S of bulk magnesium. A single van't Hoff fit over a range extended up to 550 K yields the thermodynamic parameters Delta H = 68.1 0.9 kJ/molH(2) and Delta S = 119 2 J/(Kmo1H2) for hydride decomposition. A desorption rate of 0.18 wt % H-2/min was measured at T = 423 K and p(H-2) approximate to 1 mbar, i.e., close to equilibrium, without using a Pd catalysts. The nanoparticles displayed a small absorption desorption pressure hysteresis even at low temperatures. We critically discuss the influence exerted by nanostructural features such as interface free energy, elastic clamping, and phase mixing at the single nanopartide level on equilibrium and kinetic properties of hydrogen sorption
Permeability and Selectivity of PPO/Graphene Composites as Mixed Matrix Membranes for CO2 Capture and Gas Separation
We fabricated novel composite (mixed matrix) membranes based on a permeable glassy
polymer, Poly(2,6-dimethyl-1,4-phenylene oxide) (PPO), and variable loadings of few-layer graphene,
to test their potential in gas separation and CO2 capture applications. The permeability, selectivity
and diffusivity of different gases as a function of graphene loading, from 0.3 to 15 wt %, was measured
at 35 and 65 \u25e6C. Samples with small loadings of graphene show a higher permeability and
He/CO2 selectivity than pure PPO, due to a favorable effect of the nanofillers on the polymer
morphology. Higher amounts of graphene lower the permeability of the polymer, due to the
prevailing effect of increased tortuosity of the gas molecules in the membrane. Graphene also
allows dramatically reducing the increase of permeability with temperature, acting as a \u201cstabilizer\u201d
for the polymer matrix. Such effect reduces the temperature-induced loss of size-selectivity for He/N2
and CO2/N2, and enhances the temperature-induced increase of selectivity for He/CO2. The study
confirms that, as observed in the case of other graphene-based mixed matrix glassy membranes,
the optimal concentration of graphene in the polymer is below 1 wt %. Below such threshold,
the morphology of the nanoscopic filler added in solution affects positively the glassy chains packing,
enhancing permeability and selectivity, and improving the selectivity of the membrane at increasing
temperatures. These results suggest that small additions of graphene to polymers can enhance their
permselectivity and stabilize their propertie
Biological application of Compressed Sensing Tomography in the Scanning Electron Microscope
The three-dimensional tomographic reconstruction of a biological sample, namely collagen fibrils in human dermal tissue, was obtained from a set of projection-images acquired in the Scanning Electron Microscope. A tailored strategy for the transmission imaging mode was implemented in the microscope and proved effective in acquiring the projections needed for the tomographic reconstruction. Suitable projection alignment and Compressed Sensing formulation were used to overcome the limitations arising from the experimental acquisition strategy and to improve the reconstruction of the sample. The undetermined problem of structure reconstruction from a set of projections, limited in number and angular range, was indeed supported by exploiting the sparsity of the object projected in the electron microscopy images. In particular, the proposed system was able to preserve the reconstruction accuracy even in presence of a significant reduction of experimental projections
A robust, modular approach to produce graphene\u2013MOx multilayer foams as electrodes for Li-ion batteries
Major breakthroughs in batteries would require the development of new composite electrode materials, with a precisely controlled nanoscale architecture. However, composites used for energy storage are typically a disordered bulk mixture of different materials, or simple coatings of one material onto another. We demonstrate here a new technique to create complex hierarchical electrodes made of multilayers of vertically aligned nanowalls of hematite (Fe2O3) alternated with horizontal spacers of reduced graphene oxide (RGO), all deposited on a 3D, conductive graphene foam. The RGO nanosheets act as porous spacers, current collectors and protection against delamination of the hematite. The multilayer composite, formed by up to 7 different layers, can be used with no further processing as an anode in Li-ion batteries, with a specific capacity of up to 1175 \u3bcA h cm 122 and a capacity retention of 84% after 1000 cycles. Our coating strategy gives improved cyclability and rate capacity compared to conventional bulk materials. Our production method is ideally suited to assemble an arbitrary number of organic\u2013inorganic materials in an arbitrary number of layers
Improvement of Dye Solar Cell Efficiency by Photoanode Posttreatment
The basic concept for efficiency improvement in dye-sensitized solar cells (DSSC) is limiting the electron-hole recombination. One way to approach the problem is to improve the photogenerated charge carriers lifetime and consequently reduce their recombination probability. We are reporting on a facile posttreatment of the mesoporous photoanode by using a colloidal solution of TiO2 nanoparticles. We have investigated the outcome of the different sintering temperature of the posttreated photoanodes on their morphology as well as on the conversion efficiency of the DSSC. The DSSCs composed of posttreated photoanodes at 450°C showed an increase in JSC and consequently an increase in efficiency of 10%. Investigations were made to determine the electron recombination via the electrolyte by the OCVD technique. We found that the posttreatment has the effect of reducing the surface trap states and thus increases the electron lifetime, which is responsible for the increase of the overall cell efficiency
Poly(3-hexylthiophene) Nanoparticles Containing Thiophene-S,S-dioxide: Tuning of Dimensions, Optical and Redox Properties, and Charge Separation under Illumination
We describe the preparation of poly(3-hexylthiophene-S,S-dioxide) nanoparticles using Rozen's reagent, HOF·CH3CN, either on poly(3-hexylthiophene) (P3HT) or on preformed P3HT nanoparticles (P3HT-NPs). In the latter case, core-shell nanoparticles (P3HT@PTDO-NPs) are formed, as confirmed by X-ray photoelectron spectroscopy measurements, indicating the presence of oxygen on the outer shell. The different preparation modalities lead to a fine-tuning of the chemical-physical properties of the nanoparticles. We show that absorption and photoluminescence features, electrochemical properties, size, and stability of colloidal solutions can be finely modulated by controlling the amount of oxygen present. Atomic force microscopy measurements on the nanoparticles obtained by a nanoprecipitation method from preoxidized P3HT (PTDO-NPs) display spherical morphology and dimensions down to 5 nm. Finally, Kelvin probe measurements show that the coexistence of p- and n-type charge carriers in all types of oxygenated nanoparticles makes them capable of generating and separating charge under illumination. Furthermore, in core-shell nanoparticles, the nanosegregation of the two materials, in different regions of the nanoparticles, allows a more efficient charge separation
effect of charge, dipole and molecular structure
We study the mechanism of surface adsorption of organic dyes on graphene, and
successive exfoliation in water of these dye-functionalized graphene sheets. A
systematic, comparative study is performed on pyrenes functionalized with an
increasing number of sulfonic groups. By combining experimental and modeling
investigations, we find an unambiguous correlation between the graphene–dye
interaction energy, the molecular structure and the amount of graphene flakes
solubilized. The results obtained indicate that the molecular dipole is not
important per se, but because it facilitates adsorption on graphene by a
“sliding” mechanism of the molecule into the solvent layer, facilitating the
lateral displacement of the water molecules collocated between the aromatic
cores of the dye and graphene. While a large dipole and molecular asymmetry
promote the adsorption of the molecule on graphene, the stability and pH
response of the suspensions obtained depend on colloidal stabilization, with
no significant influence of molecular charging and dipole
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