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•Modification of heterogeneous photocatalytic material with gold nanoparticles.•Acetylacetone as reducing agent for the growth of gold nanoparticles (AuNPs).•Samples with different ...wt.% of Au were tested and structurally characterized.•The new Au-TiO2 material showed a lowering of band gap energy.•Photocatalytic kinetic constant for Alizarin Red S degradation was improved.
A new approach to obtain a heterogeneous photocatalytic material with gold nanoparticles and TiO2 semiconductor was performed exploiting the reducing ability of acetylacetone, a chemical present in the TiO2 paste formulation. Gold/TiO2 heterogeneous catalyst supported on polypropylene PP@Au-TiO2A was prepared; composition, structure and morphology of this new material were defined by using UV–Vis spectroscopy, Scanning Electron Microscopy (SEM), Atomic Force Microscopy (AFM), X-ray diffraction (XRD), X-ray Fluorescence (XRF), Raman Spectroscopy, Photoluminescence and Diffuse Reflectance Spectroscopy. The new material was tested in the photocatalytic degradation of Alizarin Red S in water solution, as target pollutant, under visible light and correlated with structural and spectroscopic characterizations. PP@Au-TiO2A showed higher photocatalytic activity respect to pure PP@TiO2A with an improvement of photodegradation kinetic. The best performance was obtained using PP@Au-TiO2A sample with 0.006 wt.% of Au and the photocatalytic improvement was correlated with the band gap energy decrease of photocatalyst.
Abstract Black soldier fly (BSF) melanin is a new supply of the brown-black pigment eumelanin. Given that eumelanin is a model bioelectronic material for applications such as medical devices and ...sensors, understanding BSF melanin’s electrical properties is important to confirm its viability as an advanced material. Presented here is a systematic, hydration dependent alternating current study of BSF melanin utilising both H 2 O and D 2 O vapours. There is a clear difference between the vapours, enabling a thorough analysis including Nyquist plots with model circuit analysis, broad band dielectric spectroscopic modelling as well as applying the Trukhan model to understand free ion concentration and mobility changes as a function of hydration. We find that BSF melanin behaves similarly to previous reports on synthetic systems, and the analysis here sheds additional light on potential charge transport changes. Significantly, a key finding is that there are two different mobility mechanisms for ion transport depending on hydration.
It is well known that the Al2O3 coating of the LiMn2O4 cathodes leads to improvement of the performance of these electrodes. However, the effect of the coating on the fundamental processes occurring ...on the interface with the active material which results in the formation of the solid permeable interphase is yet to be investigated. These effects should be more pronounced in the first cycle when a dynamic interaction of the active material at high voltage with the electrolyte and binder leads to the formation of this passivation layer. Here, we present a detailed investigation of the solid permeable interphase formation in alumina-coated and uncoated LiMn2O4 electrodes using X-ray absorption spectroscopy and analysis on the electrodes at the predesigned charging/discharging states. We demonstrate that the alumina coating leads to modification of the solid permeable layer and its dynamics. We also discuss the possible influences of interface modifications via coating on the battery performance.
After the recent finding that CrI3, displays ferromagnetic order down to its monolayer, extensive studies have followed to pursue new two-dimensional (2D) magnetic materials. In this article, we ...report on the growth of single crystal CrCl3 in the layered monoclinic phase. The system after mechanical exfoliation exhibits stability in ambient air (the degradation occurs on a time scale at least four orders of magnitude longer than is observed for CrI3). By means of mechanical cleavage and atomic force microscopy (AFM) combined with optical identification, we demonstrate the systematic isolation of single and few layer flakes onto 270 nm and 285 nm SiO2/Si (100) substrates with lateral size larger than graphene flakes isolated with the same method. The layer number identification has been carried with statistically significant data, quantifying the optical contrast as a function of the number of layers for up to six layers. Layer dependent optical contrast data have been fitted within the Fresnel equation formalism determining the real and imaginary part of the wavelength dependent refractive index of the material. A layer dependent (532 nm) micro-Raman study has been carried out down to two layers with no detectable spectral shifts as a function of the layer number and with respect to the bulk.
We examine the formation of the solid electrolyte interface (SEI) on anodes made of carbon encapsulated zinc ferrite (ZnFe2O4) nanoparticles (50 nm ZFO-C) as a standard metal oxide electrode ...prototype. The SEI formation and phase evolution are studied by two soft X-ray absorption techniques with different probing depths in the 10–100 nm range and by surface-sensitive X-ray photoemission spectroscopy at several specific capacities of the ZFO-C anodes. These techniques are shown to be able to provide information about the nature and extension of the individual chemical species within the SEI with a typical spatial resolution of 1–5 nm. A peculiar footprint of the interphase formations is obtained by comparing the chemical history of the reactive element sites in the anodes. The progressive development of the SEI in the first cycle and the variety of compositional transformations prior to stabilization are elucidated. Formation of a reversible alkyl carbonate layer, with maximum thickness of 7 nm, is detected at the SEI topmost region. On the basis of these results, we have obtained a map of suitable spatial resolution of the evolution of the different components of the interface layer.
We investigate the experimentally challenging CrCl3 surface by photon energy dependent photoemission (PE). The core and valence electrons after cleavage of a single crystal, either in a ultra-high ...vacuum (UHV) or in air, are studied by keeping the samples at 150 °C, aiming at confirming the atomic composition with respect to the expected bulk atomic structure. A common spectroscopic denominator revealed by data is the presence of a stable, but only partially ordered Cl–O–Cr surface. The electronic core levels (Cl 2p, Cr 2p and 3p), the latter ones of cumbersome component determination, allowed us to quantify the electron charge transfer to the Cr atom as a net result of this modification and the increased exchange interaction between metal and ligand atoms. In particular, the analysis of multiplet components by the CMT4XPS code evidenced the charge transfer to be favored, and similarly the reduced crystal field due to the established polarization field. Though it is often claimed that a significant amount of Cl and Cr atomic vacancies has to be included, such a possibility can be excluded on the basis of the sign and the importance of the shift in the binding energy of core level electrons. The present methodological approach can be of great impact to quantify the structure of ordered sub-oxide phases occurring in mono or bi-layer Cr trihalides.
We investigate the experimentally challenging CrCl
surface by photon energy dependent photoemission (PE). The core and valence electrons after cleavage of a single crystal, either in a ultra-high ...vacuum (UHV) or in air, are studied by keeping the samples at 150 °C, aiming at confirming the atomic composition with respect to the expected bulk atomic structure. A common spectroscopic denominator revealed by data is the presence of a stable, but only partially ordered Cl-O-Cr surface. The electronic core levels (Cl 2p, Cr 2p and 3p), the latter ones of cumbersome component determination, allowed us to quantify the electron charge transfer to the Cr atom as a net result of this modification and the increased exchange interaction between metal and ligand atoms. In particular, the analysis of multiplet components by the CMT4XPS code evidenced the charge transfer to be favored, and similarly the reduced crystal field due to the established polarization field. Though it is often claimed that a significant amount of Cl and Cr atomic vacancies has to be included, such a possibility can be excluded on the basis of the sign and the importance of the shift in the binding energy of core level electrons. The present methodological approach can be of great impact to quantify the structure of ordered sub-oxide phases occurring in mono or bi-layer Cr trihalides.
The implementation of high potential materials as positive electrodes in high energy Li-ion batteries requires to develop scalable and smart synthetic routes. In the case of the LiNi0.5Mn1.5O4 (LNMO) ...spinel material, a successful preparation strategy must drive the phase formation in order to obtain structural, morphological and surface properties capable to boost performances in lithium cells and minimize the electrolyte degradation. Here we discuss a novel simple and easily scalable mechanochemical synthetic route, followed by a high temperature annealing in air, to prepare LMNO materials starting from oxides. A synergic doping with chromium and iron has been incorporated, resulting in the spontaneous segregation of a CrOx-rich surface layer. The effect of the annealing temperature on the physico-chemical properties of the LMNO material has been investigated as well as the effect on the performances in Li-cells.
FERMI@Elettra is a free electron-laser (FEL)-based user facility that, after two years of commissioning, started preliminary users' dedicated runs in 2011. At variance with other FEL user facilities, ...FERMI@Elettra has been designed to deliver improved spectral stability and longitudinal coherence. The adopted scheme, which uses an external laser to initiate the FEL process, has been demonstrated to be capable of generating FEL pulses close to the Fourier transform limit. We report on the first instance of FEL wavelength tuning, both in a narrow and in a large spectral range (fine- and coarse-tuning). We also report on two different experiments that have been performed exploiting such FEL tuning. We used fine-tuning to scan across the 1s-4p resonance in He atoms, at 23.74 eV (52.2 nm), detecting both UV-visible fluorescence (4p-2s, 400 nm) and EUV fluorescence (4p-1s, 52.2 nm). We used coarse-tuning to scan the M4,5 absorption edge of Ge (∼29.5 eV) in the wavelength region 30-60 nm, measured in transmission geometry with a thermopile positioned on the rear side of a Ge thin foil.
The use of Polypropylene as support material for nano-TiO2 photocatalyst in the photodegradation of Alizarin Red S in water solutions under the action of visible light was investigated. The ...optimization of TiO2 pastes preparation using two commercial TiO2, Aeroxide P-25 and Anatase, was performed and a green low-cost dip-coating procedure was developed. Scanning electron microscopy, Atomic Force Microscopy and X-Ray Diffraction analysis were used in order to obtain morphological and structural information of as-prepared TiO2 on support material. Equilibrium and kinetics aspects in the adsorption and successive photodegradation of Alizarin Red S, as reference dye, are described using polypropylene-TiO2 films in the Visible/TiO2/water reactor showing efficient dyes degradation.
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