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Register a new userPhotocatalytic hydrogen production of Co(OH)2 nanoparticle-coated {alpha}-Fe2O3 nanorings
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Added by
Luiz Fernando Zagonel
Publication date
2016
fields
Physics
and research's language is
English
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The production of hydrogen from water using only a catalyst and solar energy is one of the most challenging and promising outlets for the generation of clean and renewable energy. Semiconductor photocatalysts for solar hydrogen production by water photolysis must employ stable, non-toxic, abundant and inexpensive visible-light absorbers capable of harvesting light photons with adequate potential to reduce water. Here, we show that a-Fe2O3 can meet these requirements by means of using hydrothermally prepared nanorings. These iron oxide nanoring photocatalysts proved capable of producing hydrogen efficiently without application of an external bias. In addition, Co(OH)2 nanoparticles were shown to be efficient co-catalysts on the nanoring surface by improving the efficiency of hydrogen generation. Both nanoparticle-coated and uncoated nanorings displayed superior photocatalytic activity for hydrogen evolution when compared with TiO2 nanoparticles, showing themselves to be promising materials for water-splitting using only solar light.
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Single-crystalline alpha-Fe2O3 nanorings (short nanotubes) and nanotubes were synthesized by a hydrothermal method. High-resolution transmission electron microscope and selected-area electron diffraction confirm that the axial directions of both nanorings and nanotubes are parallel to the crystalline c-axis. What is intriguing is that the Morin transition occurs at about 210 K in the short nanotubes with a mean tube length of about 115 nm and a mean outer diameter of 169 nm while it disappears in the nanotubes with a mean tube length of about 317 nm and a mean outer diameter of 148 nm. Detailed analyses of magnetization data, x-ray diffraction spectra, and room-temperature Mossbauer spectra demonstrate that this very strong shape dependence of the Morin transition is intrinsic to hematite. We can quantitatively explain this intriguing shape dependence in terms of opposite signs of the surface magnetic anisotropy constants in the surface planes parallel and perpendicular to the c-axis (that is, K_parallel = -0.37 erg/cm^2 and K_perp = 0.42 erg/cm^{2}).
We report the magnetotransport properties of self-assembled Co@CoO nanoparticle arrays at temperatures below 100 K. Resistance shows thermally activated behavior that can be fitted by the general expression of R exp{(T/T0)^v}. Efros-Shklovskii variable range hopping (v=1/2) and simple activation (hard gap, v=1) dominate the high and low temperature region, respectively, with a strongly temperature-dependent transition regime in between. A giant positive magnetoresistance of >1,400% is observed at 10K, which decreases with increasing temperature. The positive MR and most of its features can be explained by the Zeeman splitting of the localized states that suppresses the spin dependent hopping paths in the presence of on-site Coulomb repulsion.
We investigate the photocatalytic performance of nanocomposites prepared in a one-step process by liquid-phase exfoliation of graphite in the presence of TiO$_2$ nanoparticles (NPs) at atmospheric pressure and in water, without heating or adding any surfactant, and starting from low-cost commercial reagents. The nanocomposites show enhanced photocatalytic activity, degrading up to 40$%$ more pollutants with respect to the starting TiO$_2$-NPs. In order to understand the photo-physical mechanisms underlying this enhancement, we investigate the photo-generation of reactive species (trapped holes and electrons) by ultrafast transient absorption spectroscopy. We observe an electron transfer process from TiO$_2$ to the graphite flakes within the first picoseconds of the relaxation dynamics, which causes the decrease of the charge recombination rate, and increases the efficiency of the reactive species photo-production.
We study the optical properties of gold nanoparticles coated with a nematic liquid crystal whose director field is distributed around the nanoparticle according to the anchoring conditions at the surface of the nanoparticle. The distribution of the nematic liquid crystal is obtained by minimization of the corresponding Frank free-energy functional whilst the optical response is calculated by the discrete-dipole approximation. We find, in particular, that the anisotropy of the nematic liquid-crystal coating does not affect much the (isotropic) optical response of the nanoparticle. However, for strong anchoring of the nematic liquid-crystal molecules on the surface of nanoparticle, the inhomogeneity of the coating which is manifested by a ring-type singularity (disclination or Saturn ring), produces an enhancement of the extinction cross spectrum over the entire visible spectrum.
Defined substoichiometric titanium oxides (Ti$_x$O$_{2x-1}$ with $3 < x < 10$) called Magneli phases have been investigated mostly for their unusual high conductivity and metal-like behavior. In photocatalysis, Magneli phase containing titania particles have been reported to provide favorable charge separation resulting in enhanced reaction efficiency. In the current work we describe a one-step synthesis of Magneli-containing mixed phase nanoparticles that carry directly integrated minute amounts of Pt. Phase optimized nanoparticles that contain only a few hundred ppm Pt are very effective photocatalysts for H$_2$ evolution (they provide a 50-100 times higher H$_2$ evolution than plain anatase loaded with a similar amount of Pt). These photocatalysts are synthesized in a setup combining a hot-wall reactor that is used for TiOx synthesis with a spark generator producing Pt nanoparticles. Different reactor temperatures result in various phase ratios between anatase and Magneli phases. The titania nanoparticles (ca. 24 - 53 nm) were characterized using XRD, HRTEM, XPS and EPR spectra as well as ICP-OES analysis. The best photocatalyst prepared at 900$^circ$C (which consists of mixed phase particles of 32% anatase, 11% rutile and 57% Magneli phases loaded with 290 ppm of Pt) can provide a photocatalytic H$_2$ evolution rate of ca. 5432 micromol h$^{-1} g$^{-1}$ for UV and ca. 1670 micromol h$^{-1} g$^{-1}$ for AM1.5 illumination. For powders converted to higher amounts of Magneli phases (1000$^circ$C and 1100$^circ$C), a drastic loss of the photocatalytic H$_2$ generation activity is observed. Thus, the high photocatalytic efficiency under best conditions is ascribed to an effective synergy between multi-junctions of Magneli titania and Pt that enable a much more effective charge separation and reaction than conventional Pt/anatase junctions.
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