154 resultados para ONE-ELECTRON OXIDATION


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In our previous work, it was shown that LiLaNiO/gamma-Al2O3 was an excellent catalyst for partial oxidation of heptane to syngas in a fixed-bed reactor at high temperature and the selectivity of CO was about 93%. However, pure oxygen was used as the oxidant. We have developed a dense oxygen permeation membrane Ba0.5Sr0.5Co0.8Fe0.2O3 that can supply pure oxygen for the reaction. In this work, the membrane was combined with the catalyst LiLaNiO/gamma-Al2O3 in one rector for the partial oxidation of heptane that is typical component of gasoline. A good performance of the membrane reactor has been obtained, with 100% n-heptane conversion and >94% hydrogen selectivity at the optimized reaction conditions. (C) 2004 Elsevier B.V. All rights reserved.

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The structures, properties and electron transfer reactivity of the ClO/ClO- coupling system are studied in this paper at ab initio (UHF and UMP2) levels and the Density Functional Theory (DFT: UB3LYP, UB3P86, UB3PW91) levels employing 6311 + G(3df) basis set and on the basis of the Golden-rule of the time-dependent perturbation theory. Investigations indicate that the results obtained using the UB3LYP method employing 6-311 + G(3df) basis set is in excellent agreement with the experiment. For this coupling system, six stable coupling modes have been found which correspond to six different encounter complexes and denote six different electron transfer mechanism: four O-O directly linked structures (one collinear: D-h, one anti-parallel: C-s, two twist: C-2) and two Cl-O linked structures (cis- and anti- C-s structures). The activation energies, the stabilization energies and the electronic coupling matrix elements have also been calculated for the electron transfer reactions via these six different mechanism at the UB3LYP/6-311 + G(3df) level, and then the electron transfer rates are determined at the same level. The most favorable coupling mode to the electron transfer is the anti-parallel mechanism. The averaged electron transfer rate is about 5.58 X 10(11) M-1 s(-1). It is also implied that the B3LYP method can give more reasonable results for the electron transfer reactivity of this system. (C) 2003 Elsevier B.V. All rights reserved.

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City Univ Hong Kong

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Three-dimensional (3D) macroporous Pt (MPPt) with highly open porous walls has been successfully synthesized using the hydrogen bubble dynamic template synthesis and galvanic replacement reaction. Scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and electrochemical methods were adopted to characterize their structures and properties.

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Here we present a simple wet-chemical approach to synthesize flower-like silver nanostrip assembling architecture at room temperature. Transmission electron microscopy (TEM) and scanning electron microscopy (SEM) images indicate that these microstructures with the diameter of similar to 500nm exhibit hietarchical characteristic. X-ray diffraction (XRD), energy-dispersed X-ray spectroscopy (EDX) and Raman spectroscopy indicate that poly (o-diaminobenzene) (PDB) also exists in the silver hierarchical microstructure.

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Highly crystalline and nearly monodisperse In2O3 nanocrystals with both cube and flower shapes were successfully synthesized in one step through a facile aqueous solvothermal method for the first time, free of any surfactant or template. X-ray diffraction (XRD), transmission electron microscopy (TEM), selective area electron diffraction (SAED), and high-resolution transmission electron microscopy (HRTEM) were used to characterize the samples. In our work, the use of diethylene glycol (DEG) is a crucial factor for the formation of the In2O3 phase.

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In this paper, nanocrystalline YVO4:Eu3+ powders have been successfully synthesized via high-temperature solution-phase synthesis process. The nanocrystalline YVO4:Eu3+ particles were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), UVNis absorption spectra and luminescence spectra, luminescence decay curve and Fourier transform infrared (FT-IR), X-ray photoelectron spectra (XPS) respectively. The as-prepared nanocrystalline YVO4:Eu3+ particles are well crystallized with ellipsoidal morphology.

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A novel method for immobilization of tris(2,2'-bipyridyl)ruthenium(II) (Ru(bpy)(3)Cl-2) on electrode surfaces based on the vapor-surface sol-gel deposition strategy is first demonstrated in this paper. Ru(bpy)(3)Cl-2 immobilized sol-gel (Ru(bpy)(3)Cl-2/sol-gel) films were characterized by UV-vis spectroscopy and field-emitted scanning electron microscopy (FE-SEM). These results showed that Ru(bpy)(3)Cl-2 was successfully incorporated into the silica sol-gel film. it was found that many irregular Ru(bpy)(3)Cl-2/sol-gel clusters were formed on surfaces through one deposition and thick sol-gel films were observed after further deposition.

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A novel water-soluble electroactive polymer, aniline pentamer crosslinked chitosan (Pentamer-c-Chi), was prepared by condensation polymerization of the terminal carboxyl groups in aniline pentamer with the amino side groups in chitosan in aqueous solution. The carboxyl groups were activated by N-hydroxysuccinimide (NHS) and N,N'-dicyclohexylcarbodiimide (I)CC). The electrochemical behavior of aniline pentamer in this kind of crosslinked polymer was studied in acidic aqueous solution by means of cyclic voltammetry (CV), UV-vis, and electron spin resonance (ESR) spectroscopy.

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Both the behavior and the general key factors for assembling flexible SWNT films at the water/oil interface were investigated; the electron transfer, one of the most fundamental chemical processes, at the SWNT-sandwiched water/oil interface was also firstly illustrated using scanning electrochemical microscopy.

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A simple layer-by-layer (LBL) electrostatic adsorption technique was developed for deposition of films composed of alternating layers of positively charged poly(diallyldimethylammonium chloride) (PDDA) and negatively charged multiwall carbon nanotubes bearing platinum nanoparticles (Pt-CNTs). PDDA/Pt-CNT film structure and morphology up to six layers were characterized by scanning electron microscopy and ultraviolet-visible spectroscopy, showing the Pt-CNT layers to be porous and uniformly deposited within the multilayer films.

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A selective oxidation technique has been applied to form a diffusion barrier on the Ni-based superalloy substrate by heating the substrate with electron beam of the electron beam-physical vapor deposition (EB-PVD) facility. The interdiffusion behavior, cross-sectional morphology, isothermal and cyclic oxidations were studied for thermal barrier coatings (TBCs) with and without diffusion barrier.

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A novel colloid method using (WO3)(n)center dot xH(2)O as colloidal source was developed to prepare Pd/C catalyst for formic acid oxidation. Transmission electron microscopy image shows that the Pd/C nanoparticles have an average size of 3.3 nm and a narrow size distribution. Electrochemical measurements indicate that the Pd/C catalyst exhibits significantly high electrochemical active surface area and high catalytic activity with good stability for formic acid oxidation compared with that prepared by common method.

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A simple and rapid synthesis method (denoted as modified impregnation method, MI) for PtRu/CNTs (MI) and PtRu/C (MI) was presented. PtRu/CNTs (MI) and PtRu/C (MI) catalysts were characterized by transmission electron microscopy (TEM) and X-ray diffractometry. It was shown that Pt-Ru particles with small average size (2.7 nm) were uniformly dispersed on carbon supports (carbon nanotubes and carbon black) and displayed the characteristic diffraction peaks of Pt face-centered cubic structure.

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NaYF4:Yb3+, Er3+ nanoparticles were successfully prepared by a polyol process using diethyleneglycol (DEG) as solvent. After being functionalized with SiO2-NH2 layer, these NaYF4:Yb3+, Er3+ nanoparticles can conjugate with activated avidin molecules (activated by the oxidation of the oligosaccharide chain). The as-formed NaYF4:Yb3+, Er3+ nanoparticles, NaYF4:Yb3+, Er3+ nanoparticles functionalized with amino groups, avidin conjugated amino-functionalized NaYF4:Yb3+, Er3+ nanoparticles were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), atomic force microscopy (AFM), Fourier transform infrared (FT-IR), UV/Vis absorption spectra, and up-conversion luminescence spectra, respectively.