355 resultados para Aerobic oxidation


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In this paper, it was found that the electrocatalytic activity of a Pt electrode for the electro-oxidation of formic acid could be dramatically enhanced with the modification of macrocycle compounds, such as iron-tetrasulfophthalocyanine (FeTSPc). The electro-oxidation of formic acid on a modified Pt electrode with FeTSPc occurs mainly through a direct pathway. A series of macrocycle compounds were also investigated as modifiers and exhibited a promotion effect similar to the Pt electrode.

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The mechanism of formic acid electrooxidation on iron tetrasulfophthalocyanine (FeTSPc) modified Pt electrode was investigated with electrochemical methods. It was found that a "third-body" effect of FeTSPc on Pt electrode predominates during the electrooxidation process based on unusual electrochemical results. The modification leads formic acid electrooxidation to take place through a desired direct pathway, in which the mechanism is proposed to be the gradual dehydrogenation of formic acid and the reaction of formate with hydroxyl species.

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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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Pd/C catalysts with designed lattice constants were synthesized for the electro-oxidation of formic acid. By changing the solvents in the preparation procedure, it was demonstrated that the different lattice constants of Pd crystallites could be controlled as desired. The varied lattice constants may be attributed to the difference in the interactions between solvents and PdCl2. it was found that the lattice constant had an obvious effect on the electro-catalytic performance of Pd.

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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.

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We firstly reported a novel polymer matrix fabricated by type I collagen and polymers, and this matrix can be used as nanoreactors for electrodepositing platinum nanoclusters (PNCs). The type I collagen film has a significant effect on the growth of PNCs. The size of the platinum nanoparticles could be readily tuned by adjusting deposition time, potential and the concentration of electrolyte, which have been verified by field-emitted scanning electron microscopy (FE-SEM). Furthermore, cyclic voltammetry (CV) has demonstrated that the as-prepared PNCs can catalyze methanol directly with higher activity than that prepared on PSS/PDDA film, and with better tolerance to poisoning than the commercial E-TEK catalyst. The collagen-polymer matrix can be used as a general reactor to electrodeposit other metal nanostructures.

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Liquid phase oxidation of cyclohexane was carried out under mild reaction condition over copper pyrophosphate catalyst in CH3CN using hydrogen peroxide as an oxidant at the temperature between 25 and 80 degrees C. The copper pyrophosphate catalyst was characterized by means of XRD, FT-IR and water contact angle measurement. It was found that appropriate surface hydrophobicity is the key factor for the excellent performance of the catalyst. In addition, a significant improvement for the cyclohexane conversion in the presence of organic acid was observed.

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Electrospun carbon nanofiber-supported bimetallic PtxAu100-x electrocatalysts (PtxAu100-x/CNF) were prepared by electrochemical codeposition method. The composition of PtAu bimetallic nanoparticles could be controlled by varying the ratio of H2PtCl6 and HAuCl4. Scanning electron microscopy images showed that bimetallic nanoparticles had coarse surface morphology with high electrochemically active surface areas. X-ray diffraction analysis testified the formation of PtAu alloys. PtxAu100-x/CNF electrocatalysts exhibited improved electrocatalytic activities towards formic acid oxidation by providing the selectivity of the reaction via dehydrogenation pathway and suppressing the formation/adsorption of poisoning CO intermediate, indicating that PtxAu100-x/CNF is promising electrocatalyst in direct formic acid fuel cells.

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A modified impregnation method was used to prepare highly dispersive carbon-supported PtRu catalyst (PtRu/C). Two modifications to the conventional impregnation method were performed: one was to precipitate the precursors ((NH4)(2)PtCl6 and Ru(OH)(3)) on the carbon support before metal reduction: the other was to add a buffer into the synthetic solution to stabilize the pH. The prepared catalyst showed a much higher activity for methanol electro-oxidation than a catalyst prepared by the conventional impregnation method. even higher than that of current commercially available, state-of-the-art catalysts. The morphology of the prepared catalyst was characterized using TEM and XRD measurements to determine particle sizes, alloying degree, and lattice parameters. Electrochemical methods were also used to ascertain the electrochemical active surface area and the specific activity of the catalyst.

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Non-ionic surfactant Triton X-100 was used as a stabilizer to prepare PtRu/C catalysts for methanol oxidation reaction (MOR). The cyclic voltammogram was used to investigate the catalytic activity for MOR of different PtRu/C catalysts. TG-DTA, EDX, XRD, XPS and TEM were Used to characterize the composition, structure and morphology of the as-prepared PtRu/C catalysts. It is found that the heat treatment plays a crucial role in the particles size, particles distribution of the PtRu/C catalysts and the oxidation state of platinum. The results show that 350 degrees C is an optimum heat treatment temperature. The as-synthesized catalyst heat-treated at this temperature exhibits the best catalytic performance for MOR.

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The oxidation of formic acid at the Pd/C catalyst electrode is a completely irreversible kinetic process with the reaction order of 1.0. The oxidation rate of formic acid is increased with increasing the concentration of formic acid and is decreased with increasing H+ concentration. The apparent negative reaction order with respect to H+ is about -0.18 or -0.04 in H2SO4 or HClO4 solution respectively, because bisulfate anions would inhibit formic acid oxidation at some extent. The kinetic parameters, charge transfer coefficient and the diffusion coefficient of formic acid were obtained under the quasi steady-state conditions.

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Preparation of monodispersed platinum nanoparticles with average size 2.0 nm stabilized by amino-terminated ionic liquid was demonstrated. The resulting platinum nanoparticles (Pt-IL) retained long-term stability without special protection. The Pt-IL nanoparticles exhibited high electrocatalytic activity toward reduction of oxygen and oxidation of methanol. Rotating disk electrode voltammetry and rotating ring-disk electrode voltammetry confirmed that the Pt-IL films could catalyze an almost four-electron reduction of dioxygen to water.

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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. The biofunctionalization of the NaYF4:Yb3+, Er3+ nanoparticles has less effect on their luminescence properties, i.e., they still show the up-conversion emission (from Er3+, with S-4(3/2) -> I-4(15/2) at similar to 540 nm and F-4(9/2) -> I-4(15/2) at similar to 653 nm), indicative of the great potential for these NaYF4:Yb3+, Er3+ nanoparticles to be used as fluorescence probes for biological system.

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Ti70Zr10Co20 containing an icosahedral quasicrystalline phase has been fabricated, and presents high activity and selectivity in catalyzing the oxidation of cyclohexane with oxygen under solvent-free conditions.