35 resultados para ELECTROCATALYST

em Chinese Academy of Sciences Institutional Repositories Grid Portal


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A 40 wt% Pt/C cathode electrocatalyst with controlled Pt particle size of similar to 2.9 nm showing better performance than commercial catalyst for direct methanol fuel cell was prepared by a polyol process with water but without using stabilizing agent.

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The electrocatalysts of Pt/C, PtRu/C and Ru/C were prepared by the impregnation method. The facet characterization, the dispersion and the particle size for the catalysts were determined by means of X-ray diffraction and transmission electron microscopy. X-ray photoelectron spectroscopy was also used to analyze the state and the valency of the noble metals. The results show that the particle size was in nanometer range and the binary metals have come into being an alloy. The platinum in the catalysts existed in zero valency. The valency of the ruthenium on the surface is different from that in the body, while the ruthenium on the surface existed in oxide-form. PtRu/C and Pt/C are of good activity to the electrooxidation of hydrogen except Ru/C. PtRu/C is more tolerant of CO than Pt/C, and CO is only adsorbed on Pt.

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In this paper, a hollow Au/Pd core/shell nanostructure with a raspberry surface was developed for methanol, ethanol, and formic acid oxidation in alkaline media. The results showed that it possessed better electrocatalyst performance than hollow Au nanospheres or Pd nanoparticles. The nanostructure was fabricated via a two-step method. Hollow Au nanospheres were first synthesized by a galvanic replacement reaction, and then they were coated with a layer of Pd grains. Several characterizations such as transmission electron microscopy (TEM), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), and X-ray photoelectron spectroscopy (XPS) were used to investigate the prepared nanostructures.

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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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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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A prominent methanol-tolerant characteristic of the PtCeOx/C electrocatalyst was found during oxygen reduction reaction process. The carbon-supported platinum modified with cerium oxide (PtCeOx/C) as cathode electrocatalyst for direct methanol fuel cells was prepared via a simple and effective route. The synthesized electrocatalysts were characterized by X-ray diffraction and transmission electron microscopy. It was found that the cerium oxide within PtCeOx/C present in an amorphous form on the carbon support surface and the PtCeOx/C possesses almost similar disordered morphological structure and slightly smaller particle size compared with the unmodified Pt/C catalyst.

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The PtRu/C electrocatalyst with high loading (PtRu of 60 wt%) was prepared by synergetic effect of ultrasonic radiation and mechanical stirring. Physicochemical characterizations show that the size of PtRu particles of as-prepared PtRu/C catalyst is only several nanometers (2-4 nm), and the PtRu nanoparticles were homogeneously dispersed on carbon surface. Electrochemistry and single passive direct methanol fuel cell (DMFC) tests indicate that the as-prepared PtRu/C electrocatalyst possessed larger electrochemical active surface (EAS) area and enhanced electrocatalytic activity for methanol oxidation reaction (MOR). The enhancement could be attributed to the synergetic effect of ultrasound radiation and mechanical stirring, which can avoid excess concentration of partial solution and provide a uniform environment for the nucleation and growth of metal particles simultaneously hindering the agglomeration of PtRu particles on carbon surface.

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A high-efficiency and low-cost spongelike Au/Pt core/shell electrocatalyst with hollow cavity has been facilely obtained via a simple two-step wet chemical process. Hollow gold nanospheres were first synthesized via a modified galvanic replacement reaction between Co nanoparticles in situ produced and HAUCl(4). The as-prepared gold hollow spheres were employed as seeds to further grow spongelike Pt shell. It is found that the surface of this hybrid nanomaterial owns many Pt nanospikes, which form a spongelike nanostructure. All experimental data including scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, and UV-vis-near-infrared spectroscopy have been employed to characterize the obtained Au/Pt hybrid nanomaterial. The rapid development of fuel cell has inspired us to investigate the electrocatalytic properties for dioxygen and methanol of this novel hybrid nanomaterial. Spongelike hybrid nanomaterial mentioned here exhibits much higher catalytic activity for dioxygen reduction and methanol oxidation than the common Pt electrode.

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The deliberate tailoring of nanostructured metallic catalysts at the monolayer-level is an ongoing challenge and could lead to new electronic and catalytic properties, since surface-catalyzed reactions are extremely sensitive to the atomic-level details of the catalytic surface. In this article, we present a novel electrochemical strategy to nanoparticle-based catalyst design using the recently developed underpotential deposition (UPD) redox replacement technique. A single UPD Cu replacement with Pt2+ yielded a uniform Pt layer on colloid gold surfaces. The ultrathin (nominally monolayer-level) Pt coating of the novel nanostructured particles was confirmed by cyclic voltammetry and X-ray photoelectron spectra (XPS). The present results demonstrate that ultrathin Pt coating effects efficiently and behaves as the nanostructured monometallic Pt for electrocatalytic oxygen reduction, and also shows size-dependent, tunable electrocatalytic ability. The as-prepared ultrathin Pt-coated Au nanoparticle monolayer electrodes reduce O-2 predominantly by four electrons to H2O, as confirmed by the rotating ring-disk electrode (RRDE) technique.

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In this paper, a simple route for the preparation of Pt nanoparticles is described. PtCl62- and [tetrakis-(N-methylpyridyl)porphyrinato] cobalt (CoTMPyP) were assembled on a 4-aminobenzoic acid modified glassy carbon electrode through the layer-by-layer method. The three-dimensional Pt nanoparticle films are directly formed on an electrode surface by electrochemical reduction of PtCl62- sandwiched between CoTMPyP layers. Regular growth of the multilayer films is monitored by UV-vis spectroscopy. X-ray photoelectron spectroscopy verifies the constant composition of the multilayer films containing Pt nanoparticles. Atomic force microscopy proves that the as-prepared Pt nanoparticles are uniformily distributed with average particle diameters of 6-10 nm. The resulting multilayer films containing Pt nanoparticles on the modified electrode possess catalytic activity for the reduction of dissolved oxygen. Rotating disk electrode voltammetry and rotating ring-disk electrode voltammetry confirm that Pt nanoparticle containing films can catalyze an almost four-electron reduction of O-2 to water in 0.5 M H2SO4 solution.

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It is reported for the first time that the Pt/TiO2 electrocatalyst was successfully used for the electrocatalytic oxidation of CO in the electrochemical gas sensor with a controlled potential mode. The stability of electrocatalytic activity of the Pt-TiO2 electrocatalyst for the CO oxidation is better than that of Pt.