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1.
Nano Lett ; 11(2): 361-4, 2011 Feb 09.
Artigo em Inglês | MEDLINE | ID: mdl-21204550

RESUMO

Herein we demonstrate the extra-low-temperature oxygen storage capacity (OSC) of cerium oxide nanocrystals with cubic (100) facets. A considerable OSC occurs at 150 °C without active species loading. This temperature is 250 °C lower than that of irregularly shaped cerium oxide. This result indicates that cubic (100) facets of cerium oxide have the characteristics to be a superior low-temperature catalyst.


Assuntos
Cério/química , Cristalização/métodos , Nanoestruturas/química , Nanoestruturas/ultraestrutura , Nanotecnologia/métodos , Oxigênio/química , Oxigênio/isolamento & purificação , Temperatura Baixa , Substâncias Macromoleculares/química , Teste de Materiais , Conformação Molecular , Tamanho da Partícula , Propriedades de Superfície
2.
J Am Chem Soc ; 132(38): 13154-5, 2010 Sep 29.
Artigo em Inglês | MEDLINE | ID: mdl-20825187

RESUMO

We introduce a new concept for a nanomaterial in terms of both synthesis and properties. The nanomaterial, aggregates of ceria particles around central silver metal (CeO(2)-Ag), was fabricated by a one-pot selective redox reaction using cerium(III) and silver(I) autocatalyzed by silver metal without the need for surfactants or organic compounds. This unique nanostructure is suitable as a catalyst, in contrast to core-shell materials wherein the shell deactivates the catalyst metal. The material was developed to be intimately related to catalytic carbon oxidation.

3.
Phys Chem Chem Phys ; 12(10): 2365-72, 2010 Mar 14.
Artigo em Inglês | MEDLINE | ID: mdl-20449349

RESUMO

States of NO(2) adsorption and kinetics of NO(2) desorption over a Fe-loaded ZSM-5 type zeolite were investigated using Fourier transform infrared (FT-IR) spectroscopy and temperature-programmed desorption (TPD). The FT-IR spectra in NO(2)/N(2) flows showed that several adsorption species (NO(2), nitrite, nitrate, and NO(+)) existed; except for NO(2), these were considered to be formed via NO(2) dimerization and disproportionation reactions. The TPD spectra showed two distinct peaks, a low-temperature (LT) peak that can be assigned to weakly adsorbed NO(x) in the zeolite channel and a high-temperature (HT) peak that can be assigned to chemisorbed NO(x) bonded to ion-exchanged Fe sites. By varying flow rates and heating rates in TPD measurements, the peak maximum temperatures in the both peaks were found to be constant with the former, but shifted to higher temperatures with the latter; this suggests that desorption is not controlled by an adsorption/desorption equilibrium, i.e., in the no-readsorption limit. Furthermore, it was found that desorption at both LT and HT peaks proceeds at second order; this implies that the reverse reaction of NO(2) dimerization and disproportionation and/or some sort of lateral interaction between NO(2) molecules might be occurring. The desorption energies and the pre-exponential factors were estimated to be 67 +/- 1 kJ mol(-1) and 10(5.5+/-0.2) s(-1) for the LT peak and 138 +/- 4 kJ mol(-1) and 10(9.8+/-0.3) s(-1) for the HT peak. These values show that interaction strengths between adsorbed NO(x) and Fe sites are relatively large.


Assuntos
Ferro/química , Dióxido de Nitrogênio/química , Temperatura , Zeolitas/química , Adsorção , Catálise , Cinética , Espectroscopia de Infravermelho com Transformada de Fourier , Propriedades de Superfície
4.
Rev Sci Instrum ; 78(10): 104102, 2007 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-17979437

RESUMO

A procedure for the quantitative analysis of transient surface catalytic reactions in millisecond time resolution has been studied constructing a specially designed apparatus employing (1) pulsed-gas valves for the injection of reactant molecules onto catalysts and (2) a time-of-flight mass spectrometer (TOF-MS) to detect every reaction product simultaneously. For a better understanding of the catalytic activity and selectivity for products quantitatively, a procedure for measuring an amount of reactant molecules injected onto catalyst surface and calibrating the intensity of mass signal were proposed and implemented. We tested the applicability of this procedure for the quantitative analysis of products of NO+H(2) reaction on Pt-Al(2)O(3) catalysts (a planar catalyst: Pt-Al(2)O(3)Si substrates inserted into a micro-tube-reactor with SiC balls). Although the surface area of the planar catalyst was very small, the mass signal intensities of the reaction products were found to be sufficient for the above procedure. We measured the fragmentation patterns and the inherent sensitivity factors in the TOF-MS using the mixture of the internal standard gas Ar and the N-containing gases. The relative sensitivity factors for NH(3), N(2), NO, and N(2)O and the relative intensities of fragment peaks to the molecular ion peak of H(2)O and N(2)O were estimated. The procedure constructed here has enabled us to analyze the transient consecutive secondary catalytic reactions as well as primary reactions based on the formation rate of product molecules per millisecond instead of the mass signal intensities of the reaction products.


Assuntos
Análise de Injeção de Fluxo/instrumentação , Teste de Materiais/instrumentação , Manejo de Espécimes/instrumentação , Espectrometria de Massas por Ionização e Dessorção a Laser Assistida por Matriz/instrumentação , Propriedades de Superfície , Catálise , Desenho de Equipamento , Análise de Falha de Equipamento , Análise de Injeção de Fluxo/métodos , Teste de Materiais/métodos , Reprodutibilidade dos Testes , Sensibilidade e Especificidade , Manejo de Espécimes/métodos , Espectrometria de Massas por Ionização e Dessorção a Laser Assistida por Matriz/métodos
8.
Chem Commun (Camb) ; 48(89): 10987-9, 2012 Nov 18.
Artigo em Inglês | MEDLINE | ID: mdl-23034602

RESUMO

Mesoporous ferrihydrite nanoparticles with incorporated Mn (MMnFh) were prepared for the first time, and MMnFh exhibits excellent performance in removing organic contaminants (CH(3)CHO and toluene) in air. The interesting physico-chemical properties and remarkable activity of MMnFh give great commercial potential in air purification application in diverse sectors.

9.
Chem Commun (Camb) ; 47(13): 3966-8, 2011 Apr 07.
Artigo em Inglês | MEDLINE | ID: mdl-21344096

RESUMO

An addition of rare earth metals with trivalent cation radii of 1.05-1.15 Å to Fe/BEA zeolites improves hydrothermal stability for selective catalytic reduction of NO by NH(3).


Assuntos
Metais Terras Raras/química , Óxidos de Nitrogênio/química , Zeolitas/química , Catálise , Troca Iônica , Oxirredução , Temperatura
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