Tomoyuki Kayama

Nanostructured Ceria-Silver Synthesized in a One-Pot Redox Reaction Catalyzes Carbon Oxidation

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.

Quantitative analysis of transient surface reactions on planar catalyst with time-resolved time-of-flight mass spectrometry.

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.