41 research outputs found
Fabrication and catalytic activity of thermally stable gold nanoparticles on ultrastable Y (USY) zeolites
Au was deposited on ultrastable Y (USY) zeolites using an ion-exchange method. Up to 5.5 wt% Au was introduced into the NH4-form of USY zeolites. In contrast, deposition of Au hardly took place on the H- and Na-forms of Y-type zeolites, NH4-forms of mordenite, and ZSM-5. Treatment of the Au-loaded USY zeolite in a H2 atmosphere, afforded Au0 nanoparticles. These particles were thermally stable even at 973 K, where their mean particle diameter was 3.7 nm. In contrast, highly aggregated Au particles were observed after thermal treatment at temperatures lower than 523 K, followed by storage in air for a month. The resulting particle sizes were in good correlation with the IR band intensity of the adsorbed CO and the catalytic activity of Au in the aerobic oxidation of benzyl alcohol. The Au nanoparticles showed highest activity when the Au/USY zeolite was thermally treated at 673–973 K. A negligible deactivation was observed after repeating the reaction at least 12 times. In the case of Au/TiO2 catalyst prepared by the deposition-precipitation method, the highest activity was observed at 573 K, which was lower than the temperature used for the Au/USY zeolites. This study demonstrated the potential use of the NH4-form of USY zeolites for supporting Au
Catalytic performance and QXAFS analysis of Ni catalysts modified with Pd for oxidative steam reforming of methane
Pd–Ni bimetallic catalysts prepared by co-impregnation and sequential impregnation methods were compared in the catalytic performance in oxidative steam reforming of methane. The sequential impregnation was more effective to the suppression of hot spot formation. According to the structural analysis by in situ quick-scanning X-ray absorption fine structure (QXAFS) during the temperature programmed reduction, the sequential impregnation method gave the bimetallic particles with higher Pd surface composition because of the low possibility of the Pd–Ni bond formation. Higher surface composition of Pd with higher reducibility than Ni is connected to the enhancement of the catalyst reducibility and the suppression of the hot spot formation
Assignments of Bending Vibrations of Ammonia Adsorbed on Solid Surfaces
Bending vibrations in the infrared (IR) spectra of ammonia adsorbed on Lewis acidic metal oxides, i.e., Al2O3, ZrO2 and TiO2, and zeolite were analyzed with an aid of density functional theory (DFT) calculations. The results by DFT methods reveal the wavenumbers of the vibration modes (ν4 and ν2) of NH4 bonded to Brønsted acid site and the vibration modes (δs and δd) of NH3 species coordinated to a Lewis acidic metal center (M = Al, Zr or Ti). The wavenumbers calculated based on DFT were reasonably in agreement with the experimentally observed values. The estimation of wavenumbers suggests that the δs vibration of NH3 hydrogen-bonded is invisible on a zeolite, because it is hidden by an intense absorption due to skeletal vibration. On the other hand, multiple bands of asymmetric bending modes (δd and ν2) observed on a zeolite were assigned. A quantification method of Brønsted and Lewis acid sites, and hydrogen-bonded NH3 is provided based on the peak assignments
Immunomodulating Activity of Agaricus brasiliensis KA21 in Mice and in Human Volunteers
We performed studies on murine models and human volunteers to examine the immunoenhancing effects of the naturally outdoor-cultivated fruit body of Agaricus brasiliensis KA21 (i.e. Agaricus blazei). Antitumor, leukocyte-enhancing, hepatopathy-alleviating and endotoxin shock-alleviating effects were found in mice. In the human study, percentage body fat, percentage visceral fat, blood cholesterol level and blood glucose level were decreased, and natural killer cell activity was increased. Taken together, the results strongly suggest that the A. brasiliensis fruit body is useful as a health-promoting food
Enhancement in the Catalytic Activity of Pd/USY in the Heck Reaction Induced by H2 Bubbling
Pd was loaded on ultra stable Y (USY) zeolites prepared by steaming NH4-Y zeolite under different conditions. Heck reactions were carried out over the prepared Pd/USY. We found that H2 bubbling was effective in improving not only the catalytic activity of Pd/USY, but also that of other supported Pd catalysts and Pd(OAc)2. Moreover, the catalytic activity of Pd/USY could be optimized by choosing appropriate steaming conditions for the preparation of the USY zeolites; Pd loaded on USY prepared at 873 K with 100% H2O gave the highest activity (TOF = 61,000 h−1), which was higher than that of Pd loaded on other kinds of supports. The prepared Pd/USY catalysts were applicable to the Heck reactions using various kinds of substrates including bromo- and chloro-substituted aromatic and heteroaromatic compounds. Characterization of the acid properties of the USY zeolites revealed that the strong acid site (OHstrong) generated as a result of steaming had a profound effect on the catalytic activity of Pd
Regulation of the Dispersion of PdO through the Interaction with Acid Sites of Zeolite Studied by Extended X-ray Absorption Fine Structure
Characterization and Design of Zeolite Catalysts: Solid Acidity, Shape Selectivity and Loading Properties
Zeolites are microporous, aluminosilicate minerals commonly used as commercial adsorbents. Zeolite-based catalysts are used by industrial chemical companies in the interconversion of hydrocarbons and the alkylation of aromatic compounds. The current book deals with the characterization of specific properties of Zeolites and calculations for the design of catalysts. Measurements and utilization of solid acidity, shape selectivity, and loading properties, that are three prominent properties of a Zeolite catalyst, are treated in detail. These features concern chemical vapor deposition of silica, shape selectivity, loading properties, solid activity, Brønsted or Lewis character, ammonia temperature programmed desorption, control of the pore-opening size by chemical vapor deposition of silica and XAFS analysis of metals being highly dispersed inside and outside a framework