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101.
102.
A self-assembled monolayer (SAM) of a novel cobalt(II)porphyrin disulphide derivative was prepared on flat gold(1 1 1) electrode. Evidence for surface modification was provided by electrochemical reductive desorption of the monolayer and ellipsometry, consistent with a coverage of 2.5 × 10−10 mol cm−2 and a thickness of 13 Å, respectively. Both results support the presence of SAMs where the molecules share an intermediate position between perpendicular and flat orientation. Scanning tunnelling microscopy have also proven the formation of CoPSS SAMs, however high-resolution images could only be obtained when the CoPSS molecules were diluted in an hexanethiol SAM. The electrocatalytic activity of the surface confined Co-porphyrin was evaluated for the oxygen reduction. Voltammetric data indicate that reaction involves two electrons consistent with the formation of hydrogen peroxide. Under similar experimental conditions the data obtained for an iron-porphyrin analogue points for a full reduction of dioxygen to water. 相似文献
103.
Arman Bonakdarpour George D. Vernstrom Alison K. Schmoeckel Jeff R. Dahn 《Electrochimica acta》2007,53(2):688-694
We report on extensive measurements of oxygen reduction activity of Pt and Pt-Co-Mn electrocatalysts using the rotating ring-disk electrode (RRDE) method. The electrocatalysts were prepared by sputtering from Pt or Pt, Co and Mn targets onto 3M's nano-structured thin film support (NSTF) structures. The area specific activity of Pt/NSTF, measured in 0.1 M HClO4 and at room temperature, is similar to that of bulk Pt. The area specific measurements show a 20 mV reduction in the Pt-Co-Mn/NSTF overpotential compared to Pt/NSTF. The corresponding kinetic gain in the area specific activity of the ternary alloy is about a factor of two. This ORR enhancement factor observed in the ternary Pt-Co-Mn/NSTF by RRDE measurements is similar to the results obtained in 50 cm2 H2/air fuel cells. 相似文献
104.
Direct nitric oxide decomposition over perovskites is fairly slow and complex, its mechanism changing dramatically with temperature. Previous kinetic study for three representative compositions (La0.87Sr0.13Mn0.2Ni0.8O3−δ, La0.66Sr0.34Ni0.3Co0.7O3−δ and La0.8Sr0.2Cu0.15Fe0.85O3−δ) has shown that depending on the temperature range, the inhibition effect of oxygen either increases or decreases with temperature. This paper deals with the effect of CO2, H2O and CH4 on the nitric oxide decomposition over the same perovskites studied at a steady-state in a plug-flow reactor with 1 g catalyst and total flowrates of 50 or 100 ml/min of 2 or 5% NO. The effect of carbon dioxide (0.5–10%) was evaluated between 873 and 923 K, whereas that of H2O vapor (1.6 or 2.5%) from 723 to 923 K. Both CO2 and H2O inhibit the NO decomposition, but inhibition by CO2 is considerably stronger. For all three catalysts, these effects increase with temperature. Kinetic parameters for the inhibiting effects of CO2 and H2O over the three perovskites were determined. Addition of methane to the feed (NO/CH4=4) increases conversion of NO to N2 about two to four times, depending on the initial NO concentration and on temperature. This, however, is still much too low for practical applications. Furthermore, the rates of methane oxidation by nitric oxide over perovskites are substantially slower than those of methane oxidation by oxygen. Thus, perovskites do not seem to be suitable for catalytic selective NO reduction with methane. 相似文献
105.
High surface area Mn-based porous oxides (MANPO) containing additives like Ce, Sr and La were found to be very active and selective materials under 0.67% CH4/0.2% NO/5% O2 lean-deNO
x
conditions in the 200–300°C low-temperature range. These materials perform also impressively in the presence of 4% H2O in the feed stream, where a N2 selectivity of 98% and an excellent stability over 24 h on stream have been observed. The MANPO materials can be considered serious competitors of noble metals for low-temperature lean-deNO
x
applications. 相似文献
106.
Controlled calcination of ion-exchanged Wyoming Bentonite in the presence and absence of ammonia leads to layer charge reductions. Detailed chemical analyses of both unexchangeable and exchangeable species lead to the conclusion that in no case is there migration of the original interlamellar cations into the octahedral region of the layers although, in terms of ionic radius alone, Mg2+, Ni2+ and, possibly Co2+, might be expected to do so. The production of unexchangeable Mg, Ni or Co, is identified as resulting from high temperature hydrolysis leading to hydroxide or oxide formation. 相似文献
107.
108.
109.
Masaru Takahashi Tetsu Nakatani Shinji Iwamoto Tsunenori Watanabe Masashi Inoue 《Applied catalysis. B, Environmental》2007,70(1-4):73-79
The solvothermal reaction of mixtures of aluminum isopropoxide (AIP) and gallium acetylacetonate (Ga(acac)3) directly yielded the mixed oxides of γ-Ga2O3-Al2O3. In the solvothermal synthesis, the crystal structure of mixed oxides was controlled by the initial formation of γ-Ga2O3 nuclei. The mixed oxides prepared in diethylenetriamine have extremely high activities for selective catalytic reduction (SCR) of NO with methane as a reducing agent. With increasing crystallite size of the spinel structure, the catalytic activity increased. The ratio of the amount of methane consumed by combustion to total methane conversion was proportional to the density of acid sites on the surface of the mixed oxides. The mixed oxide catalysts prepared in diethylenetriamine had lower densities of acid sites and showed a higher methane-efficiency for CH4-SCR than those prepared in other solvents. These catalysts maintained their high activity even when the reaction was carried out under the severe conditions (i.e., high space velocity and low NO concentration). 相似文献
110.