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91.
The absorption of oxygen and styrene in water-silicone oil emulsions was independently studied in laboratory-scale bubble reactors at a constant gas flow rate for the whole range of emulsion compositions (0-10% v/v). The volumetric mass transfer coefficients to the emulsions were experimentally measured using a dynamic absorption method. It was assumed that the gas phase contacts preferentially the water phase. In the case of oxygen absorption, it was found that the addition of silicone oil hinders oxygen mass transfer compared to an air-water system. Decreases in kLaoxygen of up to 25% were noted. Such decreases in the oxygen mass transfer coefficient, which imply longer aeration times to transfer oxygen, could represent a limiting step in biotechnological processes strongly dependent on oxygen concentration. Nevertheless, as the large affinity of silicone oil for oxygen enables greater amounts of oxygen to be transferred from the gas phase, it appears that the addition of more than 5% silicone oil should be beneficial to increase the oxygen transfer rate. In the case of styrene absorption, it was established that the volumetric mass transfer coefficient based on the emulsion volume is roughly constant with the increase in the emulsion composition. In spite of the relatively high cost of silicone oil, water-silicone oil emulsions remain relevant to treat low-solubility volatile organic compounds, such as styrene, in low-concentration gas streams. 相似文献
92.
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
93.
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
94.
Horizontal pipeline and tubular loop aerators are of interest for fermentation and waste water treatment and are ideally suited for continuous processing. A major drawback is that these pipeline contactors invariably operate in the “elongated bubble and plug” regime in which the mass transfer rate is low. This article evaluates the performance of a horizontal pipeline aerator fitted with nozzles equispaced along its length to enhance mass transfer rates by promoting turbulence and augmenting effective interfacial area. Such devices can also be advantageously used in long pipe lines as in the case of treating waste while it is being transported. Pressure drop and overall liquid-side mass transfer coefficient data are reported as functions of liquid (water) and gas flow rates and nozzle size and spacing. It is shown that for all the conditions studied, kLa = 0.026(ΔP/L)1.036 and that the pressure gradient is given by a simple correlation, provided an empirical parameter which characterises a nozzle is known. Preliminary investigations on the effect of surfactant ad the presence of suspended solids (size 75 μm) on mass transfer coefficient are also reported. Very high values of power dissipation can be achieved in such aerators without mechanically moving parts and high values of mass transfer coefficient can be realized. 相似文献
95.
The generation of oxygen gas within an amorphous anodic alumina film is reported. The film was formed by anodizing aluminum, which was first electropolished and then chemically polished in CrO3-H3PO4 solution, in sodium tungstate electrolyte. The procedure results in incorporation of mobile Cr3+ species, from the chemical polishing film, and mobile W6+ species, from the electrolyte, into the amorphous structure. The tungsten species are present in the outer 27% of the film thickness, while Cr6+ species occupy a thin layer within the tungsten-containing region. Above the Cr3+ containing layer, a band develops that contains oxygen bubbles of a few nanometres size. The oxygen is generated by oxidation of O2− ions of the alumina. A mechanism of oxygen generation within the alumina is proposed based on the electronic band structure of the oxide, modified by the Cr3+ and W6+ species, and on the ionic transport processes during oxide growth. 相似文献
96.
Preparation of anodes for oxygen evolution in seawater electrolysis was carried out. Manganese-molybdenum double oxides, Mn1−xMoxO2+x, prepared by anodic deposition from MnSO4-Na2MoO4 solutions showed the 100% oxygen evolution efficiency at a current density of 1000 A m−2 in 0.5 M NaCl at 30 °C and pH 12, but an increase in solution temperature resulted in dissolution of the oxides as molybdate and permanganate ions. In order to increase the stability of the electrodes at higher temperatures the addition of iron to the manganese-molybdenum oxides was performed by anodic deposition in MnSO4-Na2MoO4-FeNH4(SO4)2 solutions. The electrodes thus prepared showed the 100% oxygen evolution efficiency at 1000 A m−2 in 0.5 M NaCl at 30-90 °C, when proper amounts of molybdenum and iron were contained. The iron addition also enhanced the oxygen evolution efficiency. The electrodes were not composed of oxide mixtures but triple oxides, Mn1−x−yMoxFeyO2+x−0.5y, consisting of Mn4+, Mo6+ and Fe3+. The formation of the triple oxides seemed responsible for enhancement of both oxygen evolution efficiency and stability. 相似文献
97.
The oxidation and reforming kinetics of methane by O2, CO2 and H2O were studied on a stepped Pt(5 5 7) single crystal from 623 to 1050 K under methane rich conditions. The rate of carbon deposition was followed by ex-situ Auger electron spectroscopy under non-oxidative conditions. The apparent activation energy for methane decomposition was significantly lower than the apparent barriers measured for both total oxidation, CO2 and H2O reforming. Total oxidation of methane to CO2 and H2O followed by combined dry and steam reforming (combined combustion-reforming) led to CO production rates which were higher than direct CO2 or H2O reforming rates. The enhanced rates are most likely due to the ability of adsorbed oxygen to prevent carbon nucleation and/or scavenge carbon enabling the reforming reaction to turnover on a larger fraction of sites. Comparable amounts of carbon were found by Auger electron spectroscopy measurements after both direct dry or steam reforming, while combined oxidation-reforming had considerable less carbon. During direct dry or steam reforming, CO2 and H2O serve only to scavenge adsorbed atomic carbon, while in the presence of oxygen, carbon is removed by both combustion and reforming routes. 相似文献
98.
Yuhao Lu 《Electrochimica acta》2007,52(7):2562-2569
The electrochemical behavior of cobalt phthalocyanine/platinum as methanol-resistant oxygen-reduction electrocatalyst for DMFC was investigated. Platinum was chemically deposited on the carbon-supported cobalt phthalocyanine (CoPc), and then it was heat-treated in high purity nitrogen at 300 °C, 635 °C and 980 °C. In order to evaluate the electrocatalytic behavior of CoPc-Pt/C, the PtCo/C and Pt/C as reference catalysts were employed. TGA, XRD, EDAX, XPS and electrochemical experiments were used to study the thermal stability, crystal structure, physical characterization and electrochemical behavior of these catalysts. These catalysts exhibited similar electrocatalytic activity for oxygen reaction in 0.5 M H2SO4 solution. In methanol tolerance experiments, Pt/C, PtCo/C and CoPc-Pt/C heated at 980 °C were active for the methanol oxidation reaction (MOR). The presence of Co did not improve resistance to methanol poisoning. However, the CoPc-Pt/C after 300 °C or 635 °C heat-treatment demonstrated significant inactivity for MOR, hence they have a good ability to resist methanol poisoning. The current study indicated that the macrocyclic structure of phthalocyanine is the most important factor to improve the methanol tolerance of CoPc-Pt/C as the oxygen-reduction reaction (ORR) electrocatalyst. The CoPc-Pt based catalyst should be a good alternation for oxygen electro-reduction reaction in DMFC. 相似文献
99.
Free acids of the iron substituted heteropoly acids (HPA), H7[(P2W17O61)FeIII(H2O)] (HFe1) and H18[(P2W15O56)2FeIII2(H2O)2] (HFe2) were prepared from the salts K7[(P2W17O61)FeIII(H2O)] (KFe1) and Na12[(P2W15O56)2FeIII4(H2O)2] (NaFe4), respectively. The iron-substituted HPA were adsorbed on to XC-72 carbon based GDLs to form HPA doped GDEs after water washing with HPA loadings of ca. 1 μmol. The HPA was detected throughout the GDL by EDX. Solution electrochemistry of the free acids are reported for the first time in sulfate buffer, pH 1-3. The hydrogen oxidation reaction was catalyzed by KFe1 at 0.33 V, with an exchange current density of 38 mA/cm2. Moderate activity for the oxygen reduction reaction was observed for the iron substituted HPA, which was dramatically improved by selectively removing oxygen atoms from the HPA by cycling the fuel cell cathode under N2 followed by reoxidation to give a restructured oxide catalyst. The nanostructured oxide achieved an OCV of 0.7 V with a Tafel slope of 115 mV/decade. Cycling the same catalysts in oxygen resulted in an improved catalyst/ionomer/carbon configuration with a slightly higher Tafel slope, 128 mV/decade but a respectable current density of 100 mA/cm2 at 0.2 V. 相似文献
100.
A series of compounds La2Mo2−xWxO9 (x = 0-2) were synthesized using a freeze-dried precursor method at relatively low temperatures (673-823 K). These materials were characterised by thermogravimetric and differential thermal analysis (TG/DTA), differential scanning calorimetric (DSC), X-ray diffraction (XRD), and transmission electron microscopy (TEM) and dilatometric measurements. Oxygen stoichiometry was evaluated by coulometric titration and thermogravimetric analysis at 873-1273 K. The ionic and electronic conductivities of these materials were analysed by impedance spectroscopy and a Hebb-Wagner ion-blocking method under moderately reducing conditions. The presence of W6+ leads to an increase of the stability range (about 10−16 Pa for La2Mo0.5W1.5O9 at 1073 K) and prevents oxygen loss and amorphisation. Within the stability range, the electronic conductivity increases gradually as the temperature increases and as the oxygen partial pressure reduces. This indicates that the electronic transport is mainly n-type as a result of the oxygen-content decreasing in the molybdate lattice. Further reduction of the oxygen partial pressure gave rise to the decomposition of La2Mo2−xWxO9, leading to the formation of new phases with molybdenum in lower oxidation states, which further enhances the electronic conductivity. The results of the coulometric titration and the thermogravimetric studies under a dry 5% H2/Ar flow suggest that tungsten doped lanthanum molybdate materials can be used as electrolyte only at low temperature and under moderate reducing conditions. 相似文献