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1.
This work describes the environmentally friendly technology for oxidation of ammonia (NH3) to form nitrogen at temperatures range from 423K to 673K by selective catalytic oxidation (SCO) over a nanosized Pt-Rh/γ-Al2O3 catalyst prepared by the incipient wetness impregnation method of hexachloroplatinic acid (H2PtCl6) and rhodium (III) nitrate (Rh(NO3)3) with γ-Al2O3 in a tubular fixed-bed flow quartz reactor (TFBR). The characterization of catalysts were thoroughly measured using transmission electron microscopy (TEM), threedimensional excitation-emission fluorescent matrix (EEFM) spectroscopy, UV-Vis absorption, dynamic lightscattering (DLS), zeta potential meter, and cyclic voltammetry (CV). The results demonstrated that at a temperature of 673K and an oxygen content of 4%, approximately 99% of the NH3 was removed by catalytic oxidation over the nanosized Pt-Rh/γ-Al2O3 catalyst. N2 was the main product in NH3-SCO process. Further, it reveals that the oxidation of NH3 was proceeds by the over-oxidation of NH3 into NO, which was conversely reacted with the NH3 to yield N2. Therefore, the application of nanosized Pt-Rh/γ-Al2O3 catalyst can significantly enhance the catalytic activity toward NH3 oxidation. One fluorescent peak for fresh catalyst was different with that of exhausted catalyst. It indicates that EEFM spectroscopy was proven to be an appropriate and effective method to characterize the Pt clusters in intrinsic emission from nanosized Pt-Rh/γ-Al2O3 catalyst. Results obtained from the CV may explain the significant catalytic activity of the catalysts.  相似文献   

2.
In this paper, factors influencing the mineralization of dimethyl phthalate (DMP) during catalytic ozonation with a cerium-doped Ru/Al2O3 catalyst were studied. The catalytic contribution was calculated through the results of a comparison experiment. It showed that doping cerium significantly enhanced catalytic activity. The total organic carbon (TOC) removal over the doped catalyst at 100 min reached 75.1%, 61.3% using Ru/Al2O3 catalyst and only 14.0% using ozone alone. Catalytic activity reached the maximum when 0.2% of ruthenium and 1.0% of cerium were simultaneously loaded onto Al2O3 support. Results of experiments on oxidation by ozone alone, adsorption of the catalyst, Ce ion’s and heterogeneous catalytic ozonation confirmed that the contribution of heterogeneous catalytic ozonation was about 50%, which showed the obvious effect of Ru-Ce/Al2O3 on catalytic activity.  相似文献   

3.
N2O is a powerful greenhouse gas and plays an important role in destructing the ozone layer. This present work investigated the effects of Pd doping on N2O formation over Pt/BaO/Al2O3 catalyst. Three types of catalysts, Pt/BaO/Al2O3, Pt/Pd mechanical mixing catalyst (Pt/BaO/Al2O3 + Pd/Al2O3) and Pt-Pd co-impregnation catalyst (Pt-Pd/BaO/Al2O3) were prepared by incipient wetness impregnation method. These catalysts were first evaluated in NSR activity tests using H2/CO as reductants and then carefully characterized by BET, CO chemisorption, CO-DRIFTs and H2-TPR techniques. In addition, temperature programmed reactions of NO with H2/CO were conducted to obtain further information about N2O formation mechanism. Compared with Pt/BaO/Al2O3, (Pt/BaO/ Al2O3 + Pd/Al2O3) produced less N2O and more NH3 during NO x storage and reduction process, while an opposite trend was found over (Pt-Pd/BaO/Al2O3 + Al2O3). Temperature programmed reactions of NO with H2/CO results showed that Pd/Al2O3 component in (Pt/BaO/Al2O3 + Pd/Al2O3) played an important role in NO reduction to NH3, and the formed NH3 could reduce NO x to N2 leading to a decrease in N2O formation. Most of N2O formed over (Pt-Pd/BaO/Al2O3 + Al2O3) was originated from Pd/BaO/Al2O3 component. H2-TPR results indicated Pd-Ba interaction resulted in more difficultto- reduce PdOx species over Pd/BaO/Al2O3, which inhibits the NO dissociation and thus drives the selectivity to N2O in NO reduction.
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4.
In this work, a catalytic membrane using Mn/Mo/Ru/Al2O3 as the catalyst was employed to remove elemental mercury (Hg0) from flue gas at low temperature. Compared with traditional catalytic oxidation (TCO) mode, Mn/Al2O3 membrane catalytic system had much higher removal efficiency of Hg0. After the incorporation of Mo and Ru, the production of Cl2 from the Deacon reaction and the retainability for oxidants over Mn/Al2O3 membrane were greatly enhanced. As a result, the oxidization of Hg0 over Mn/Al2O3 membrane was obviously promoted due to incorporation of Mo and Ru. In the presence of 8 ppmv HCl, the removal efficiency of Hg0 by Mn/Mo/Ru/Al2O3 membrane reached 95% at 423 K. The influence of NO and SO2 on Hg0 removal were insignificant even if 200 ppmv NO and 1000 ppmv SO2 were used. Moreover, compared with the TCO mode, the Mn/Mo/Ru/Al2O3 membrane catalytic system could remarkably reduce the demanded amount of oxidants for Hg0 removal. Therefore, the Mn/Mo/Ru/Al2O3 membrane catalytic system may be a promising technology for the control of Hg0 emission.  相似文献   

5.
Selective catalytic reduction of NO x by H2 in the presence of oxygen has been investigated over Pt/ Al2O3 catalysts pre-treated under different conditions. Catalyst preparation conditions exert significant influence on the catalytic performance, and the catalyst pre-treated by H2 or H2 then followed by O2 is much more active than that pre-treated by air. The higher surface area and the presence of metallic Pt over Pt/Al2O3 pre-treated by H2 or pretreated by H2 then followed by O2 can contribute to the formation of NO2, which then promotes the reaction to proceed at low temperatures.  相似文献   

6.
MnO2 microspheres with various surface structures were prepared using the hydrothermal method, and Au/MnO2 catalysts were synthesized using the sol-gel method. We obtained three MnO2 microspheres and Au/MnO2 samples: coherent solid spheres covered with wire-like nanostructures, solid spheres with nanosheets, and hierarchical hollow microspheres with nanoplatelets and nanorods. We investigated the properties and catalytic activities of formaldehyde oxidation at room temperature. Crystalline structures of MnO2 are the main factor affecting the catalytic activities of these samples, and γ-MnO2 shows high catalytic performance. The excellent redox properties are responsible for the catalytic ability of γ-MnO2. The gold-supported interaction can change the redox properties of catalysts and accelerate surface oxygen species transition, which can account for the catalytic activity enhancement of Au/MnO2. We also studied intermediate species. The dioxymethylene (DOM) and formate species formed on the catalyst surface were considered intermediates, and were ultimately transformed into hydrocarbonate and carbonate and then decomposed into CO2. A proposed mechanism of formaldehyde oxidation over Au/MnO2 catalysts was also obtained.  相似文献   

7.
A highly effective Ag-Al2O3 catalyst was prepared using the in-situ sol-gel method, and characterized by surface area using nitrogen adsorption, scanning electron microscopy (SEM), and transmission electron microscopy (TEM) techniques. The catalyst performance was tested on a real lean-burn gasoline engine. Only unburned hydrocarbons and carbon monoxide in the exhaust were directly used as reductant (without any external reductant), the maximum NO x conversion could only reach 40% at 450°C. When an external reductant, ethanol was added, the average NO x conversion was greater than 60%. At exhaust gas temperature range of 350–500°C, the maximum NO x conversion reached about 90%. CO and HC could be efficiently oxidized with Pt-Al2O3 oxidation catalyst placed at the end of SCR converter. However, NO x conversion drastically decreased because of the oxidation of some intermediates to NO x again. The possible reaction mechanism was proposed as two typical processes, nitration, and reduction in HC-SCR over Ag-Al2O3.  相似文献   

8.
Fe3O4 was supported on mesoporous Al2O3 or SiO2 (50 wt.%) using an incipient wetness impregnation method, and Fe3O4/Al2O3 exhibited higher catalytic efficiency for the degradation of 2,4-dichlorophenoxyacetic acid and para-chlorobenzoic acid aqueous solution with ozone. The effect and morphology of supported Fe3O4 on catalytic ozonation performance were investigated based on the characterization results of X-ray diffraction, X-ray photoelectron spectroscopy, BET analysis and Fourier transform infrared spectroscopy. The results indicated that the physical and chemical properties of the catalyst supports especially their Lewis acid sites had a significant influence on the catalytic activity. In comparison with SiO2, more Lewis acid sites existed on the surface of Al2O3, resulting in higher catalytic ozonation activity. During the reaction process, no significant Fe ions release was observed. Moreover, Fe3O4/Al2O3 exhibited stable structure and activity after successive cyclic experiments. The results indicated that the catalyst is a promising ozonation catalyst with magnetic separation in drinking water treatment.  相似文献   

9.
To decompose efficiently hydrogen cyanide (HCN) in exhaust gas, g-Al2O3-supported bimetallicbased Cu–Ni catalyst was prepared by incipient-wetness impregnation method. The effects of the calcination temperature, H2O/HCN volume ratio, reaction temperature, and the presence of CO or O2 on the HCN removal efficiency on the Cu–Ni/g-Al2O3 catalyst were investigated. To examine further the efficiency of HCN hydrolysis, degradation products were analyzed. The results indicate that the HCN removal efficiency increases and then decreases with increasing calcination temperature and H2O/HCN volume ratio. On catalyst calcined at 400°C, the efficiency reaches a maximum close to 99% at 480 min at a H2O/HCN volume ratio of 150. The HCN removal efficiency increases with increasing reaction temperature within the range of 100°C–500°C and reaches a maximum at 500°C. This trend may be attributed to the endothermicity of HCN hydrolysis; increasing the temperature favors HCN hydrolysis. However, the removal efficiencies increases very few at 500°C compared with that at 400°C. To conserve energy in industrial operations, 400°C is deemed as the optimal reaction temperature. The presence of CO facilitates HCN hydrolysis andincreases NH3 production. O2 substantially increases the HCN removal efficiency and NO x production but decreases NH3 production.
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10.
The kinetics of ferrate(VI) (FeVIO4 2−, Fe(VI)) oxidation of an antiphlogistic drug, ibuprofen (IBP), as a function of pH (7.75–9.10) and temperature (25–45°C) were investigated to see the applicability of Fe(VI) in removing this drug from water. The rates decrease with an increase in pH and the rates are related to protonation of ferrate(VI). The rates increase with an increase in temperature. The E a of the reaction at pH 9.10 was calculated as 65.4±6.4 kJ mol−1. The rate constant of the HFeO4 with ibuprofen is lower than with the sulphur drug, sulfamethoxazole. The use of Fe(VI) to remove ibuprofen is briefly discussed.  相似文献   

11.
The underlying physiological mechanisms explaining why the adult penaeid prawn Litopenaeus stylirostris cannot successfully face heavy stressful events on the low edge of its thermopreferendum (20–22°C) were studied during the austral winter. Prawns were studied during recovery from net fishing and rapid transfer from outdoor earthen ponds into indoor facilities. This was assimilated to a predator–prey interaction. O2-consumption, hemolymph osmotic pressure (OPh), arterial O2 partial pressure (PO2), a–v O2-capacitance and mortality rates were analysed. Data were compared to similar challenges performed at 28°C during the austral summer. At 20–22°C, mortality of up to 70% was observed after 2 days whereas at 28°C, maximum mortality was 3–5%. Mortality occurred when OPh shifted towards equilibrium with seawater, the resting O2-consumption, the a–v O2-capacitance and the arterial PO2 went down to minimal values. These events can be counterbalanced by transiently hyper-oxygenating the hemolymph or by blocking the OPh shift in isosmotic water (Wabete et al. in Aquaculture 260:181–193, 2006): both led to a dramatic decrease in mortality. It is concluded that in penaeid prawns L. stylirostris, a mismatch between O2-demand and O2-supply contributes to setting the geographical limits for this animal species through an impairment of their hemolymph O2-carrying capacity during heavy stressful events like chasing by predators.  相似文献   

12.
Al2O3, MgO, SiO2 and ZnO-supported nickel catalysts were prepared and evaluated in the ethanol steam reforming for hydrogen production. It is shown that the catalytic behavior can be influenced depending on the experimental conditions employed and chemical composition of the catalyst.  相似文献   

13.
Hematite (Fe2O3) chemical reduction into FeO and Fe3O4 by releasing O2 at high temperatures is considered one of the generally accepted mechanisms for processing waste minerals and clay into lightweight aggregate construction materials. In many case studies, this mechanism has not been strictly confirmed. To verify whether hematite can effectively release O2 at 1,000–1,260°C, a material containing hematite, simulating waste sediments from a Taiwanese reservoir, was shaped into pellets and fired into lightweight aggregates at high temperatures for 20 min and studied with various techniques. As revealed by the X-ray absorption near-edge structure technique, almost all the hematite remained as Fe(III) in the pellets when fired at 1,000–1,260°C, implying a negligible release of O2 leading to the creation of pores. This finding shows that the generally accepted mechanism for lightweight aggregate formation associated with hematite decomposition into FeO, Fe3O4, and O2 is invalid. Furthermore, Fe(III)-containing composites were formed in the fired pellets. Although firing at 1,000°C can trigger the decomposition of the components K2CO3, Na2CO3, and CaCO3 with a release of CO2, the sintering reaction was seemingly too weak to encapsulate the gases effectively. For pellets fired at 1,050–1,150°C, pores grew in size because the sintering reaction sufficed to generate a glassy phase that could better encapsulate gases.  相似文献   

14.
Microwave and Fenton's reagent oxidation of wastewater   总被引:16,自引:0,他引:16  
We compared two H2O2 oxidation methods for the treatment of industrial wastewater: oxidation using Fenton's reagent [H2O2/Fe(II)] and microwave irradiation. Both methods were applied to the treatment of synthetic phenol solutions (100 mg L−1) and of an industrial effluent containing a mixture of ionic and non-ionic surfactants at high load (20 g L−1 of COD). The effects of initial pH, initial H2O2 concentration, Fenton catalyst amount and irradiation time were assessed. According to the oxidation of phenol, it has been found that the oxidation by Fenton's reagent is dependent on the pH, contrary to the microwave system, which is not influenced by this parameter. For both systems, a limiting amount of oxidant has been found; above this point the oxidation of phenol is not improved by a further addition of peroxide. The oxidation of the industrial surfactant effluent has only been successful with the Fenton's reagent. In this case, large amounts of ferrous ions are necessary for the precipitation of the ionic surfactants of the effluent, followed by the oxidation of the non-ionic constituents of the solution. Electronic Publication  相似文献   

15.
The effect of Zr on the catalytic performance of Pd/y-A1203 for the methane combustion was investigated. The results show that the addition of Zr can improve the activity and stability of Pd/γ-Al2O3 catalyst, which, based on the catalyst characterization (N2 adsorption, XRD, CO- Chemisorption, XPS, CHa-TPR and O2-TPO), is ascribed to the interaction between Pd and Zr. The active phase of methane combustion over supported palladium catalyst is the Pd^0/Pd^2+ mixture. Zr addition inhibits Pd aggregation and enhances the redox properties of active phase Pd^0/ Pd^2+. H2 reduction could effectively reduce the oxidation degree of Pd species and regenerate the active sites (Pd^0/ pd^2+).  相似文献   

16.
The cytotoxicity of 13 and 22 nm aluminum oxide (Al2O3) nanoparticles was investigated in cultured human bronchoalveolar carcinoma-derived cells (A549) and compared with 20 nm CeO2 and 40 nm TiO2 nanoparticles as positive and negative control, respectively. Exposure to both Al2O3 nanoparticles for 24 h at 10 and 25 µg mL?1 doses significantly decreased cell viability compared with control. However, the cytotoxicity of 13 and 22 nm Al2O3 nanoparticles had no difference at 5–25 µg mL?1 dose range. The cytotoxicity of both Al2O3 nanoparticles were higher than negative control TiO2 nanoparticles but lower than positive control CeO2 nanoparticles (TiO2 < Al2O3 < CeO2). A real-time single cell imaging system was employed to study the cell membrane potential change caused by Al2O3 and CeO2 nanoparticles using a membrane potential sensitive fluorescent probe DiBAC4(3). Exposure to the 13 nm Al2O3 nanoparticles resulted in more significant depolarization than the 30 nm Al2O3 particles. On the other hand, the 20 nm CeO2 particles, the most toxic, caused less significant depolarization than both the 13 and 22 nm Al2O3. Factors such as exposure duration, surface chemistry, and other mechanisms may contribute differently between cytotoxicity and membrane depolarization.  相似文献   

17.
4A zeolite supported nanoparticulate zero-valent iron (nZVI/4A zeolite), synthesized through borohydride reduction method, was used as a catalyst with H2O2 to build Fenton-like reaction system to degrade methylene blue (MB) in model wastewater. The characteristics and primary mechanisms of the catalyst were investigated. The results show that nZVI/4A zeolite has the potential as a Fenton-like catalyst, and (about 30 mg/L) MB was degraded completely in 3 h with 10 mM H2O2, 0.2 g/L catalyst, and initial pH of 3.0. The MB degradation rates were obtained at least 70% in the tests with initial pH ranged from 2.0 to 9.0 and the catalyst dose rose from 0.2 to 5.0 g/L. Importantly, the catalyst also has a distinctive ability to increase the solution pH value from its initial acidic pH and then maintain the value at close to neutrality. This ability was controlled by both the initial pH and the catalyst dose. MB degradation clarified that hydroxyl radical was the dominated active oxidative specie in the tests with initial acidic pH and low catalyst dose (less 2.5 g/L); otherwise, Fe(VI) oxidation was the main mechanism for MB degradation; and the two processes shared synergistic effect in MB degradation in the present test. The catalyst has high operational stability in both of the composites with low iron leaching (less 2%) and catalyzing ability. Therefore, nZVI/4A zeolite has great potential as a Fenton-like catalyst and is used with H2O2 to build Fenton-like system which could be used to degrade MB efficiently.  相似文献   

18.
Respiration rates and elemental composition (carbon and nitrogen) were determined for four dominant oncaeid copepods (Triconia borealis, Triconia canadensis, Oncaea grossa and Oncaea parila) from 0–1,000 m depth in the western subarctic Pacific. Across the four species of which dry weight (DW) varied from 2.0 to 32 μg, respiration rates measured at in situ temperature (3°C) increased with DW, ranging from 0.84 to 7.4 nl O2 individual−1 h−1. Carbon (C) and nitrogen (N) composition of the four oncaeid species ranged from 49–57% of DW and 7.0–10.3% of DW, respectively, and the resultant C:N ratios were 4.8–8.3. The high C contents and C:N ratios were reflected by large accumulation of lipids in their body. Specific respiration rates (SR, a fraction of body C respired per day) ranged between 0.5 and 1.3% day−1. Respiration rates adjusted to a body size of 1 mg body N (i.e. adjusted metabolic rates, AMR) of the four oncaeid species [0.6–1.1 μl O2 (mg body N)−0.8 h−1 at 3°C] were significantly lower than those (1.7–5.1) reported in the literature for oithonid and calanoid copepods at the same temperature. The present results indicate that lower metabolic expenditure due to less active swimming (pseudopelagic life mode) together with rich energy reserve in the body (as lipids) are the characters of oncaeid copepods inhabiting in the epi- and mesopelagic zones of this region.  相似文献   

19.
 Short-term effects of temperature and irradiance on oxygenic photosynthesis and O2 consumption in a hypersaline cyanobacterial mat were investigated with O2 microsensors in a laboratory. The effect of temperature on O2 fluxes across the mat–water interface was studied in the dark and at a saturating high surface irradiance (2162 μmol photons m−2 s−1) in the temperature range from 15 to 45 °C. Areal rates of dark O2 consumption increased almost linearly with temperature. The apparent activation energy of 18 kJ mol−1 and the corresponding Q 10 value (25 to 35 °C) of 1.3 indicated a relative low temperature dependence of dark O2 consumption due to mass transfer limitations imposed by the diffusive boundary layer at all temperatures. Areal rates of net photosynthesis increased with temperature up to 40 °C and exhibited a Q 10 value (20 to 30 °C) of 2.8. Both O2 dynamics and rates of gross photosynthesis at the mat surface increased with temperature up to 40 °C, with the most pronounced increase of gross photosynthesis at the mat surface between 25 and 35 °C (Q 10 of 3.1). In another mat sample, measurements at increasing surface irradiances (0 to 2319 μmol photons m−2 s−1) were performed at 25, 33 (the in situ temperature) and 40 °C. At all temperatures, areal rates of gross photosynthesis saturated with no significant reduction due to photoinhibition at high irradiances. The initial slope and the onset of saturation (E k = 148 to 185 μmol photons m−2 s−1) estimated from P versus E d curves showed no clear trend with temperature, while maximal photosynthesis increased with temperature. Gross photosynthesis was stimulated by temperature at each irradiance except at the lowest irradiance of 54 μmol photons m−2 s−1, where oxygenic gross photosynthesis and also the thickness of the photic zone was significantly reduced at 40 °C. The compensation irradiance increased with temperature, from 32 μmol photons m−2 s−1 at 25 °C to 77 μmol photons m−2 s−1 at 40 °C, due to increased rates of O2 consumption relative to gross photosynthesis. Areal rates of O2 consumption in the illuminated mat were higher than dark O2 consumption at corresponding temperatures, due to an increasing O2 consumption in the photic zone with increasing irradiance. Both light and temperature enhanced the internal O2 cycling within hypersaline cyanobacterial mats. Received: 30 November 1999 / Accepted: 11 April 2000  相似文献   

20.
In this study, post plasma-catalysis degradation of mixed volatile organic compounds (benzene, toluene, and xylene) has been performed in a hybrid surface/packed-bed discharge plasma reactor with Ag-Ce/g-Al2O3 catalyst at room temperature. The effect of relative air humidity on mixed VOCs degradation has also been investigated in both plasma-only and PPC systems. In comparison to the plasma-only system, a significant improvement can be observed in the degradation performance of mixed VOCs in PPC system with Ag-Ce/γ-Al2O3 catalyst. In PPC system, 68% benzene, 89% toluene, and 94% xylene were degraded at 800 J·L–1, respectively, which were 25%, 11%, and 9% higher than those in plasma-only system. This result can be attributed to the high catalytic activity of Ag-Ce/γ-Al2O3 catalyst to effectively decompose O3 and lead to generating more reactive species which are capable of destructing the VOCs molecules completely. Moreover, the presence of Ag-Ce/γ-Al2O3 catalyst in plasma significantly decreased the emission of discharge byproducts (NOx and O3) and promoted the mineralization of mixed VOCs towards CO2. Adding a small amount of water vapor into PPC system enhanced the degradation efficiencies of mixed VOCs, however, further increasing water vapor had a negative impact on the degradation efficiencies, which was primarily attributed to the quenching of energetic electrons by water vapor in plasma and the competitive adsorption of water vapor on the catalyst surface. Meanwhile, the catalysts before and after discharge were characterized by the Brunauer-Emment-Teller and X-ray photoelectron spectroscopy.
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