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1.
The objective of this study was to prepare a new photocatalyst with high activities for degradation of organic pollutants. Coupled ZrO2/ZnO photocatalyst was prepared with a simple precipitation method with cheap raw materials zinc acetate and zirconium oxychloride, and was characterized by X-ray diffraction (XRD) and transmission electron microscopy (TEM). Reactive brilliant red X-3B was used as a model compound to investigate the photocatalytic activity of synthesized catalysts in water under 254 nm UV irradiation. Results show that the optimal calcination temperature and coupling molar ratio of Zr were 350°C And 2.5%, respectively. At the calcination temperature of 350°C, ZrO2 was dispersed on the surface of hexagonal ZnO in the form of amorphous clusters. The particle size of ZrO2/ZnO decreased with the decrease of calcination temperature and the increase of Zr coupling amount. ZrO2/ZnO has better photocatalytic activity for degradation of reactive brilliant red (RBR) X-3B than pure ZnO and P25-TiO2.  相似文献   

2.
• Cu0.15-ACF performs the best for H2S and PH3 simultaneous removal. • 550°C and 90°C are separately calcination and reaction temperatures. • The reason why Cu0.15/ACF shows better performance was found. • The accumulation of H2PO4 and SO42−(H2O)6 is the deactivation cause of Cu0.15/ACF. Poisonous gases, such as H2S and PH3, produced by industrial production harm humans and damage the environment. In this study, H2S and PH3 were simultaneously removed at low temperature by modified activated carbon fiber (ACF) catalysts. We have considered the active metal type, content, precursor, calcination, and reaction temperature. Experimental results exhibited that ACF could best perform by loading 15% Cu from nitrate. The optimized calcination temperature and reaction temperature separately were 550°C and 90°C. Under these conditions, the most removal capacity could reach 69.7 mg/g and 132.1 mg/g, respectively. Characterization results showed that moderate calcination temperature (550°C) is suitable for the formation of the copper element on the surface of ACF, lower or higher temperature will generate more cuprous oxide. Although both can exhibit catalytic activity, the role of the copper element is significantly greater. Due to the exceptional dispersibility of copper (oxide), the ACF can still maintain the advantages of larger specific surface area and pore volume after loading copper, which is the main reason for better performance of related catalysts. Finally, increasing the copper loading amount can significantly increase the crystallinity and particle size of copper (oxide) on the ACF, thereby improving its catalytic performance. In situ IR found that the reason for the deactivation of the catalyst should be the accumulation of generated H2PO4 and SO42−(H2O)6 which could poison the catalyst.  相似文献   

3.
In this work, xylene removal from waste gas streams was investigated via catalytic oxidation over Pd/carbon-zeolite and Pd/carbon-CeO2 nanocatalysts. Activated carbon was obtained from pine cone chemically activated using ZnCl2 and modified by H3PO4. Natural zeolite of clinoptilolite was modified by acid treatment with HCl, while nano-ceria was synthesized via redox method. Mixed supports of carbon-zeolite and carbonceria were prepared and palladium was dispersed over them via impregnation method. The prepared samples were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), Brunauer-Emmett-Teller surface area (BET), Fourier transform infrared spectroscopy (FTIR) and thermogravimetric (TG) techniques. Characterization of nanocatalysts revealed a good morphology with an average particle size in a nano range, and confirmed the formation of nano-ceria with an average crystallite size below 60 nm. BET analysis indicated a considerable surface area for catalysts (~1000 m2·g?1). FTIR patterns demonstrated that the surface groups of synthesized catalysts are in good agreement with the patterns of materials applied in catalyst synthesis. The performance of catalysts was assessed in a low-pressure catalytic oxidation pilot in the temperature range of 100° C-250°C. According to the reaction data, the synthesized catalysts have been shown to be so advantageous in the removal of volatile organic compounds (VOCs), representing high catalytic performance of 98% for the abatement of xylene at 250°C. Furthermore, a reaction network is proposed for catalytic oxidation of xylene over nanocatalysts.  相似文献   

4.
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   

5.
ZrO2掺杂的V2O5/TiO2催化剂表征及催化还原NOx   总被引:1,自引:0,他引:1  
采用共沉淀法制备出不同锆掺杂量的钛锆复合载体(TiO2-ZrO2),运用XRD和BET研究其微观结构,结果显示钛锆物质的量之比1∶1时复合载体具有最大的比表面积,可达256.01 m.2g-1.以此为载体制备了V2O5/TiO2-ZrO2催化剂,并添加少量CeO2对其改性.采用XRD、BET、H2-TPR、原位FT-IR等手段研究其活性组分的表面分散状态、氧化还原特性和表面酸性.结果显示,V2O5高度分散在载体上;与纯V2O5相比,复合载体上V2O5的还原峰向低温方向发生了偏移;催化剂表面包含了大量的B酸和L酸.模拟氨气催化还原NO(NH3-SCR)的脱硝反应活性测试表明,V2O5/TiO2-ZrO2催化剂具有较好的热稳定性和较宽的活性窗口,少量CeO2的加入提高了催化剂的低温活性.  相似文献   

6.
 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   

7.
On the eastern shore of Nova Scotia late summer atmospheric systems cause upwelling of shelf water; the associated temperature variations of 10 °C with a 6 to 8 d period are comparable in magnitude to the seasonal variation. A laboratory study was undertaken to assess the effects of these temperature fluctuations on sea scallop (Placopecten magellanicus) growth and metabolism. In a factorial design, scallops were subjected to constant (10 °C) or a variable (6 to 15 °C) 8 d temperature cycle, and either a low (seston in filtered seawater) or high (seston supplemented with cultured phytoplankton) food diet. During the 48 d experiment scallop mortality was low and growth positive in all treatments. Shell and total tissue growth rate did not differ between temperature treatments, but growth in the high food treatments was 40 to 50% higher than in the low food treatments. However, soft tissue (excluding adductor) growth did show a temperature treatment effect; growth rates were significantly higher in the fluctuating temperature treatment, due in part to greater gonad development. Weight-standardized rates of scallop oxygen consumption (V sO2 , μmol O2 g−1 h−1) were 20 to 25% higher in high food than in low food treatments, consistent with the expected increase in respiration due to the higher growth rates. Scallop metabolism did not acclimate to the fluctuating temperature cycle; V sO2 and ammonium excretion (V sNH+ 4, μmol O2 g−1 h−1) remained dependent on ambient temperature throughout the experiment. V sNH+ 4 Q10 (2.77) was higher than V sO2 Q10 (2.01) which was reflected in a decrease in the O:N ratio at 15 °C, indicating a shift toward increased protein catabolism and a stressed state. At 10 °C, V sO2 and V sNH+ 4 in the variable temperature treatments were 15 to 18% lower than in the constant temperature treatments, a difference that was not detected in growth measurements. Results demonstrate that the metabolism of Placopecten magellanicus, unlike some bivalve species, is tightly coupled to fluctuations in ambient temperature. Although an absence of compensatory acclimation had a minimal effect on growth in this study, if high temperatures were combined with low food conditions a reduction in scallop production could result. Received: 23 June 1998 / Accepted: 8 February 1999  相似文献   

8.
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.
  相似文献   

9.
● A series of Cu-ZSM-5 catalysts were tested for DMF selective catalytic oxidation. ● Cu-6 nm samples showed the best catalytic activity and N2 selectivity. ● Redox properties and chemisorbed oxygen impact on DMF catalytic oxidation. ● Isolated Cu2+ species and weak acidity have effects on the generation of N2. N, N-Dimethylformamide (DMF), a nitrogen-containing volatile organic compound (NVOC) with high emissions from the spray industry, has attracted increasing attention. In this study, Cu-ZSM-5 catalysts with different CuO particle sizes of 3, 6, 9 and 12 nm were synthesized and tested for DMF selective catalytic oxidation. The crystal structure and physicochemical properties of the catalyst were studied by various characterization methods. The catalytic activity increases with increasing CuO particle size, and complete conversion can be achieved at 300–350 °C. The Cu-12 nm catalyst has the highest catalytic activity and can achieve complete conversion at 300 °C. The Cu-6 nm sample has the highest N2 selectivity at lower temperatures, reaching 95% at 300 °C. The activity of the catalysts is determined by the surface CuO cluster species, the bulk CuO species and the chemisorbed surface oxygen species. The high N2 selectivity of the catalyst is attributed to the ratio of isolated Cu2+ and bulk CuO species, and weak acidity is beneficial to the formation of N2. The results in this work will provide a new design of NVOC catalytic oxidation catalysts.  相似文献   

10.
The aim of the plesent investigation was to study the effect of SiO2 addition on the thermal deactivation of V2O5/WO3/TiO2 catalysts used for NOx pollution abatement. The results suggest that the degradation of the catalytic properties is strongly correlated to the structural ageing which is, in turn, mainly related to the anatase–rutile phase transformation and to the WO3 phase segregation. The addition of SiO2 strongly influences the temperature at which these phenomena occur. In fact, it was found that the introduction of this oxide stabilizes the material, retarding the collapse of surface area, and increases the temperature of the anatase to rutile phase transition.  相似文献   

11.
The Au/Al2O3 and Au–Rh/Al2O3 catalysts were prepared by deposition–precipitation. The promotional effect of Rh on the performance of the Au/Al2O3 catalyst for CO oxidation was studied. The results indicate that using Au/Al2O3 catalyst, CO can be completely oxidized at 0°C or much lower temperature but the catalyst deactivated very fast. Rh can improve the stability of Au/Al2O3 catalyst more than 10 times, which gives an important hint to develop high stable catalyst for CO oxidation at low temperature.  相似文献   

12.
V2O5/AC催化剂对氨还原NO的研究   总被引:16,自引:0,他引:16  
考察了V2O5/AC催化剂对NH3选择催化还原NO的影响,结果表明,以浓硝酸预氧化处理的活性焦为载体对催化剂活性有很大提高,这是由于浓硝酸预氧化后,活性焦表面产生了较多的含氧官能团可能吸附更多的NH3,并且提高了活性组分V2O5的含量,反应气氛中加入SO2后,二都活性都增加,但差异消失,这是由于SO2存在时,反应生成的SO4^2-离子的酸性强于浓硝酸预氧化产生的含氧官能团的酸性,催化剂在使用前经过煅烧和氧化对催化剂活性有很大改善。SO2存在时,V2O5含量为1wt%的催化剂活性提高。  相似文献   

13.
The Ti-modified sepiolite (Ti-Sep)-supported Mn-Cu mixed oxide (yMn5Cu/Ti-Sep) catalysts were synthesized using the co-precipitation method. The materials were characterized by the X-ray diffraction scanning electron microscope, N2 adsorption-desorption, H2-TPR, O2-TPD, and XPS techniques, and their catalytic activities for CO oxidation were evaluated. It was found that the catalytic activities of yMn5Cu/Ti-Sep were higher than those of 5Cu/Ti-Sep and 30Mn/Ti-Sep, and the Mn/Cu molar ratio had a distinct influence on catalytic activity of the sample. Among the yMn5Cu/Ti- Sep samples, the 30Mn5Cu/Ti-Sep catalyst showed the best activity (which also outperformed the 30Mn5Cu/Sep catalyst), giving the highest reaction rate of 0.875 × 10–3 mmol·g–1·s–1 and the lowest T 50% and T 100% of 56°C and 86°C, respectively. Moreover, the 30Mn5Cu/Ti-Sep possessed the best low-temperature reducibility, the lowest O2 desorption temperature, and the highest surface Mn3+/Mn4+ atomic ratio. It is concluded that factors, such as the strong interaction between the copper or manganese oxides and the Ti-Sep support, good low-temperature reducibility, and good mobility of chemisorbed oxygen species, were responsible for the excellent catalytic activity of 30Mn5Cu/Ti-Sep.
  相似文献   

14.
A series of Co-La catalysts were prepared using the wet impregnation method and the synthesis of catalysts were modified by controlling pH with the addition of ammonium hydroxide or oxalic solution. All the catalysts were systematically investigated for NO oxidation and SO2 resistance in a fixed bed reactor and were characterized by Brunanuer–Emmett–Teller (BET) method, Fourier Transform infrared spectroscopy (FTIR), X–ray diffraction (XRD), Thermogravimetric (TG) and Ion Chromatography (IC). Among the catalysts, the one synthesized at pH = 1 exhibited the maximum NO conversion of 43% at 180°C. The activity of the catalyst was significantly suppressed by the existence of SO2 (300 ppm) at 220°C. Deactivation may have been associated with the generation of cobalt sulfate, and the SO2 adsorption quantity of the catalyst might also have effected sulfur resistance. In the case of the compact selective catalytic reduction (SCR), the activity increased from 74% to 91% at the highest gas hourly space velocity (GHSV) of 300000 h–1 when the NO catalyst maintained the highest activity, in excess of 50% more than that of the standard SCR.
  相似文献   

15.
以锐钛矿TiO2(P25)为载体采用原位生长法负载锰氧化物制备了Mn/TiO2催化剂,再以等体积浸渍-煅烧法对该催化剂掺杂氧化铈制备Ce(x)Mn/TiO2-y催化剂用以烟气低温SCR脱硝.在固定锰负载量(质量分数为8%)的基础上,考察了铈掺杂量(铈锰摩尔比)、煅烧温度对催化剂SCR脱硝性能的影响.采用TEM、BET、XRD和XPS等手段表征了催化剂的理化结构特性.结果发现,当Ce/Mn的摩尔比例为1.0,煅烧温度为300℃时,Ce(1.0)Mn/TiO2-300催化剂在150—300℃温度范围内、10500—27000 h-1的空速范围内,能够保持90%以上的NO转化率.理化性能分析结果表明,煅烧温度对催化剂的微观形貌影响显著,随着煅烧温度的升高,Ce(1.0)Mn/TiO2-500催化剂活性物种颗粒集聚明显、比表面积降低,且锰氧化物价态分布偏向于低价态;铈的掺杂有助于Ce(1.0)Mn/TiO2-300催化剂活性物种在载体表面的均匀分散,可以促进产生更多的Mn4+物种和更多的吸附氧,有利于催化剂低温SCR脱硝性能的提升.  相似文献   

16.
Chromium oxide and manganese oxide promoted ZrO2-CeO2 catalysts were prepared by a homogeneous precipitation method for the selective catalytic reduction of NO x with NH3. A series of characterization including X-ray diffraction (XRD), high-resolution transmission electron microscope (HR-TEM), Brunauer–Emmett–Teller (BET) surface area analysis, H2 temperatureprogrammed reduction (H2-TPR), and X-ray photoelectron spectroscopy (XPS) were used to evaluate the influence of the physicochemical properties on NH3-SCR activity. Cr-Zr-Ce and Mn-Zr-Ce catalysts are much more active than ZrO2-CeO2 binary oxide for the low temperature NH3-SCR, mainly because of the high specific surface area, more surface oxygen species, improved reducibility derived from synergistic effect among different elements. Mn-Zr-Ce catalyst exhibited high tolerance to SO2 and H2O. Cr-Zr-Ce mixed oxide exhibited>80% NO x conversion at a wide temperature window of 100°C–300°C. In situ DRIFT studies showed that the addition of Cr is beneficial to the formation of Bronsted acid sites and prevents the formation of stable nitrate species because of the presence of Cr6 +. The present mixed oxide can be a candidate for the low temperature abatement of NO x .
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17.
The NO/H2/O2 reaction was studied under oxidizing conditions in the 100-400 °C range over 0.1 wt% Pt supported on various metal oxides such as MgO, CeO2, SiO2, La2O3, CaO, Y2O3 and TiO2. The Pt/MgO and Pt/CeO2 catalysts showed good catalytic behaviours. Here, we find that the Pt/Mg-Ce-O catalyst, prepared from MgO and CeO2 by the sol-gel method, is a very active and selective catalyst towards N2 formation in the whole 100–400 °C range. This catalyst appears to be the most active, selective and stable one ever reported in the literature for the NO/H2/O2 reaction, even in the presence of 5%v H2O or 20 ppmv of SO2 in the feed stream.Selected article from the Regional Symposium on Chemistry and Environment, Krusevac, Serbia, June 2003, organised by Dr. Branimir Jovancicevic.  相似文献   

18.
Titanium dioxide is coated on the surface of MCM-41 wafer through the plasma enhanced chemical vapor deposition (PECVD) method using titanium isopropoxide (TTIP) as a precursor. Annealing temperature is a key factor affecting crystal phase of titanium dioxide. It will transform an amorphous structure to a polycrystalline structure by increasing temperature. The optimum anatase phase of TiO2 which can acquire the best methanol conversion under UV-light irradiation is obtained under an annealing temperature of 700°C for 2 h, substrate temperature of 500°C, 70 mL·min?1 of oxygen flow rate, and 100W of plasma power. In addition, the films are composed of an anatase-rutile mixed phase, and the ratio of anatase to rutile varies with substrate temperature and oxygen flow rate. The particle sizes of titanium dioxide are between 30.3 nm and 59.9 nm by the calculation of Scherrer equation. Under the reaction conditions of 116.8 mg·L-1 methanol, 2.9 mg·L?1 moisture, and 75°C of reaction temperature, the best conversion of methanol with UV-light is 48.2% by using the anatase-rutile (91.3/8.7) mixed phase TiO2 in a batch reactor for 60 min. While under fluorescent light irradiation, the best photoactivity appears by using the anatase-rutile (55.4/44.6) mixed phase TiO2 with a conversion of 40.0%.  相似文献   

19.
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   

20.
Various iron oxides are used for Fenton reactions to degrade organic pollutants. The degradation efficiency may be improved by transforming an iron oxide phase to another. Here, we report on the transformation of goethite into hematite by thermal treatment at 400 °C. The products were analyzed by X-ray diffractometry, Raman spectroscopy, scanning electron microscopy and N2-physisorption. The catalytic activities were measured for orange II bleaching at initial concentration of 25 mg L?1, pH 3, catalyst concentration of 0.2 g L?1; 5 mM H2O2, 30 °C. Results show that the synthesized goethite was successfully transformed into hematite, and the specific surface area of the material increased from 134 to 163 m2 g?1. The bleaching efficiency of the orange II dye reached 100 % for the hematite product, versus 78 % for goethite. Therefore, a moderate thermal treatment of a plasma-synthesized goethite improves the catalytic oxidation of organic pollutants.  相似文献   

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