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1.
Manganese acetate (MnAc) and manganese nitrate (MnN) were employed as precursors for the preparation of MnAc)/TiO2, Mn (N)/TiO2, Mn(Ac)-Ce/TiO2, and Mn(N)-Ce/TiO2 by impregnation. These complexes were used as catalysts in the low-temperature selective catalytic reduction of NO with NH3. The influence of manganese precursors on catalyst characteristics, the reduction activity, and the stability of the catalysts to poisoning by H2O and SO2 were studied. Experiments showed that Mn(N) produced MnO2 with large grain sizes in Mn(N)/TiO2 catalyst. On the contrary, Mn(Ac) led to highly dispersed and amorphous Mn2O3 in Mn (Ac)/TiO2 catalyst, which had better catalytic activity and stability to SO2 at low temperatures. The doping of cerium reduced the differences in catalytic performance between the catalysts derived from different Mn precursors.  相似文献   

2.
Wang CH  Lin SS  Chen CL  Weng HS 《Chemosphere》2006,64(3):503-509
A fixed bed reactor was used to assess the catalytic incineration of toluene by various transition-metal oxide species supported on gamma-Al(2)O(3). CuO/gamma-Al(2)O(3) was found to be the most active of seven catalysts investigated. The CuO species, with a Cu content of 5% (wt), was hence used with four different supports (CeO(2), gamma-Al(2)O(3), TiO(2) and V(2)O(5)) in order to define the optimal combination. Results of the catalytic incineration of toluene, X-ray diffraction (XRD) analysis, oxygen-temperature programmed desorption (O(2)-TPD), toluene-temperature programmed desorption (toluene-TPD) and hydrogen-temperature programmed reduction (H(2)-TPR) showed that CuO/CeO(2) was the most active catalyst, followed by CuO/gamma-Al(2)O(3). The activity of CuO/CeO(2) with respect to the VOC molecule was observed to follow this sequence: toluen>p-xylene>benzene. The addition of water vapor or CO(2) significantly inhibited the activity of the CuO/CeO(2) and CuO/gamma-Al(2)O(3) catalysts. The inhibiting effect of both was reversible for CuO/gamma-Al(2)O(3). For CuO/CeO(2), the inhibiting effect of CO(2) was reversible and even insignificant at a higher temperature (220 degrees C), but the effect of H(2)O vapor was somewhat irreversible at lower incineration temperatures (220 degrees C). For complete oxidation of toluene, the required reaction temperature increased with gas hourly space velocity (GHSV) and toluene inlet concentration.  相似文献   

3.
Janbey A  Clark W  Noordally E  Grimes S  Tahir S 《Chemosphere》2003,52(6):1041-1046
Using a bench-scale rig, the activities of Pt, Pd and Pt+Pd catalysts supported on gamma-Al(2)O(3) and on TiO(2) (anatase) for the complete oxidation of methane (300 ppmv) in air have been measured as a function of temperature; values of T(10), T(50) and T(90) together with the Arrhenius parameters (activation energy and pre-exponential factor) are reported. Pt is less active than Pd when deposited on the surface of the TiO(2), but more active when deposited on gamma-Al(2)O(3), however when combined, the Pt+Pd mixture is more active than either metal individually. The T(10) for Pt+Pd/gamma-Al(2)O(3) was being as low as 228 degrees C. The significance of the Arrhenius parameters, for metal containing catalysts is that they exhibit compensation with increasing activation energy, while securing a more rapid increase in conversion from 0% to 100% when the temperature is increased.  相似文献   

4.
Chang L  Chen IP  Lin SS 《Chemosphere》2005,58(4):485-492
It has been shown that the CeO2/gamma-Al2O3 catalyst is a feasible alternative to CeO2 for the catalytic wet air oxidation (CWAO) of phenol because it remains an effective catalyst and yet is cheaper to prepare. In this study, we found that the optimal cerium content in the CeO2/gamma-Al2O3 catalyst was 20 wt.%, regardless of catalyst loading. Furthermore, at 180 degrees C, with a phenol concentration of 1000 mg l(-1), and an O2 partial pressure of 1.0M Pa or 1.5M Pa, the optimal catalyst loading was 3.0 gl (-1). The efficacy of CWAO of phenol improved with O2 partial pressure, although the effects of O2 pressure were more significant between 0.5 MPa and 1.5 MPa than between 1.5 MPa and 2.0 MPa. After 2 h of reaction, approximately 100% phenol conversion and 80% total organic carbon (TOC) removal was recorded at 180 degrees C, 1000 mg l(-1) of phenol and 3.0 g l(-1) of catalyst. Because these percentages subsequently leveled off, it is suggested that 2 h is a suitable time over which to run the reaction. The efficacy of CWAO of phenol decreased as initial phenol concentration was raised (from 400 to 2500 mg l(-1)), with the exception of phenol conversion after about 2 h, for which 400 mg l(-1) produced the lowest phenol conversion figure. Higher phenol concentrations require both catalyst loading and O2 partial pressure to be increased to maintain high performance. For example, for 2000 mg l(-1) and 2500 mg l(-1) phenol, nearly 100% phenol conversion and 90% TOC removal after 4 h of reaction at 180 degrees C required 4.0 g l(-1) of catalyst and 2.0 MPa.  相似文献   

5.
Potassium-fly ash (K-FA) sorbents were investigated for high-temperature CO2 sorption. K-FAs were synthesised using coal fly ash as source of silica and aluminium. The synthesised materials were also mixed with Li2CO3 and Ca(OH)2 to evaluate their effect on CO2 capture. Temperature strongly affected the performance of the K-FA sorbents, resulting in a CO2 uptake of 1.45 mmol CO2/g sorbent for K-FA 1:1 at 700 °C. The CO2 sorption was enhanced by the presence of Li2CO3 (10 wt%), with the K-FA 1:1 capturing 2.38 mmol CO2/g sorbent at 700 °C in 5 min. This sorption was found to be similar to previously developed Li-Na-FA (2.54 mmol/g) and Li-FA (2.4 mmol/g) sorbents. The presence of 10 % Li2CO3 also accelerated sorption and desorption. The results suggest that the increased uptake of CO2 and faster reaction rates in presence of K-FA can be ascribed to the formation of K-Li eutectic phase, which favours the diffusion of potassium and CO2 in the material matrix. The cyclic experiments showed that the K-FA materials maintained stable CO2 uptake and reaction rates over 10 cycles.  相似文献   

6.
This paper concerns the incineration of isopropyl alcohol (IPA) using the ferrospinel catalyst MnFe2O4. It covers the preparation of the ferrospinel catalyst, the screening of catalytic activity, catalytic incineration testing, and 72-hr decay testing of the catalyst. The experimental results of catalyst screening reveal that the Mn/Fe catalyst is the best of five prepared catalysts (chromium/iron [Cr/Fe], manganese/iron [Mn/Fe], zinc/iron [Zn/Fe], nickel/iron [Ni/Fe], and pure magnetite [Fe3O4]). In tests of the catalytic incineration system used to convert IPA, 98% conversion was obtained at a space velocity of 24,000 hr(-1), an oxygen (O2) content of 21%, 1700 ppm of IPA, and a reaction temperature of 200 degrees C.  相似文献   

7.
Five sorption materials were studied with a focus on polishing pretreated stormwater: crushed limestone, shell-sand, zeolite, and two granulates of olivine. These materials are commercially available at comparatively low cost and have been subjected to a minimum of modification from their natural states. The sorbents were tested for phosphorus, arsenic, cadmium, chromium, copper, nickel, lead, and zinc at concentration and conditions relevant for typical stormwater. The materials were tested for sorption capacity and kinetics. Desorption was tested under neutral and alkaline conditions and in the presence of chloride. For most sorbent/sorbate combinations, significant sorption occurred within the first minutes of contact between sorbent and sorbate. Treatment to the low microgram per liter range could be achieved by contact times of less than 1 hour. The study indicated that sorption filters can be designed for long life expectancy at comparatively low cost by applying the materials tested.  相似文献   

8.
Chen IP  Lin SS  Wang CH  Chang SH 《Chemosphere》2007,66(1):172-178
The effect of promoter addition on activity of CeO(2)/gamma-Al(2)O(3) was assessed via the CWAO of phenol. Adding Cu as the promoter rendered the most effective performance, followed by Mn, although the performance of Mn-promoted catalyst was inferior to CeO(2)/gamma-Al(2)O(3). Mineralization of phenol was effectively implemented at 160 degrees C using Cu-promoted catalyst (Ce15Cu5). Furthermore, at 180 degrees C this catalyst produced about 100% conversion of phenol (1h) and 95% removal of chemical oxygen demand (4h), higher than that of CeO(2)/gamma-Al(2)O(3). In contrast, Mn-promoted catalyst (Ce15Mn5) required a temperature above 220 degrees C for acceptable performance. Activity of re-used catalyst declined noticeably, due to deposits of carbonaceous compounds and leaching of metal ions. Regeneration with acetone rinsing after the first run was effective in recovering activity of Ce15Cu5, although after a second run further regeneration with acetone rinsing had only a moderate effect, due to residual carbonaceous deposits and the additive effect of leached metal species in each run. As an alternative to acetone, HCl or HNO(3) solution (0.01 M) was less effective at regenerating activity. In promoted catalysts, leached metal ions accounted for the majority of mineralization of phenol, while the solid catalyst played a dual role of initiator and terminator of free radicals. Despite a superior catalytic performance, leaching of Cu(2+) from the promoted catalyst caused a severe decline in activity and poses the problem of secondary pollution of treated wastewater. Therefore, addition of Cu, as well as other metal species, is unfavorable in promoting the CeO(2)/gamma-Al(2)O(3) catalyst.  相似文献   

9.
Wang CH  Lin SS  Liou SB  Weng HS 《Chemosphere》2002,49(4):389-394
The CuO-MoO3/gamma-Al2O3 catalyst, confirmed previously as having good activity in the catalytic incineration of (CH3)2S2, was employed as the principal catalyst in this study. With the aim of improving catalyst activity and resistance to deactivation by sulfur compounds, a promoter was added either before adding the precursors of Cu and Mo or together with Cu and Mo onto the gamma-Al2O3. Promoters included transition metals and elements from groups IA-VIIA in the chemical periodic table. Experimental results reveal Cr2O3 as the most effective promoter, with an optimal composition of 5 wt.% Cu, 6 wt.% Mo and 4 wt.% Cr (designated as Cu(5)-Mo(6)-Cr(4)/gamma-Al2O3). Knowing that higher acidity can improve activity, we further investigated the effect of acid treatment on the performance of the Cu(5)-Mo(6)-Cr(4)/gamma-Al2O3 catalyst. Experimental results indicate the H2SO4-treated catalyst (Cu(5)-Mo(6)-Cr(4)/sulfated-gamma-Al2O3) has a better activity and durability. A study for finding an appropriate rate expression for the catalytic incineration of (CH3)2S2 by Cu(5)-Mo(6)-Cr(4)/sulfated-gamma-Al2O3 was carried out in a differential reactor. The results show that the Mars-Van Krevelen model is applicable to this destructive oxidation reaction. Results additionally reveal that competitive adsorption of CH4 reduces conversion of (CH3)2S2.  相似文献   

10.
This is a laboratory study on the reduction of combustion-generated hydrochloric acid (HCl) emissions by in-furnace dry-injection of calcium-based sorbents. HCl is a hazardous gaseous pollutant emitted in significant quantities by municipal and hazardous waste incinerators, coal-fired power plants, and other industrial furnaces. Experiments were conducted in a laboratory furnace at gas temperatures of 600-1000 degrees C. HCl gas diluted with N2, and sorbent powders fluidized in a stream of air were introduced into the furnace concurrently. Chlorination of the sorbents occurred in the hot zone of the furnace at gas residence times approximately 1 s. The sorbents chosen for these experiments were calcium formate (CF), calcium magnesium acetate (CMA), calcium propionate (CP), calcium oxide (CX), and calcium carbonate (CC). Upon release of organic volatiles, sorbents calcine to CaO at approximately 700 degrees C, and react with the HCl according to the reaction CaO + 2HCl <=> CaCl2 + H2O. At the lowest temperature case examined herein, 600 degrees C, direct reaction of HCl with CaCO3 may also be expected. The effectiveness of the sorbents to capture HCl was interpreted using the "pore tree" mathematical model for heterogeneous diffusion reactions. Results show that the thin-walled, highly porous cenospheres formed from the pyrolysis and calcination of CF, CMA, and CP exhibited high relative calcium utilization at the upper temperatures of this study. Relative utilizations under these conditions reached 80%. The less costly low-porosity sorbents, calcium carbonate and calcium oxide also performed well. Calcium carbonate reached a relative utilization of 54% in the mid-temperature range, while the calcium oxide reached an 80% relative utilization at the lowest temperature examined. The data matched theoretical predictions of sorbent utilization using the mathematical model, with activation energy and pre-exponential factors for the calcination reaction of 17,000 K and 300,000 (g gas/cm2/s/atm gas), respectively. Thus, the kinetics of the calcination reaction were found to be much faster (approximately 500 times) than those of the sulfation reaction examined previously in this laboratory.  相似文献   

11.
Fe(3+)-, Cr(3+)-, Cu(2+)-, Mn(2+)-, Co(2+)-, and Ni(2+)-exchanged Al2O3-pillared interlayer clay (PILC) or TiO2-PILC catalysts are investigated for the selective catalytic reduction (SCR) of nitric oxide by ammonia in the presence of excess oxygen. Fe(3+)-exchanged pillared clay is found to be the most active. The catalytic activity of Fe-TiO2-PILC could be further improved by the addition of a small amount of cerium ions or cerium oxide. H2O and SO2 increase both the activity and the product selectivity to N2. The maximum activity on the Ce-Fe-TiO2-PILC is more than 3 times as active as that on a vanadium catalyst. Moreover, compared to the V2O5-WO3/TiO2 catalyst, the Fe-TiO2-PILC catalysts show higher N2/N2O product selectivities and substantially lower activities (by approximately 85%) for SO2 oxidation to SO3 under the same reaction conditions. A 100-hr run in the presence of H2O and SO2 for the CeO2/Fe-TiO2-PILC catalyst showed no decrease in activity.  相似文献   

12.
Catalyst sorbents based on alumina-supported CuO, CeO2, and CuO-CeO2 were applied to a dry scrubber to clean up the SO2/HCl/NO simultaneously from pilot-scale fluidized-bed incineration flue gas. In the presence of organic compounds, CO and the submicron particles SO2 and HCI removed by the fresh catalyst sorbents and NO reduced to N2 by NH3 under the catalysis of fresh and spent desulfurization/dechloridization (DeSO2/DeHCl) catalyst sorbents (copper compounds, Cu, CuO, and CuSO4) were evaluated in this paper. The fresh and spent catalyst sorbents were characterized by the Brunner-Emmett-Teller method (BET), X-ray powder diffraction (XRPD), scanning electron microscopy (SEM), inductively coupled plasma-mass spectrometry (ICP-MS), and the elemental analyzer (EA). The study showed that the performances of CuO, CeO2, and CuO-CeO2/gamma-Al2O3 were better than that of Ca(OH)2. The removal efficiency of SO2 and HCl was 80-95% in the dry scrubber system. Under NH3/NO = 1, NO could not be reduced to N2 because it was difficult to control the ratio of air/fuel in the flue gas. For estimating the feasibility of regenerating the spent catalyst sorbents, BET and EA analyses were used. They indicated that the pore structures were nearly maintained and a small amount of carbon accumulated on their surface.  相似文献   

13.
The species of copper and zinc, such as bioexchangeable, skeletal, easily reducible (Fe and Mn oxides), moderately reducible (crystalline Mn oxide), organic combined with sulfides, and detritus with minerals, in mud and sand, separated from the surface Antarctic Ocean and the Taiwan Erhjin Chi coastal (including river and estuarine) sediments, have been analyzed by sequential leaching methods. Results show that in the Antarctic Ocean sediments, high concentrations of total copper (128 mg/kg) and zinc (458 mg/kg) were found in the high mud (99.09%) content samples compared with the low concentrations of total copper (83.8 mg/kg) and zinc (288 mg/kg) in low mud (51.69%) content samples. High concentrations of copper, zinc, manganese and iron are possibly due to the characteristics of manganese nodules, in which the species of copper and zinc are mainly contained in the crystalline Mn oxide phase. In the Taiwan Erhjin Chi coastal sediments, the total copper and zinc concentrations in mud and sand vary with season and location. High values were generally observed in the river sediments during the dry season, and low values were in the estuarine and coastal sediments during the heavy rainy season. High percentages of copper (as high as 49.4%) and zinc (as high as 76.7%) in mud and sand were in the bioexchangeable phase including the skeletal phase. This result might be correlated with the problems arising from human impact on copper and zinc as well as sewage pollution in Taiwan. In the organic combined phase, biogenic particulate matter related to higher primary productivity in the Antarctic Ocean is also discussed.  相似文献   

14.
Kahle M  Stamm C 《Chemosphere》2007,68(7):1224-1231
Substantial amounts of sulfonamides, ionizable, polar veterinary antimicrobials, may reach the environment by spreading of manure. Sorption to soils and sediments is a crucial but not sufficiently understood process influencing the environmental fate of sulfonamides. Therefore, we investigated sorption of sulfathiazole to clay minerals (montmorillonite, illite) and ferrihydrite for varying pH values and two contact times (1d, 14 d) under sterile conditions. Results were compared to sulfathiazole sorption to organic sorbents. Sulfathiazole sorption to inorganic sorbents exhibited pronounced pH dependence consistent with sorbate speciation and sorbent charge properties. While sulfathiazole cations were most important for sorption to clay minerals, followed by neutral species, ferrihydrite was a specific anion sorbent, showing significant sorption only between pH 5.5-7. Experiments revealed a substantial increase of sorption with time for ferrihydrite (pH 5.5-7) and illite (pH<5.5). Reasons may be disaggregation of clay minerals and, for ferrihydrite, diffusion and sorption of sulfathiazole in micropores. Independent of contact time and pH, sorption to inorganic sorbents was more than an order of magnitude lower than to organic sorbents. This implies that in many topsoils and sediments inorganic sorbents play a minor role. Our results highlight the need to account for contact time and speciation when predicting sulfonamide sorption in the environment.  相似文献   

15.
Abstract

An entrained-flow system has been designed and constructed to simulate in-flight mercury (Hg) capture by sorbent injection in ducts of coal-fired utility plants. The test conditions of 1.2-sec residence time, 140 °C gas temperature, 6.7 m/sec (22 ft/sec) gas velocity, and 0–0.24 g/m3 (0–15 lbs of sorbent per 1 million actual cubic feet of flue gas [lb/MMacf]) sorbent injection rates were chosen to simulate conditions in the ducts. Four kinds of sorbents were used in this study. Darco Hg-LH served as a benchmark sorbent with which Hg control capability of other sorbents could be compared. Also, Darco-FGD was used as a representative raw activated carbon sorbent. Two different copper chloride-impregnated sorbents were developed in our laboratory and tested in the entrained-flow system to examine the possibility of using these sorbents at coal-fired power plants. The test results showed that one of the copper chloride sorbents has remarkable elemental mercury (Hg0) oxidation capability, and the other sorbent demonstrated a better performance in Hg removal than Darco Hg-LH.  相似文献   

16.
Studies on the catalytic destruction of 1,2-dichlorobenzene were carried out on a specially constructed semi-technical equipment whose most important element was a catalytic reactor with a monolithic catalyst in the form of 150 x 150 x 100 mm cubes. A catalyst made from cordierite with an active layer composed of Al2O3 - 64 wt%, TiO2 - 26 wt%, V2O5 - 6.6 wt% and WO3 - 3.4 wt% was used. The reactor made it possible to carry out the process in the temperature range 150-350 degrees C, at variable catalyst loading and different velocities of gas flow through the reactor. The content of 1,2-dichlorobenzene in the air was analysed by a chromatographic method. A significant effect of catalyst loading and temperature on 1,2-dichlorobenzene destruction efficiency was observed and no effect of the linear flow velocity through the catalyst on o-dichlorobenzene destruction efficiency was reported. The applied vanadium-tungsten catalyst on a monolithic carrier made from TiO2/gamma-Al2O3 revealed very good activity that resulted in an over 80% efficiency of 1,2-dichlorobenzene destruction at the temperature around 250 degrees C at a very high catalyst loading reaching ca. 8200 h(-1). Additionally, in this study the kinetics of 1,2-dichlorobenzene decomposition was determined, specifying the order of reaction and dependence of the decomposition rate constant on temperature, using a simple power-rate law model.  相似文献   

17.
Orlov A  Klinowski J 《Chemosphere》2009,74(2):344-348
Catalytic combustion of volatile organic compounds, such as propene, has been studied on manganese modified mesoporous molecular sieves. Powder X-ray diffraction, (29)Si nuclear magnetic resonance, nitrogen sorption and transmission electron microscopy show that the SBA-15 mesoporous silica molecular sieve can be modified with manganese using Mn(2)(CO)(10) or Mn(O(2)CMe)(2) without significant distortion of the host structure. The two products were catalytically active in propene oxidation, with SBA-15 modified with Mn(2)(CO)(10) showing significantly higher activity, possibly due to higher Mn content, than SBA-15 modified with Mn(O(2)CMe)(2).  相似文献   

18.
In the urban-rural transitional area of Hangzhou, China, 74 topsoil samples were collected from vegetable fields to measure the contents of arsenic (As), copper (Cu), cobalt (Co), cadmium (Cd), chromium (Cr), mercury (Hg), manganese (Mn), nickel (Ni), lead (Pb) and zinc (Zn). The combination of multivariate statistical and geostatistical methods successfully separated the contaminating elements (As, Cd, Cu, Hg, Pb and Zn) from uncontaminated elements (Co, Cr, Ni and Mn). A significant correlation was found between these uncontaminated elements and total Al2O3, Fe2O3, and SiO2 of the soils, indicating that the source of these elements was mainly controlled by soil-forming factors. On the other hand, these contaminating elements showed relatively weaker correlation and higher spatial variability, indicating that their enrichment and spatial heterogeneity were mostly affected by anthropic inputs. Through the pollution evaluation, it was found that only 30.8% of the study area did not suffer from moderate or severe pollution.  相似文献   

19.
Use of biomass sorbents for oil removal from gas station runoff   总被引:1,自引:0,他引:1  
The use of biomass sorbents, which are less expensive and more biodegradable than synthetic sorbents, for oil removal from gas station runoff was investigated. A bench-scale flume experiment was conducted to evaluate the oil removal and retention capabilities of the biomass sorbents which included kapok fiber, cattail fiber, Salvinia sp., wood chip, rice husk, coconut husk, and bagasse. Polyester fiber, a commercial synthetic sorbent, was also experimented for comparison purpose. Oil sorption and desorption tests were performed at a water flow rate of 20 lmin-1. In the oil sorption tests, a 50 mgl(-1) of used engine oil-water mixture was synthesized to simulate the gas station runoff. The mass of oil sorbed for all sorbents, except coconut husk and bagasse, was greater than 70%. Cattail fiber and polyester fiber were the sorbents that provided the least average effluent oil concentrations. Oil selectivity (hydrophobic properties) and physical characteristics of the sorbents are the two main factors that influence the oil sorption capability. The used sorbents from the sorption tests were employed in the desorption tests. Results indicated that oil leached out of all the sorbents tested. Polyester fiber released the highest amount of oil, approximately 4% (mass basis) of the oil sorbed.  相似文献   

20.
The objective of this study is to optimize experimental conditions of sorbent preparation from sewage sludge using experimental design methodology. Series of carbonaceous sorbents have been prepared by chemical activation with sulfuric acid. The sorbents produced were characterized, and their properties (surface chemistry, porous and adsorptive properties) were analyzed as a function of the experimental conditions (impregnation ratio, activation temperature and time). Carbonaceous sorbents developed from sludge allow copper ion, phenol and dyes (Acid Red 18 and Basic Violet 4) to be removed from aqueous solution as well as VOC from gas phase. Indeed, according to experimental conditions, copper adsorption capacity varies from 77 to 83 mg g(-1), phenol adsorption capacity varies between 41 and 53 mg g(-1) and VOC adsorption capacities (acetone and toluene) range from 12 to 54 mg g(-1). Each response has been described by a second-order model that was found to be appropriate to predict most of the responses in every experimental region. The most influential factors on each experimental design response have been identified. Regions in which optimum values of each factor were achieved for preparation of activated carbons suitable for use in wastewater and gas treatments have been determined using response surfaces methodology. In order to have a high mass yield and to minimize the energetic cost of the process, the following optimal conditions, 1.5 g of H2SO4 g(-1) of sludge, 700 degrees C and 145 min are more appropriate for use of activated carbon from sludge in water and gas treatments.  相似文献   

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