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1.
Hung WT  Lin CF 《Chemosphere》2003,53(7):727-735
Catalytic destruction of chlorinated compounds is one of the key methods in reducing pollutant emissions. For the purpose of utilizing waste materials, a catalyst was regenerated from ferric ion sludge, obtained from the addition of iron salts to precipitate heavy metals. The sludge was dewatered, heated (800 degrees C for 4 h), and ground into smaller particles. The regenerated ferric oxide particles were then used as the oxidation catalyst to destroy CO formation during the combustion of three chlorinated solvents and to suppress dioxin formation in flue gas in a real waste solvent. In the presence of catalyst, the combustion efficiency (ratio of CO(2) to the sum of CO(2) and CO) for chlorobenzene was more than 98% at 850 degrees C in a pilot-scale incinerator. The destruction and removal efficiencies of chlorobenzene, 2,4-dichlorophenol and trichlorofluoroethane were more than three nines. In the absence of catalysts, the flue gas emission from a real waste could not meet the regulatory dioxin standard of 0.1 ng-TEQ/Nm(3) even with the powdered activated carbon injection. The use of catalyst at either 100 or 300 g/h, however, was able to meet the emission standard.  相似文献   

2.
The effect of temperature on polyvinylchloride (PVC) combustion using a downstream tubular furnace was investigated for the formation of polycylcic aromatic hydrocarbons (PAHs) and chlorinated compounds. As the temperature increased, higher levels of PAHs were generated. Chlorinated compounds reached a peak at 600 degrees C, with low emissions recorded at 300 and 900 degrees C. There was a close correlation (R2 = 0.97) among polychlorinated biphenyls (PCBs), hexachlorobenzene, pentachlorobenzene, and polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans (PCDD/Fs). PAHs at all temperatures were analyzed in the gas phase. PCDD/Fs and PCBs were emitted as a solid phase at 300 and 600 degrees C and as a gas phase at 900 degrees C. For some PAHs, chlorobenzenes, and PCDD/Fs, a mathematical equation between the gas and solid phase and the reciprocal temperature in semilog proportion was derived. The proposed equation, which is log (amount in gas phase/amount in solid phase) = -A/T + B, where T is the temperature of the furnace and A and B are constants, for these species relating their gas/solid distributions showed a good relationship.  相似文献   

3.
Bae SW  Roh SA  Kim SD 《Chemosphere》2006,65(1):170-175
The effect of the additives on the selective non-catalytic reduction (SNCR) reaction has been determined in a three-stage laboratory scale reactor. The optimum reaction temperature is lowered and the reaction temperature window is widened with increasing concentrations of the gas additives (CO, CH4). The optimum reaction temperature is lowered and the maximum NO removal efficiency decreases with increasing the concentration of alcohol additives (CH3OH, C2H5OH). The addition of phenol lowers the optimum reaction temperature about 100-150 degrees C similar to that of the toluene addition. The volatile organic compounds (VOCs: C6H5OH, C7H8) can be utilized in the SNCR process to enhance NO reduction and removed at the same time. A previously proposed simple kinetic model can successfully apply the NO reduction by NH3 and the present additives.  相似文献   

4.
Catalytic oxidation of gaseous PCDD/Fs with ozone over iron oxide catalysts   总被引:2,自引:0,他引:2  
Wang HC  Chang SH  Hung PC  Hwang JF  Chang MB 《Chemosphere》2008,71(2):388-397
Catalytic oxidation of PCDD/Fs (polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans) with ozone (catalytic ozonation) over nano-sized iron oxides (denoted as FexOy) was carried out at temperature of 120-180 degrees C. The effects of operating temperature, ozone concentration, space velocity (SV) and water vapor contents on PCDD/F removal and destruction efficiencies via catalytic ozonation were investigated. High activity of the iron oxide catalyst towards PCDD/F decomposition was observed even at low temperatures with the aid of ozone. The PCDD/F removal and destruction efficiencies achieved with FexOy/O3 at 180 degrees C reach 94% and 91%, respectively. In the absence of ozone, the destruction efficiencies of all PCDD/F congeners are below 20% and decrease with increasing chlorination level of PCDD/F congener at lower temperature (120 degrees C). However, in the presence of ozone, the destruction efficiencies of all PCDD/F congeners are over 80% on FexOy/O3 at 180 degrees C. Higher temperature and ozone addition increase the activity of iron oxide for the decomposition of PCDD/Fs. Additionally, in the presence of 5% water vapor, the destruction efficiency of the PCDD/Fs is above 90% even at lower operating temperature (150 degrees C). It indicates that the presence of appropriate amount of water vapor enhances the catalytic activity for the decomposition of gas-phase PCDD/Fs.  相似文献   

5.
The object of this study is to investigate the effect of different operation conditions on the catalytic oxidation of trace organic compounds [i.e., benzene, toluene, ethylbenzene, and xylene (BTEX); and polyaromatic hydrocarbons (PAHs)] in incineration flue gas. A commercial Pd-based honeycomb catalyst, which is applied to treat flue gas with low organic concentrations and high gas velocity, is employed in this study. The investigated parameters include (1) effect of different space velocities, (2) effect of heavy metals, (3) effect of acid gas, and (4) effect of water vapor and ash particles. In this work, an effective catalyst oxidation system is constructed and expected to purify the incineration flue gas. Catalyst oxidation is a potential purification system that will meet the stricter regulations on the emissions of incineration systems. Experimental results showed that the destruction efficiency of PAHs and BTEX in Pd catalyst was generally greater than 80%. Decreasing the space velocity increased the decomposition efficiency of organic compounds. When the feedstock contained the heavy metals Pb and Cr, the oxidation of organic compounds was not inhibited. But the presence of Cd significantly decreased the oxidation efficiency. The acid gases SO2 and HCl in the flue gas could have influenced the crystal structure of PdO and subsequently deactivated/poisoned the Pd catalyst. The effect of water vapor on the catalytic destruction of PAHs and BTEX was not obvious.  相似文献   

6.
Supercritical fluid extraction (SFE) was used to extract polycyclic aromatic hydrocarbons (PAH) from a certified sample of marine sediment. This sample contains a great number of organic pollutants that are present in low concentrations. The extractions were carried out at 50 and 80 degrees C, at a pressure varying from 230 to 600 bar and using CO2 in the supercritical phase and the effect of three organic modifiers (methanol, n-hexane and toluene), added at 5%/vol, at the same temperature and pressure conditions, were then considered. PAHs were characterized by GC-MS and the recover yield was estimated for 6 PAHs that were representative of those present in the sample, according to their molecular weight and to the number of condensed rings. The analytical conditions giving the best recovery efficiency were used on an unpolluted soil sample spiked with 11 PAHs of environmental importance at a concentration similar to that certified for the sediment sample. An increase in the yield of recovered PAHs, using methanol as co-solvent, was observed while higher temperatures caused a negative effect on the quantity of recovered pollutants. The recovery yield for PAHs from the spiked soil sample was measured and found to be greater than 90%. Better recoveries were obtained for those compounds with higher molecular weight.  相似文献   

7.
Chang MB  Huang TF 《Chemosphere》2000,40(2):159-164
In this study, the effects of the temperature, oxygen content in the gas stream and carbon content in ash particles on PCDD/Fs formation on the fly ash surface were investigated. The optimum temperatures for dioxin formation were found at 350 degrees C for boiler ash, 300 degrees C for cyclone ash and 250 degrees C for ESP ash, respectively. Preliminary results indicate that the optimum temperature will decrease as the particle size decreases. When the O2 concentration is varied between 0% and 100%, the optimum oxygen content for PCDD/Fs formation is found to be at 7.5% for cyclone ash, and the PCDD/PCDF ratio increases with the increase of oxygen content. Dioxin formation is observed even for the gas containing no oxygen passed through the fly ash. Hence, other reacted routes that do not need O2 for dioxin formation take place on fly ash. The carbon content in fly ash is varied between 0% and 20% in this study, and the results have indicated that the maximum dioxin formation is to be found at 5%. The precursors are not injected into the fly ash or gas stream in all formation experiments, however, dioxin is still formed in fly ash. Consequently, other chlorinated routes besides Deacon reactions may take place on the fly ash surface.  相似文献   

8.
Chang MB  Chi KH  Chang SH  Yeh JW 《Chemosphere》2007,66(6):1114-1122
Partitioning of PCDD/F congeners between vapor/solid phases and removal and destruction efficiencies achieved with selective catalytic reduction (SCR) system for PCDD/Fs at an existing municipal waste incinerator (MWI) and metal smelting plant (MSP) in Taiwan are evaluated via stack sampling and analysis. The MWI investigated is equipped with electrostatic precipitators (EP, operating temperature: 230 degrees C), wet scrubbers (WS, operating temperature: 70 degrees C) and SCR (operating temperature: 220 degrees C) as major air pollution control devices (APCDs). PCDD/F concentration measured at stack gas of the MWI investigated is 0.728 ng-TEQ/Nm(3). The removal efficiency of WS+SCR system for PCDD/Fs reaches 93% in the MWI investigated. The MSP investigated is equipped with EP (operating temperature: 240 degrees C) and SCR (operating temperature: 290 degrees C) as APCDs. The flue gas sampling results also indicate that PCDD/F concentration treated with SCR is 1.35 ng-TEQ/Nm(3). The SCR system adopted in MSP can remove 52.3% PCDD/Fs from flue gases (SCR operating temperature: 290 degrees C, Gas flow rate: 660 kN m(3)/h). In addition, the distributions of PCDD/F congeners observed in the flue gases of the MWI and MSP investigated are significantly different. This study also indicates that the PCDD/F congeners measured in the flue gases of those two facilities are mostly distributed in vapor phase prior to the SCR system and shift to solid phase (vapor-phase PCDD/Fs are effectively decomposed) after being treated with catalyst. Besides, the results also indicate that with SCR highly chlorinated PCDD/F congeners can be transformed to lowly chlorinated PCDD/F congeners probably by dechlorination, while the removal efficiencies of vapor-phase PCDD/Fs increase with increasing chlorination.  相似文献   

9.
Bench-scale experiments have been conducted to evaluate a series of titania-supported Pt-Pd (as oxides) catalysts in the presence and absence of MoO3 and Fe2O3 additives for their effectiveness in the complete catalytic oxidation of volatile organic compounds (VOCs) in air likely to be found in waste gases. Under oxidizing conditions, all of the catalysts promoted the complete oxidation of VOCs to CO2 and H2O. 99 % Conversion was achieved with a C2H4-C2H6 gas mixture in air at temperatures between about 160–450 °C and at a space velocity of 20,000 h?1. Oxidation activity for the titania supported catalysts were found to decrease in the order Pt-Pd-Mo-Fe > Pt-Pd-Mo > Pt-Pd-Fe > Pt-Pd. However, the addition of MoO3 and Fe2O3 increase the catalyst activity and reduce the reaction temperature for the complete destruction. Ageing was also performed in order to study the stability of the most active catalyst. Pt-Pd-Mo-Fe (as oxides) on titania catalyst is effective in oxidizing a wide range of volatile organic compounds at relatively low temperatures (220–405 °C) and and at a space velocity of 40,000 h?1 and is resistant to poisoning by halogenated and amine volatile organic compounds.  相似文献   

10.
Hart JR 《Chemosphere》2004,54(10):1539-1547
Emissions of polychlorinated dibenzo-p-dioxins and dibenzofurans (dioxins) have been found from 57 field tests on the oxidation of low (a few to a few hundred) parts per million levels of chlorinated and non-chlorinated volatile organic compounds (VOCs). The oxidation occurs in catalytic oxidizers with platinum, platinum/palladium or chromium(IV) oxide combustion catalysts, or in thermal oxidizers (without a catalyst). The catalyst inlet temperatures ranged from 293 to 573 degrees C. The thermal oxidizer operating temperatures (post-flame) were from 773 to 927 degrees C. Data of the toxic dioxin and furan isomers are reported and also weighted and expressed as international toxic equivalents (TEQ) of 2,3,7,8-tetrachlorodibenzo-p-dioxin. The maximum stack emissions, 1.07 ng/m3 TEQ, occurred at 293 degrees C. Salient results of this field study are: (1) TEQ levels in the stack exponentially increase with a decrease in operating temperature, an empirical equation is TEQ (ng/dscm)=8.4 exp(-0.0084T degrees C); (2) dioxin/furan production occurs at the combustion catalyst; (3) small variations in temperature cause large changes in the congener distribution of the dioxin and furan isomers; (4) molar TEQ yields from the parent compounds fed to the oxidizers are very small (10(-9)-10(-13)); (5) catalytic and thermal oxidizers may destroy dioxins fed from the ambient air; and (6) the oxidation of chlorinated VOCs with non-chlorinated VOCs reduces emissions of dioxins, likely due to the consumption of Cl in producing HCl. Laboratory investigations are needed to understand how dioxins are formed (and emitted) under conditions of this study.  相似文献   

11.
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   

12.
Adsorption of PCDD/F on MWI fly ash   总被引:3,自引:0,他引:3  
The removal of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/F) from waste incinerator off-gas is a costly task, because a considerable part of the PCDD/F may exist in the gas phase (often 50-100% around 200 degrees C). The volatile fraction passes the particle filter and the subsequent gas cleaning equipment, so that an additional unit is needed to remove the gaseous PCDD/F from the flue gas. Moreover, dioxins and furans can accumulate in some parts of the equipment in a way that they can act as a latent source. In this work, we investigate the possibility to adsorb the PCDD/F at the fly ash particles and to remove them during the filtration. The gas/particle partitioning of the PCDD/F depends on the temperature, the vapor pressure, the particle size, the particle number density and on the physical and chemical properties of the particle surface. These relationships are investigated by model calculations and by pilot scale experiments (500 Nm3/h) which employ one selected hexachlorinated dioxin congener. At room temperature, approx. 90% of the HxCDD are found in the particulate phase, while at 135 degrees C that portion is only 10%. This means that at ambient temperatures, the gas/particle partitioning of the dioxin corresponds well to the sublimation equilibrium. At higher temperatures, it is much different from the sublimation equilibrium and the apparent adsorption enthalpy is smaller than the enthalpy of sublimation. This observation is in agreement with literature data. From the above experiments and from similar literature data, the efficiency of fly ash particles as a sink for PCDD/F can be evaluated. The data suggest that the adsorption rate is not the limiting factor for the transfer into the particulate phase. The important factors appear to be the chemical composition of the fly ash and the temperature.  相似文献   

13.
A method involving supercritical fluid extraction (SFE) with a solid phase trap containing activated alumina was investigated for the rapid analysis of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), and dioxin like polychlorinated biphenyls (DL-PCBs) in soils and sediments. The samples were extracted by using supercritical carbon dioxide with water (2% versus CO(2) flow velocity) being used as an entrainer at a pressure of 30 MPa and a temperature of 130 degrees C for 50 min. The extracts were adsorbed on an activated alumina trap that was maintained at a temperature of 150 degrees C, and then, PCDD/DFs and DL-PCBs were eluted with 20 ml of hexane at 60 degrees C. After concentration, they were measured with a high-resolution gas chromatograph interfaced to a high-resolution mass spectrometric detector. The average concentrations of PCDD/DFs and DL-PCBs corresponded to the results obtained by the conventional method, and the reproducibility of this SFE method was below 21% of the relative standard deviations for all samples. The total time required for the analysis of the pretreatment of this method was only 2 h.  相似文献   

14.
Incineration flue gas contains polycyclic aromatic hydrocarbons (PAHs) and sulfur dioxide (SO2). The effects of SO2 concentration (0, 350, 750, and 1000 ppm), reaction temperature (160, 200, and 280 °C), and the type of activated carbon fibers (ACFs) on the removal of SO2 and PAHs by ACFs were examined in this study. A fluidized bed incinerator was used to simulate practical incineration flue gas. It was found that the presence of SO2 in the incineration flue gas could drastically decrease removal of PAHs because of competitive adsorption. The effect of rise in the reaction temperature from 160 to 280 °C on removal of PAHs was greater than that on SO2 removal at an SO2 concentration of 750 ppm. Among the three ACFs studied, ACF-B, with the highest microporous volume, highest O content, and the tightest structure, was the best adsorbent for removing SO2 and PAHs when these gases coexisted in the incineration flue gas.
ImplicationsSimultaneous adsorption of sulfur dioxide (SO2) and polycyclic aromatic hydrocarbons (PAHs) emitted from incineration flue gas onto activated carbon fibers (ACFs) meant to devise a new technique showed that the presence of SO2 in the incineration flue gas leads to a drastic decrease in removal of PAHs because of competitive adsorption. Reaction temperature had a greater influence on PAHs removal than on SO2 removal. ACF-B, with the highest microporous volume, highest O content, and tightest structure among the three studied ACFs, was found to be the best adsorbent for removing SO2 and PAHs.  相似文献   

15.
Han GB  Park NK  Yoon SH  Lee TJ 《Chemosphere》2008,72(11):1744-1750
SO(2) reduction by CO over SnO(2) catalyst was studied in this work. The parameters were the reaction temperature, space velocity (GHSV) and [CO]/[SO(2)] molar ratio. The optimal temperature, GHSV and [CO]/[SO(2)] molar ratio were 550 degrees C, 8000 h(-1) and 2.0, respectively. Under these conditions, the SO(2) conversion and sulfur selectivity were about 78% and 68%, respectively. The following reaction pathway involving two mechanisms was proposed in SO(2) reduction by CO over SnO(2) catalyst: in the first step involving Redox mechanism, the elemental sulfur was produced by the mobility of the lattice oxygen between SO(2) and SnO(2) surface. In the second step, COS was formed by the side reaction between elemental sulfur and CO or metal sulfide and CO. In the third step involving COS intermediate mechanism, the abundant elemental sulfur was produced by the SO(2) reduction by COS which was produced in the second step and was more effective reducing agent than CO.  相似文献   

16.
For the analysis of trace organic pollutants in environmental samples using a gas chromatographic (GC) instrument, large-volume injection using the programmable temperature vaporization (PTV) technique has many advantages over the traditional split/splitless injection. By increasing the injection volume from 1 or 2 microL with a split/splitless inlet to 60 microL or higher with the PTV inlet, analytical sensitivity is greatly enhanced for analytes with low concentrations. Results obtained from optimization of instrument operational parameters for analyzing polycyclic aromatic hydrocarbons (PAHs) are reported in this paper. The laboratory method detection limits for 16 PAHs and six deuterated PAH surrogates were determined using seven replicate spike samples. The initial temperature of the inlet was found to be critical in determining the analytical sensitivity of PAHs with two or three rings due to loss of these relatively highly volatile compounds during solvent vaporization. For most PAHs, the response of the mass spectrometry detector increased proportionally as the total injected volume was increased up to 150 microL. Significant interference from rubber material of the sample vial septa was observed.  相似文献   

17.
Abstract

The effect of temperature on polyvinylchloride (PVC) combustion using a downstream tubular furnace was investigated for the formation of polycylcic aromatic hydrocarbons (PAHs) and chlorinated compounds. As the temperature increased, higher levels of PAHs were generated. Chlorinated compounds reached a peak at 600°C, with low emissions recorded at 300 and 900°C. There was a close correlation (R2 = 0.97) among polychlorinated bi-phenyls (PCBs), hexachlorobenzene, pentachloroben-zene, and polychlorinated dibenzo-p-dioxins and poly-chlorinated dibenzofurans (PCDD/Fs). PAHs at all temperatures were analyzed in the gas phase. PCDD/Fs and PCBs were emitted as a solid phase at 300 and 600°C and as a gas phase at 900°C. For some PAHs, chloroben-zenes, and PCDD/Fs, a mathematical equation between the gas and solid phase and the reciprocal temperature in semilog proportion was derived. The proposed equation, which is log (amount in gas phase/amount in solid phase) = ?A/T + B, where T is the temperature of the furnace and A and B are constants, for these species relating their gas/solid distributions showed a good relationship.  相似文献   

18.
With the advances made in the past decade, catalytic incineration of volatile organic compounds (VOCs) has become the technology of choice in a wide range of pollution abatement strategies. In this study, a test was undertaken for the catalytic incineration, over a chromium oxide (Cr2O3) catalyst, of n-hexane, benzene, and an emission air/vapor mixture collected from an oil/water separator of a refinery. Reactions were carried out by controlling the feed stream to constant VOC concentrations and temperatures, in the ranges of 1300-14,700 mg/m3 and 240-400 degrees C, respectively. The destruction efficiency for each of the three VOCs as a function of influent gas temperature and empty bed gas residence time was obtained. Results indicate that n-hexane and the oil vapor with a composition of straight- and branch-chain aliphatic hydrocarbons exhibited similar catalytic incineration effects, while benzene required a higher incineration temperature or longer gas retention time to achieve comparable results. In the range of the VOC concentrations studied, at a given gas residence time, increasing the operating temperature of the catalyst bed increased the destruction efficiency. However, the much higher temperatures required for a destruction efficiency of over 99% may be not cost-effective and are not suggested. A first-order kinetics with respect to VOC concentration and an Arrhenius temperature dependence of the kinetic constant appeared to be an adequate representation for the catalytic oxidation of these volatile organics. Activation energy and kinetic constants were estimated for each of the VOCs. Low-temperature destruction of the target volatile organics could be achieved by using the Cr2O3 catalyst.  相似文献   

19.
Air pollution control devices (APCDs) are not compulsory for medical waste incinerators (MWIs) in developing countries. In South Africa, combustion gases are usually vented directly to the atmosphere at temperatures greater than the formation temperature of dioxin. The possibility of dioxin formation outside the incinerator stack has been hypothesized. A plume model has been developed and tested in the wind tunnel with a scale model of an incinerator stack. The plume temperature and trajectory predictions of the plume model were verified within a +/- 3% experimental accuracy. Using South African data, the plume model predicts that the residence time of gases in the temperature range of 150-450 degrees C in a plume is 1.3 sec on average for 5% of a year (18 days) at meteorological conditions resulting in wind speeds of less than 1 m/sec. Two published dioxin formation models were used to assess the probability of dioxin formation in the plume. The formation models predict that the average polychlorinated dibenzodioxins/furans (PCDD/Fs) formed in the plume will exceed the stack emission regulations in South Africa of 0.2 ng/Nm3 toxic equivalent quotient (TEQ) by between 2 and 40 times. The calculated concentrations do not include additional gaseous PCDD/F compounds that may be formed at high-temperature post-combustion zones through pyrosynthesis mechanisms.  相似文献   

20.
The paper deals with the use of a rotary kiln furnace for thermal destruction of dioxin combined with a baghouse filter for the recycling of entrained flyash and an activated carbon filter for adsorbtion of dioxin traces transported by gas phase.Measurements performed at a pilot plant with a throughput of 200 kg flyash/hr revealed 99.5 % destruction of dioxins and furans. Furthermore, the destruction of all organics, 95 % desorbtion of mercury and quantitative elimination of peripheral (located at the surface) Chromium (CrVI) were achieved.An activated carbon filter placed in the fluegas stream of an municipal waste incinerator was started up to investigate the influence of interfering constituants like SO2, HCl etc. on the filter performance. Loading data, removal efficiency and make up performance were collected.  相似文献   

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