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1.
The levels and homologue profile of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) from stack gas of three typical fluidized bed incinerators co-firing municipal solid waste (MSW) with Chinese coal were measured. The PCDD/Fs emission was in the range of 0.0054-0.1961 ng I-TEQ/N m(3). Comparison of PCDD/Fs detection results by HRGC/HRMS and HRGC/LRMS suggested that it was feasible to detect fly ash with high PCDD/Fs concentration by HRGC/LRMS. Several factors on PCDD/Fs emission were discussed. The primary reason for the lower PCDD/Fs emission was the inhibition mechanism of relatively high sulfur in feeding coal on PCDD/Fs formation. The emission results also showed that there was no directly correlation between PCDD/Fs levels and CO, O(2) and HCl concentration in flue gas. It was estimated that about 0.1034 g I-TEQ was annually emitted to atmosphere from the tested three MSW incinerators (total daily treatment capacity is 800 tonnes MSW).  相似文献   

2.
Levels of dioxins (PCDD/Fs) were determined in fly ash samples collected from a power plant burning bagasse for production of electricity. The concentrations ranged from 2.2 pgWHO-TEQ/g to 190 pg WHO-TEQ/g with samples collected after ESP containing significantly much higher (more than 12 times on average) levels than samples collected before ESP. Our results seem to indicate that both the de novo and the precursor mechanisms are significantly involved in the formation of dioxins the fly ash during combustion of bagasse.  相似文献   

3.
Several fly ash samples from different countries were analyzed for dibromopolychlorodibenzo-p-dioxins and -dibenzofurans (DBPCDD/Fs) using capillary column gas chromatography/high-resolution mass spectrometry. Concentrations of these compounds ranged from low to high parts-per-trillion (pptr) depending on the location where the samples were collected. The mass spectrometer, operated at greater than 10,000 mass resolution in combination with the high resolving power of capillary column GC, permitted characterization of DBPCDD/Fs in municipal waste incinerator fly ash for the first time. The isomer patterns of tetra- through octa-congener groups of DBPCDD/Fs are remarkably similar regardless of where the fly ash originated, indicating common mechanisms of formation of these compounds in the incinerators.  相似文献   

4.
Removal of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) from fly ash poses a serious problem. In the study presented here, we used a microbial biocatalyst which is a mixture of 4 bacterial and 5 fungal dioxin-degrading strains. The ability of this biocatalyst to bioremediate PCDD/Fs from contaminated municipal solid waste incinerator (MSWI) fly ash was examined by solid-state fermentation under laboratory conditions. Treatment of MSWI fly ash with the microbial biocatalyst for 21 days resulted in a 68.7% reduction in total toxic PCDD/Fs. Further analyses revealed that the microbial biocatalyst also removed 66.8% of the 2,3,7,8-substituted congeners from the fly ash. During the treatment period, the presence of the individual strains composing the microbial biocatalyst was monitored by the amplification of strain-specific DNA sequences followed by denaturing gradient gel electrophoresis (DGGE). This analysis showed that all of the bacterial and fungal strains composing this dioxin-degrading microbial mixture maintained under the dioxin treatment conditions. These results demonstrate that this microbial biocatalyst could potentially be used in the bioremediation of PCDD/Fs from contaminated fly ash.  相似文献   

5.
Polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in the surrounding environment (outdoor) and workplace air of two municipal solid waste incinerators (MSWIs, T and M) were characterized and compared. T and M represented two typical municipal solid waste incinerators in the north of Taiwan, which have different processes for controlling the PCDD/F emissions. The results of this study are summarized as follows. (1) The total PCDD/F and the total PCDD/F WHO-TEQ concentrations in the workplace air were 5-13 and 5-15 times higher than those in the outdoor air, respectively. Obviously, it is worthwhile to explore more on health risk assessment for exposure of PCDD/Fs emitted from MSWIs, particularly in the workplace air. (2) Mean total PCDD/F I-TEQ concentrations in the outdoor air ranged between 0.0216 and 0.155 pg I-TEQ/Nm(3) and averaged 0.0783 pg I-TEQ/Nm(3) (0.0828 pg WHO-TEQ/Nm(3)) during two seasons for two MSWIs, which were 6.5-fold higher than that of a remote site (0.0119 pg I-TEQ/Nm(3) or 0.0132 pg WHO-TEQ/Nm(3)) in Taiwan. However, the above outdoor air concentration levels in the MSWIs were still much lower than the air quality limitation of PCDD/Fs (0.6 pg I-TEQ/Nm(3)) in Japan []. (3) PCDFs were the primary toxicity distributors for PCDD/Fs in the outdoor air, since the ratios of PCDDs/PCDFs (I-TEQ) at all sampling sites ranged from 0.180 to 0.492 and were less than unity. (4) The OCDD, OCDF, 1,2,3,4,6,7,8-HpCDD and 1,2,3,4,6,7,8-HpCDF were the four dominant species in both workplace and outdoor air near MSWIs. (5) By spraying water on and wetting both the fly and bottom ashes, the mean total PCDD/F I-TEQ concentration in the workplace air was reduced 86.9% in the T MSWI. The above results indicate an appropriate improving action did inhibit the fugitive emission of PCDD/Fs and reduce the health risk of workers during work handling ashes in MSWIs.  相似文献   

6.
The potential of mechanochemical treatment (MC) to degrade PCDD/Fs contained in fly ash was tested via grounding with and without calcium oxide (CaO) under atmospheric pressure. Three types of fly ash collected from medical waste incineration were compared, originating either from rotary kiln fluidized bed multi-stage incinerator using activated carbon spray (FA1, FA2), or a simple stoker incinerator without activated carbon spray (FA3). In test I: CaO to FA1 mixed at ratio of 6-60% was milled at rotational speed of 350 rpm; in test II: FA2 and FA3 without CaO were milled at rotational speed of 400 rpm. The duration of the tests was 2h. The results from the present study indicate that (1) under two test conditions of with and without CaO, PCDD/Fs contained in real fly ash both can be degraded by mechanochemical treatment, (2) under condition of blending with CaO, the degradation efficiency of PCDD/Fs increased with increasing ratio of CaO, (3) the degradation efficiency of PCDD/Fs may increase with rotational speed increasing and (4) the destruction and dechlorination are major mechanism for PCDD/Fs degradation. These results show that mechanochemical treatment is a high potential technology for PCDD/Fs degradation in fly ash.  相似文献   

7.
Although many researches focused on the polychlorinated dibenzo-p-dioxins/dibenzofuran (PCDD/F) emissions from stack, in the bottom ash and in the surrounding environment, researches focused on PCDD/F mass distributions in the whole incineration plant have seldom been addressed. This study determined PCDD/F emissions in the whole plant. A high-resolution gas chromatograph/high-resolution mass spectrometer was utilized for analyzing 17 PCDD/F species. Experimental results displayed that PCDD/Fs were formed during fly ash from super heater (SH), economizer (EC), semi-dryer absorber (SDA) and fabric filter (FF) was transferred to fly ash pit. Mass distribution ratios of PCDD/Fs in g I-TEQ (Toxicity Equivalency Quantity) per week from stack, SH, EC, SDA, FF, generation and bottom residue (BR) in start-up operations were 14.6%, 0.1%, 8.3%, 1.0%, 41.7%, 33.4% and 0.9%, respectively. Above results indicated that main PCDD/F source in the MSWI was from fly ash. However, the fly ash is easily controlled and PCDD/F emitted from stack flue gases will be difficult to be handled. Therefore, we should pay more attention on PCDD/F emission from flue gases especially from start-up procedure. Besides, fly ash should be controlled by sodium hypophosphite before being landfilled. MSWI did require further detoxification treatments for the solid residues and flue gases.  相似文献   

8.
This study determined the polychlorinated dibenzo-p-dioxins/dibenzofurans (PCDD/Fs) contents in ash in the super heater (SH), economizer (EC), semi-dryer absorber (SDA), fabric filter (FF), fly ash pit (FAP) and bottom residue (BR) in a municipal solid waste incinerator (MSWI). A high-resolution gas chromatograph/high-resolution mass spectrometer (HRGC/HRMS) was utilized for analyzing 17 PCDD/F species. Experimental results showed that average PCDD/F contents in ash samples from the SH, EC, SDA, FF, FAP and BR were 0.102, 0.788, 0.210, 1.95, 2.04 and 0.0218 ng I-TEQ g(-1), respectively. PCDD/F content was very low in the SH and BR due to high temperatures (around 461 degrees C in the SH and 914 degrees C in combustion chamber). Conversely, total PCDD/F content was significantly high in ash samples from the EC (around 340 degrees C), mainly because the temperature is within the favorable range of 250-400 degrees C for PCDD/F formation due to de nova reformation mechanisms. Although the SDA operated at 245 degrees C, the PCDD/F content decreased very significantly, mainly because the temperature was relatively low and because calcium carbonate was introduced into flue gases to dechlorinate and dilute chlorine-containing species. PCDD/Fs were captured by the active carbon in the FF. Furthermore, the duration that fly ash remained in the FF was longer than that for other incinerator units, and thus causing an increasing trend of PCDD/Fs level downstream (except the SDA). Total PCDD/Fs emission factors (microg tonnes-waste(-1); microg I-TEQ tonnes-waste(-1)) in ash samples from different units were: SH (42.3; 0.846), EC (326; 6.12), SDA (58.1; 1.10), FF (1540; 61.3), FAP (2950; 107) and BR (537; 4.31). Most PCDD/Fs in ash were contributed by the FF (about 56%), and the generation of PCDD/Fs in ash was significant (about 35%) during the transfer process from different units to the FAP. A strong and positive correlation in a logarithmic form existed between PCDD/Fs and chlorine (Cl(-1)) contents in ash. In Taiwan, the government policy for incineration residues advocates their reuse as road sub-bases or secondary building materials provided that total PCDD/Fs content is below the legal limit (1 ng I-TEQ g(-1)). Thus, ash with total PCDD/Fs content below the legal limit, such as that from the SH, EC, SDA and BR, can be collected and transferred to the FAP and reused. Ash with total PCDD/Fs content exceeding the legal limit, such as that from the FF, should be collected separately and be treated properly before being disposal in a landfill.  相似文献   

9.
Different from most previous studies with quantity-limited data, this paper presents PCDD/F content characterization in the fly ash discharged from sixteen large-scale commercial MSWIs. From the results with over hundreds of data using periodically sampling and analysis, it was found that the PCDD/F contents in the fly ash were from 9.07 to 46.68 ng/g, d.w., and if based on international toxicity equivalent quantity, they were from 0.78 to 2.86 ng I-TEQ/g, d.w. The higher chlorinated PCDDs likely dominated more than lower chlorinated PCDDs, but this tendency was not for PCDFs. The OCDD had the highest contribution to the total PCDD/F content, but if based on I-TEQ content, 2,3,4,7,8-PeCDF is the PCDD/F congener with the highest toxicity contribution. Moreover, the PCDD/F characteristic index (DCI) is suggested using the representative congener content of 2,3,4,7,8-PeCDF to characterize the fly ash. The DCI is 0.875 ± 7.6% for the fly ash discharged from the MSWI with the APCD assembly of SD, AC and BF. The findings obtained in this work provide overview information on the PCDD/F content characterization in fly ash. They will provide PCDD/F fingerprint information to distinguish from other PCDD/F sources, like steel refinery industry, hazardous waste incinerators, or cement kilns, and thus be applied to fly ash management in the environment.  相似文献   

10.
Emissions of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) from an industrial park operated as Taiwan's center of metallurgical industries were investigated. The characteristics of mean PCDD/F I-TEQ concentrations, congener profiles and emission factors of each source were studied over samples of stack flue gases of individual sources. Different characteristics of congener profiles and large variations of emission factors of secondary aluminum smelters (ALSs) were observed. The mean emission factors of electric arc furnaces were comparable to those for ALSs and much greater than those of municipal solid waste incinerators and sinter plants, but still less than that of clinical waste incinerators. Annual PCDD/F emission contribution of each source was estimated, raising critical concerns over the overall PCDD/F emissions from metallurgical processes. The metallurgical industries altogether contributed approximately 98.1% of the total annual emissions, while waste incinerators only 1.9%. The contributions by sinter plants and metallurgical industries to the total annual emissions of the Park were much higher than the corresponding national averages of Taiwan. The combined dioxin emissions from the entire metallurgical processes and their controls should be seriously envisaged by industrial parks devoted to metal productions.  相似文献   

11.
In this study, a dual bag filter system was established to decrease the concentration of polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans (PCDD/Fs) in the stack flue gases of a fly ash treatment plant, which retained zinc from the fly ash of electric arc furnaces. Compared to the original single bag filter system with activated carbon injection (ACI) of 40 kg h(-1), the PCDD/F concentrations in the stack flue gas after the plant was equipped with the dual bag filter system dropped enormously from 3.38-7.73 ng I-TEQNm(-3) to 0.03 ng I-TEQNm(-3), and the total PCDD/F I-TEQ removal efficiency increased from 97.6% to 99.3% with ACI of 16 kg h(-1), that is, about 40% of the original AC usage. The AC utilization efficiency (0.560 mg I-TEQ absorbed kg ACI(-1)) of the dual bag filter system (AC: 16 kg h(-1)) was estimated about three times higher than that (0.192 mg I-TEQ absorbed kg ACI(-1)) of single bag filter system with ACI (40 kg h(-1)). The reason is that the particulate phase PCDD/Fs and some gas phase PCDD/Fs (captured by the recycled AC/ash mixture) were removed first by the first bag filter, and the rest of the gas phase PCDD/Fs were able to be adsorbed more completely by the AC/ash mixture due to a lower fly ash load, and then were removed by the second bag filter.  相似文献   

12.
针对如何在臭氧紫外光-滑动弧系统中建立稳定的二恶英发生源用于降解二恶英的实验系统.该发生源以医疗垃圾飞灰为对象,通过加热飞灰本身和飞灰索提液的方式使其中的二恶英在一段时间内连续挥发.结果表明,290℃时在飞灰发生源系统中,二恶英初始阶段挥发速率极快,后续的挥发速率急剧减小并趋于稳定,总挥发量仅为总量的10%,且难以再提高.相比而言索提液发生源系统挥发出的二恶英更多更稳定,但其挥发量受温度和注射速度的影响较大:当注射速度为1μL.min-1时,在300℃、400℃、500℃三个不同温度段分别为2.78%、7.88%和9.56%;当温度为500℃,注射速度为0.2 mL.min-1时,其挥发率提高到48.7%.研究还发现,注射针头与管壁的残余量是影响挥发效率的两个重要因素,当温度为500℃,载气为1000 mL.min-1,注射速度为0.2 mL.min-1时,连续进样1 h后,两者的残余量分别占注射总量的40.0%和16.7%.  相似文献   

13.
Calcium-based sorbents are widely employed to reduce the acidic gases emission from combustion processes, and also have effects on trace organic pollutants formation and emission. Batch experiments were conducted to investigate the effects of calcium-based sorbents on pentachlorophenol (PCP) forming PCDDs/Fs during high temperature combustion processes. The results indicated that highly chlorinated PCDD/F homologues were the predominant dioxin products from PCP thermo decomposition, and only minor increasing of PCDDs happened when Ca/Cl ratio was lower than 1, while a major jump occurred when Ca/Cl ratio increased from 1 to 2. The CaO addition clearly promoted the production of all chlorinated dibenzo-p-dioxins homologue and 4-7DFs homologue. Comparison of total PCDD/F emission and its I-TEQ for three different calcium-based sorbents addition (CaO, CaCO3, basic fly ash) indicated that CaO and fly ash containing CaO had almost the same promotion effects on PCDDs/Fs originated from PCP, while CaCO3 inhibit PCDD/F formation greatly with inhibition efficiency up to 70%. Such effects may be partly proved by the observed clearly different micro-surface structures of their reaction residues. The mechanism of CaO on condensation and dechlorination reactions for PCP forming PCDDs and acid-base interaction were proposed to speculate the promotion effects of CaO, and the reaction precedence was used to speculate the inhibition effects of CaCO3 on PCDDs/Fs originated from PCP. The results of the present paper might be useful for the industrial application of calcium-based sorbents to control PCDD/F emission.  相似文献   

14.
The gasification behavior of polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) in fly ash by thermal treatment has been investigated to estimate gas-particle partition in flue gas. The results obtained in thermal experiments under various conditions showed that gasification of PCDD/Fs depends on air flow rate and treatment weight of fly ash as well as treatment temperature. On the other hand, the results obtained in the thermal experiments using dioxin-free fly ash revealed that during thermal treatment, the de novo synthesis, gasification, and decomposition of PCDFs proceeded at different rates. This difference in the reaction rates indicates that thermal treatment time is also a factor in determining the gas-particle partition of PCDD/Fs in fly ash. Therefore, reasonable thermal treatment conditions were established and applied to three ash samples. For all samples, PCDD/Fs started to gasify at 350 degrees C treatment, whereas 53-98% of PCDD/F homologs gasified at 400 degrees C treatment, implying that gaseous PCDD/Fs are dominant in flue gas at temperatures in the range 350-400 degrees C regardless of particle concentration.  相似文献   

15.
For an accurate determination of the gas-particle partition of polychlorinated dibenzo-p-dioxins (PCDDs), dibenzofurans (PCDFs) and dioxin-like biphenyls (DLPCBs) in dust-rich flue gas, a parallel monitoring procedure with an isokinetic and a non-isokinetic train was used. For four flue gas samples, the two trains gave a significantly different weight of the collected fly ash particles despite the equal gas volume sampled. On the basis of the quantitative values of PCDD/F and DLPCB homologues and the weight of the collected particles, ratios of each homologue in the real flue gas samples in gaseous form were predicted using simultaneous equations. For the four flue gas samples examined, the predicted gaseous ratios were considerably higher that those calculated using a previously reported equation, suggesting that there are some properties which affect partitions of PCDD/Fs in flue gas besides their saturation vapor pressures and fly ash concentration. The partitions for higher temperature flue gases obtained by fractional determinations of each collection device were additionally different from those predicted by the parallel collection, indicating that conventional determination by fractional measurements is subjected to large errors in dust-rich flue gas due to severe adsorption of gaseous PCDD/Fs and DLPCBs onto particles collected on a low-temperature collection device.  相似文献   

16.
This paper deals with the optimization of accelerated solvent extraction (ASE) for the analysis of the polychlorinated dibenzo-p-dioxins, benzo-p-furans (PCDD/Fs), mixed bromine/chlorine-dibenzo-p-dioxins, and benzo-p-furans (so-called MXDD/Fs) in solid samples. Previous theoretical studies have shown that these compounds exhibit similar electronic properties. It is reasonable to assume that there is little difference in the behavior, formation, and toxicity of PCDD/Fs and MXDD/Fs. Indeed, for most of the cases, the affinity is defined by these weak interactions. Only eight native standards are available for the MXDD/Fs; hence, the use of similar compounds (native and (13)C(12)-labeled), such as PCDD/Fs, is required to optimize and to validate experimental methods. This would allow conclusions to be applied for the MXDD/Fs without extended studies involving complex synthesis methods. Experimental design methodology was used to evaluate the influence of five parameters (temperature, pressure, static time, number of cycles, and solvent nature) on the polyhalogenated dibenzodioxin and -furan (PXDD/Fs) extractions in different materials. The extraction profiles and the optimal operating conditions were determined for each matrix from the modeling of extraction performance. The two following effects, the relative peak area and the co-extracted matrix (CEM), were screened in this study. The temperature of extraction was found to be the most important parameter. ASE offers automation and appears to be as efficient as Soxhlet or Soxtet; however, a major benefit was that a 4-fold decrease in extraction time was obtained. Results suggest that extraction efficiency was quantitative with extraction times as low as 15 min for all congeners at 130 degrees C with a mixed solvent (n-hexane/acetone (1/1)). Under these operating conditions, the CEM and the degradation of the highly brominated compounds were minimized. The analysis of some real life samples from municipal solid waste incinerators showed significant amounts of PXDD/Fs.  相似文献   

17.
Medical waste (MW) ashes from different types of MW incinerators were examined to detect the characteristics and environmental impact of rare earth elements (REEs). The results showed that total REE contents in the ash samples ranged from 10.2 to 78.9mg/kg. REEs in bottom ash were apparently higher than those in fly ash. Average REE contents in the ashes followed the sequence of Ce>La>Nd>Y>Gd>Pr>Sm>Dy>Er>Yb>Ho>Eu>Tb>Lu>Tm. Some of the elements, such as Sm, Dy, Ho, Er, Yb in the ash samples were in normal or nearly normal distribution, but Y, La, Ce, Pr, Nd, Eu, Gd, Tb, Tm, Lu were not normally distributed, indicating some of the ash samples were enriched with these elements. Crust-normalized REE patterns indicated that two types of the MW ashes were obviously enriched with Gd and La. Sequential extraction results showed that REEs in the ash mainly presented as residual fraction, while exchangeable and carbonate fractions were relatively low. DTPA- and EDTA-extraction tests indicated that REEs in the MW ashes were generally in low bioavailability.  相似文献   

18.
Concentrations of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in water and suspended particulate matter (SPM) collected from the Xijiang River, China, were measured by the quarter from September 2005 to June 2006. Total PCDD/F concentration ranged from 2.659 to 4.596pg/L for water and from 562.4 to 3259.5pg/g for SPM. Concentrations were high in summer and low in winter. I-TEQ values in water and SPM were low, ranging from 0.012 to 0.075pg/L, with a mean value of 0.039pg/L. Calculated annual loadings of total PCDD/Fs and I-TEQ were 8.55kg and 0.026kg, respectively. Composition and homologue distribution of PCDD/Fs were varied because of large seasonal differences in discharge from the Xijiang River into the South China Sea. Comparison of the PCDD/Fs homologue and congener profiles of atmospheric deposition, soil, and water revealed that soil was the dominant source of PCDD/Fs in the Xijiang River. Industrial effluents were also possible sources of PCDD/Fs. A good correlation between logK(oc) and logK(ow) was observed for 2,3,7,8-substituted PCDDs and PCDFs and correlation coefficients were 0.71 and 0.84, indicating organic matter in SPM played a dominant role in PCDD/Fs partition between SPM and water.  相似文献   

19.
The concentrations of 17PCDD/F congeners as well as tetra- to octa-homologues were determined in 33 soil samples collected within a radius of 7 km from a municipal solid waste (MSW) incineration plant that is equipped with three fluidized bed incinerators (FBIs) of co-firing MSW with coal in Hangzhou, China. The total PCDD/F concentrations ranged from 0.39 to 5.04 pg I-TEQ g(-1) (54-285 pg g(-1)), with an average and a median value of 1.22 and 0.84 pg I-TEQ g(-1) (105 and 86 pg g(-1)), respectively. A systematic decrease of PCDD/F levels was observed with the increasing distances and with the decreasing downwind frequencies from the plant. The comparisons of homologue and congener patterns and multivariate analysis of soil and flue gas samples strongly indicated that most of the soil samples were influenced by the FBIs. Apart from the incineration plant, historical PCDD/F emissions of hazardous waste incinerator (HWI) and motor vehicles as well as the application of 1,3,5-trichloro-2-(4-nitrophenoxy) benzene (CNP) seemed to play an important role in soil samples adjacent to these potential sources.  相似文献   

20.
In order to understand the effect of different amounts of powder-activated carbon (PAC) injection and bio-solution (NOE-7F) addition on the removal efficiencies of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in a fly ash treatment plant with Waelz rotary kiln process, the PCDD/F concentrations in the stack flue gasses were measured and discussed. In the amount of 20, 40 and 50 kg/h PAC injection, the removal efficiencies of PCDD/Fs in the stack flue gas were 86, 96 and 97%, respectively. While adding more amounts of PAC did enhance the removal efficiencies, the reduction fractions of low chlorinated PCDD/F congeners were much higher than those of highly chlorinated PCDD/F congeners. Particularly, a lower amount of PAC injection (20 kg/h), not only cannot remove highly chlorinated PCDD/Fs, but also the carbon surface of the PAC can act as a precursor for the formation promotion of highly chlorinated PCDD/F congeners. The addition of NOE-7F in the raw materials had the dechlorination effect on the PCDD/F removal and mainly inhibited highly chlorinated PCDD/F formation. The combination of both PAC injection and NOE-7F addition has a high potential for practical application.  相似文献   

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