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1.
Aerosol particulates are generated by coal combustion. The amount and properties of aerosol particulates, specifically size distribution and composition, can be affected by combustion conditions. Understanding the formation of these particles is important for predicting emissions and understanding potential deposition. Oxy-fuel combustion conditions utilize an oxygen-enriched gas environment with CO(2). The high concentration of CO(2) is a result of recycle flue gas which is used to maintain temperature. A hypothesis is that high CO(2) concentration reduces the vaporization of refractory oxides from combustion. A high-temperature drop-tube furnace was used under different oxygen concentrations and CO(2) versus N(2) to study the effects of furnace temperature, coal type, and gas phase conditions on particulate formation. A scanning mobility particle sizer (SMPS) and aerodynamic particle sizer (APS) were utilized for particle size distributions ranging from 14.3 nm to 20 μm. In addition, particles were collected on a Berner low pressure impactor (BLPI) for elemental analysis using scanning electron microscopy and energy dispersive spectroscopy. Three particle size modes were seen: ultrafine (below 0.1 μm), fine (0.1 to 1.0 μm), and coarse (above 1 μm). Ultrafine mass concentrations were directly related to estimated particle temperature, increasing with increasing temperature. For high silicon and calcium coals, Utah Skyline and PRB, there was a secondary effect due to CO(2) and the hypothesized reaction. Illinois #6, a high sulfur coal, had the highest amount of ultrafine mass and most of the sulfur was concentrated in the ultrafine and fine modes. Fine and coarse mode mass concentrations did not show a temperature or CO(2) relationship. (The table of contents graphic and abstract graphic are adapted from ref 27.).  相似文献   

2.
Arsenic and selenium compounds may be emitted to the environment during coal conversion processes, although some compounds are retained in the fly ashes, in different proportions depending on the characteristics of the ashes and process conditions. The possibility of optimizing the conditions to achieve better trace element retention appears to be an attractive, economical option for reducing toxic emissions. This approach requires a good knowledge of fly ash characteristics and a thorough understanding of the capture mechanism involved in the retention. In this work the ability of two fly ashes, one produced in pulverized coal combustion and the other in fluidized bed combustion, to retain arsenic and selenium compounds from the gas phase in coal combustion and coal gasification atmospheres was investigated. To explore the possible simultaneous retention of mercury, the influence of the unburned coal particle content was also evaluated. Retention capacities between 2 and 22 mg g(-1) were obtained under different conditions. The unburned coal particle content in the fly ash samples does not significantly modify retention capacities.  相似文献   

3.
X-ray absorption fine structure spectroscopy has been used to determine directly the oxidation states and speciation of selenium and arsenic in 10 fly ash samples collected from full-scale utility plants. Such information is needed to assess the health risk posed by these elements in fly ash and to understand their behavior during combustion and in fly ash disposal options, such as sequestration in tailings ponds. Selenium is found predominantly as Se(IV) in selenite (SeO3(2-)) species, whereas arsenic is found predominantly as As(V) in arsenate (AsO4(3-)) species. Two distinct types of selenite and arsenate spectra were observed depending upon whether the fly ash was derived from eastern U.S. bituminous (Fe-rich) coals or from western subbituminous or lignite (Ca-rich) coals. Similar spectral details were observed for both arsenic and selenium in the two different types of fly ash, suggesting that the postcombustion behavior and capture of both of these elements are likely controlled by the same dominant element or phase in each type of fly ash.  相似文献   

4.
Ultrafine (<100 nm) ash particles in three coal fly ashes (CFA) produced by the combustion of three U.S. coals have been examined by high-resolution transmission electron microscopy (HRTEM), energy-dispersive X-ray spectroscopy (EDS), and electron diffraction. These ultrafine particles, either as primary ash particles derived directly from coal minerals or as secondary products of decomposition and vaporization-condensation processes, show quite different morphologies, compositions, and microstructures as compared to particles in coarser, micrometer-size fractions previously examined by CCSEM. An eastern U.S. bituminous CFA sample shows abundant discrete crystalline particles rich in Fe, Ti, and Al in its ultrafine ash fraction, and crystalline phases down to 10 nm size have been identified. Western U.S. low-rank CFA samples contain considerable amounts of alkaline-earth element aggregates in the form of phosphates, silicates, and sulfates and mixed species. Most of them show crystalline or crystalline plus amorphous characteristics. All three ultrafine samples also exhibit carbonaceous particles in the form of soot aggregates with primary particle size typically between 20 and 50 nm. In the western low-rank ultrafine CFAs, these carbonaceous soot particles were typically mixed or coated with multi-element inorganic species.  相似文献   

5.
Volatile arsenic and selenium compounds present in coals may cause environmental problems during coal combustion and gasification. A possible way to avoid such problems may be the use of solid sorbents capable of retaining these elements from flue gases in gas cleaning systems. Lime and limestone are materials that are extensively employed for the capture of sulfur during coal processing. Moreover, they have also proven to have good retention characteristics for arsenic and selenium during combustion. The aim of this work was to ascertain whether this sorbent is also useful for retaining arsenic and selenium species in gases produced in coal gasification. The study was carried out in a laboratory-scale reactor in which the sorbent was employed as a fixed bed, using synthetic gas mixtures. In these conditions, retention capacities for arsenic may reach 17 mg g(-1) in a gasification atmosphere free of H2S, whereas the presence of H2S implies a significant decrease in arsenic retention. In the case of selenium, H2S does not influence retention which may reach 65 mg g(-1). Post-retention sorbent characterization, thermal stability, and water solubility tests have shown that chemical reaction is one of the mechanisms responsible for the capture of arsenic and selenium, with Ca(AsO2)2 and CaSe being the main compounds formed.  相似文献   

6.
In several recent studies it was shown that high atmospheric loads of submicrometer particles in the size range below 500 nm have strong impact on human health. Therefore, extensive research concerning the reduction of fine particle emissions is needed to further improve air quality. Regarding health effects, especially the emission characteristics of fine and ultrafine particles emerging from anthropogenic sources such as combustion processes are of special interest. This study shows that the emission characteristic of an electrostatic precipitator (ESP) due to re-entrainment of fine particles and their subsequent release into the atmosphere can be significantly lowered by application of different operating conditions. For this purpose the particle collection efficiency of an ESP was studied in a municipal sewage sludge incineration plant. Particles were sampled under different operating conditions upstream and downstream from the ESP, and the particle number concentrations were measured simultaneously with aerodynamic particle sizers. In addition, the size distribution of the particles downstream from the ESP was measured with high time resolution by an electrical low-pressure impactor to investigate the particle re-entrainment into the flue gas. To determine the influence of operating conditions, different rapping cycles were investigated regarding their impact on the collection efficiency and the subsequent particle re-entrainment.  相似文献   

7.
In light of Title I of the Clean Air Act Amendments of 1990, selenium will most probably be considered for regulation in the electric power industry. This has generated interest for removing this element from fossil-fired flue gas. This study deals with coal combustion: selenium volatilization and its speciation in the cooled flue gas were investigated to better understand its chemical behavior to validate the thermodynamic approach to such complex systems and to begin developing emission control strategies. Se volatility is influenced by several factors such as temperature, residence time, fuel type, particle size, and Se speciation of the fuels, as well as the forms of the Se inthe spiked coal/coke. Spiked coke and coal samples were burned in a thermobalance, and atomic Se and its dioxide were identified in the cooled combustion flue gas by X-ray photoelectron spectroscopy (XPS). A thermodynamic calculation was applied to a complex system including 54 elements and 3,200 species that describes the coal combustion. Several theoretical predictions concerning Se behavior, such as its speciation in flue gas, agreed well with experiments, which supports using thermodynamics for predicting trace element chemistry in combustion systems.  相似文献   

8.
In this study, an axial flow cyclone was designed, fabricated, and evaluated at different conditions of air flow rates (Q0) and low-pressure environments (P), especially for the segregation and collection of ultrafine particles. An evaporation/condensation type of aerosol generation system consisting of tube furnace and mixing chamber was employed to produce test aerosols. The test aerosol was then classified by a differential mobility analyzer (DMA) and number concentration was measured by a condensation nuclei counter (CNC) and an electrometer upstream and downstream of the cyclone, respectively. The s-shaped curve of the collection efficiency in submicron particle size range was obtained to be similar to the traditional cyclone found in the literatures when the particles were largerthan 40 nm at Q0 = 1.07, 0.455 L(STP)/min, and P = 4.8-500 Torr. The curve was found to be fitted very well by a semiempirical equation described in this paper. For particles smaller than 40 nm, however, the collection efficiency was unusually increased as the particle diameter was decreased due to the fact that the diffusion deposition becomes the dominant collection mechanism in the low-pressure conditions. A model composed of centrifugal force and diffusion deposition is presented and used to fit the experimental data. The cyclone was demonstrated to separate and collect ultrafine particles effectively in the tested vacuum conditions.  相似文献   

9.
Emission factors of carbonaceous particles, including black carbon (BC) and organic carbon (OC), and polycyclic aromatic hydrocarbons (PAHs) were determined for five coals, which ranged in maturity from sub-bituminous to anthracite. They were burned in the form of honeycomb briquettes in a residential coalstove, one of the most common fuel/stove combinations in China. Smoke samples were taken through dilution sampling equipment, with a high volume sampler that could simultaneously collect emissions in both particulate and gaseous phases, and a cascade impactor that could segregate particles into six fractions. Particulate BC and OC were analyzed by a thermal-optical method, and PAHs in emissions of both phases were analyzed by GC-MS. Burning of bituminous coals produced the highest emission factors of particulate matter (12.91 g/kg), BC (0.28 g/kg), OC (7.82 g/kg), and 20 PAHs (210.6 mg/kg) on the basis of burned dry ash-free (daf) coal, while the anthracite honeycomb-briquette was the cleanest household coal fuel. The size-segregated results show that more than 94% of the particles were submicron, and calculated mass median aerodynamic diameters (MMAD) of all particles were under 0.3 microm. Based on the coal consumption in the residential sector of China, 290.24 Gg (gigagrams) of particulate matter, 5.36 Gg of BC, 170.33 Gg of OC, and 4.72 Gg of 20 PAHs mass were emitted annually from household honeycomb-briquette burning during 2000. Anthracite coal should be selected preferentially and more advanced burning conditions should be applied in domestic combustion, from the viewpoint of both climate change and adverse health effects.  相似文献   

10.
Beside major pollutants (particulates, carbon, sulfur, and nitrogen oxides), coal combustion generates emissions of potentially toxic trace elements. The current work focuses on predicting the fate of eight trace elements (As, Cd, Hg, Ni, Pb, Se, V, and Zn) in power stations that fire pulverized coal and are equipped with flue gas scrubbers. The core of the study is global equilibrium analysis carried out with the aid of three extensive databases. The first set of equilibrium constants describes conditions prevailing in the furnace and the flue gas duct, while the second set describes reactions in the flue gas scrubber. Melting behavior of ash and solubility of trace elements within the slag are described as a third set of data. To test the modeling approach taken in this paper, the predicted overall partitioning of trace elements is compared with measured data from two full-scale facilities. The results of the study indicate that As, Cd, Ni, Pb, V, and Zn are captured in the fly ash, and that the fate of these element correlates with the overall particle capture of the power plants. Calculations for the flue gas scrubber facilities show that nonvolatile trace elements are likely to dissolve in the scrubber solution, and that capture of these elements likewise is correlated with the overall particulate behavior. Theoretical predictions of the melting behavior indicate that As, Ni, Zn, and to some extent Pb are likely to dissolve in the molten ash.  相似文献   

11.
An 18 month investigation of the environmental impacts of the Tennessee Valley Authority (TVA) coal ash spill in Kingston, Tennessee combined with leaching experiments on the spilled TVA coal ash have revealed that leachable coal ash contaminants (LCACs), particularly arsenic, selenium, boron, strontium, and barium, have different effects on the quality of impacted environments. While LCACs levels in the downstream river water are relatively low and below the EPA drinking water and ecological thresholds, elevated levels were found in surface water with restricted water exchange and in pore water extracted from the river sediments downstream from the spill. The high concentration of arsenic (up to 2000 μg/L) is associated with some degree of anoxic conditions and predominance of the reduced arsenic species (arsenite) in the pore waters. Laboratory leaching simulations show that the pH and ash/water ratio control the LCACs' abundance and geochemical composition of the impacted water. These results have important implications for the prediction of the fate and migration of LCACs in the environment, particularly for the storage of coal combustion residues (CCRs) in holding ponds and landfills, and any potential CCRs effluents leakage into lakes, rivers, and other aquatic systems.  相似文献   

12.
Sulfur dioxide (SO2) and trace elements are all pollutants derived from coal combustion. This study relates to the simultaneous removal of SO2 and trace selenium dioxide (SeO2) from flue gas by calcium oxide (CaO) adsorption in the moderate temperature range, especially the effect of SO2 presence on selenium capture. Experiments performed on a thermogravimetric analyzer (TGA) can reach the following conclusions. When the CaO conversion is relatively low and the reaction rate is controlled by chemical kinetics, the SO2 presence does not affect the selenium capture. When the CaO conversion is very high and the reaction rate is controlled by product layer diffusion, the SO2 presence and the product layer diffusion resistance jointly reduce the selenium capture. On the basis of the kinetics study, a method to estimate the trace selenium removal efficiency using kinetic parameters and the sulfur removal efficiency is developed.  相似文献   

13.
Aged and weathered chromated copper arsenate (CCA) treated wood was burned in an open burn research facility to characterize the air emissions and residual ash. The objectives were to simulate, to the extent possible, the combustion of such waste wood as might occur in an open field or someone's backyard; to characterize the composition and particle size distribution (PSD) of the emitted fly ash; to determine the partitioning of arsenic, chromium, and copper between the fly ash and residual ash; and to examine the speciation of the CCA elements. This work reports preliminary air emission concentrations and estimated emission factors for total particulate matter, arsenic (As), chromium (Cr), copper (Cu), and polychlorinated dibenzodioxins/dibenzofurans (PCDD/F) totals and toxic equivalents (TEQs). The partitioning of As, Cr, and Cu between the emitted fly ash and residual ash is examined and thermochemical predictions from the literature are used to explain the observed behavior. Results indicate a unimodal fly ash PSD between 0.1 and 1.0 microm diameter. In addition to a large carbonaceous component, between 11 and 14% of the As present in the burned CCA treated wood was emitted with the air emissions, with the remainder present in the residual ash. In contrast, less than 1% of both the Cr and Cu present in the wood was emitted with the air emissions. PCDD/F levels were unremarkable, averaging 1.7 ng TEQ/kg of treated wood burned, a value typical for wood combustion. Scanning electron microscopy (SEM) was unable to resolve inorganic particles consisting of Cu, Cr, or As in the wood samples, but X-ray absorption fine structure (XAFS) spectroscopy confirmed that the oxidation states of the CCA elements in the wood were Cu2+, Cr3+, and As5+. SEM examination of the fly ash samples revealed some inorganic microcrystals within the mostly carbonaceous fly ash, while XAFS spectroscopy of the same samples showed that the oxidation states after combustion were mixed Cu+ and Cu2+, Cr3+, and mixed As3+ and As5+. Estimates of the ratios of the mixed oxidation states based on the XAFS spectra were As3+/(total As) = 0.8-0.9 and Cu+/(total Cu) = 0.65-0.7. The Cu and Cr present in the fly ash were determined to coexist predominantly in the two oxide phases CuCrO2 and CuCr2O4. These results indicate that the open burning of CCA-treated wood can lead to significant air emissions of the more toxic trivalent form of As in particle sizes that are most respirable.  相似文献   

14.
The E.U. Directive on incineration of waste regulates the harmful emissions of particles and twelve toxic elements, including copper, chromium, and arsenic. More information is critically needed on the speciation and behavior of these trace elements during combustion, including the effects of different process variables, as well as of different fuels and fuel mixtures. Using a 15 kW pellets-fueled grate burner, experiments were performed to determine the fate of copper, chromium, and arsenic during combustion of chromate copper arsenate (CCA) preservative wood. The effects of co-combustion of CCA-wood with peat were also studied since peat fuels previously have proved to generally reduce ash related problems. The fate and speciation of copper, chromium, and arsenic were determined from analysis of the flue gas particles and the bottom ash using SEM-EDS, XRD, XPS, and ICP-AES. In addition, chemical equilibrium model calculations were performed to interpret the experimental findings. The results revealed that about 5% copper, 15% chromium, and 60% arsenic were volatilized during combustion of pure CCA-wood, which is lower than predicted volatilization from the individual arsenic, chromium, and copper oxides. This is explained by the formation of more stable refractory complex oxide phases for which the stability trends and patterns are presented. When co-combusted with peat, an additional stabilization of these phases was obtained and thus a small but noteworthy decrease in volatilization of all three elements was observed. The major identified phases for all fuels were CuCrO2(s), (Fe, Mg, Cu)(Cr, Fe, Al)04(s), Cr2O3(s), and Ca3(AsO4)2(s). Arsenic was also identified in the fine particles as KH2AsO4(s) and As2O3(s). A strong indication of hexavalent chromium in the form of K2CrO4 or as a solid solution between K3Na(CrO4)2 and K3Na(SO4)2 was found in the fine particles. Good qualitative agreement was observed between experimental data and chemical equilibrium model calculations.  相似文献   

15.
Polycyclic aromatic hydrocarbons (PAHs) in manufactured gas plant (MGP) site sediments are often associated with carbonaceous particles that reduce contaminant bioavailability. Although black carbon inclusive partitioning models have been proposed to describe elevated PAH partitioning behavior, questions remain on the true loading and association of PAHs in different particle types in industrially impacted sediments. In the studied MGP sediments, the light density organic particles (coal, coke, wood, and coal tar pitch) comprised 10-20% of the total mass and 70-95% of the PAHs. The remainder of the PAHs in sediment was associated with the heavy density particles (i.e., sand, silt, and clays). Among the different particle types, coal tar pitch (quantified by a quinoline extraction method) contributed the most to the bulk sediment PAH concentration. Aqueous partition coefficients for PAHs measured using a weathered pitch sample from the field were generally an order of magnitude higher than reported for natural organic matter partitioning, and match well with theoretical predictions based on a coal tar-water partitioning model. A pitch-partitioning inclusive model is proposed that gives better estimates of the measured site-specific PAH aqueous equilibrium values than standard estimation based on natural organic matter partitioning only. Thus, for MGP impacted sediments containing weathered pitch particles, the partitioning behavior may be dominated by the sorption characteristics of pitch and not by natural organic matter or black carbon.  相似文献   

16.
Polycyclic aromatic hydrocarbons (PAHs) bound in nano/ ultrafine particles from vehicle emissions may cause adverse health effects. However, little is known about the characteristics of the nanoparticle-bound PAHs and the PAH-associated carcinogenic potency/cytotoxicity; therefore, traffic-related nano/ultrafine particles were collected in this study using a microorifice uniform deposition impactor(MOUDI) and a nano-MOUDI. For PM0.056--18, the difference in size-distribution of particulate total-PAHs between non-after-rain and after-rain samples was statistically significant at alpha = 0.05; however, this difference was not significant for PM0.01--0.056. The PAH correlation between PM0.01--0.1 and PM0.1--1.8 was lower for the after-rain samples than forthe non-after-rain samples. The average particulate total-PAHs in five samplings displayed a trimodal distribution with a major peak in the Aitken mode (0.032--0.056 microm). About half of the particulate total-PAHs were in the ultrafine size range. The BaPeq sums of BaP, IND, and DBA (with toxic equivalence factors > or = 0.1) accounted for approximately 90% of the total-BaPeq in the nano/ultrafine particles, although these three compounds contributed little to the mass of the sampled particles. The mean content of the particle-bound total-PAHs/-BaPeqs and the PAH/BaPeq-derived carcinogenic potency followed the order nano > ultrafine > fine > coarse. For a sunny day sample, the cytotoxicity of particle extracts (using 1:1 (v/v) n-hexane/dichloromethane) was significantly higher (p < 0.05) for the nano (particularly the 10-18 nm)/ultrafine particles than for the coarser particles and bleomycin. Therefore, traffic-related nano and ultrafine particles are possibly cytotoxic.  相似文献   

17.
This study reports on the first complex data set of emission factors (EFs) of selected pollutants from combustion of five fuel types (lignite, bituminous coal, spruce, beech, and maize) in six different domestic heating appliances of various combustion designs. The effect of fuel as well as the effect of boiler type was studied. In total, 46 combustion runs were performed, during which numerous EFs were measured, including the EFs of particulate matter (PM), carbon monoxide, polyaromatic hydrocarbons (PAH), hexachlorobenzene (HxCBz), polychlorinated dibenzo-p-dioxins and furans (PCDD/F), etc. The highest EFs of nonchlorinated pollutants were measured for old-type boilers with over-fire and under-fire designs and with manual stoking and natural draft. Emissions of the above-mentioned pollutants from modern-type boilers (automatic, downdraft) were 10 times lower or more. The decisive factor for emission rate of nonchlorinated pollutants was the type of appliance; the type of fuel plays only a minor role. Emissions of chlorinated pollutants were proportional mainly to the chlorine content in fuel, but the type of appliance also influenced the rate of emissions significantly. Surprisingly, higher EFs of PCDD/F from combustion of chlorinated bituminous coal were observed for modern-type boilers (downdraft, automatic) than for old-type ones. On the other hand, when bituminous coal was burned, higher emissions of HxCBz were found for old-type boilers than for modern-type ones.  相似文献   

18.
Ionization air purifiers are increasingly used to remove aerosol particles from indoor air. However, certain ionization air purifiers also emit ozone. Reactions between the emitted ozone and unsaturated volatile organic compounds (VOC) commonly found in indoor air produce additional respirable aerosol particles in the ultrafine (<0.1 microm) and fine (<2.5 microm) size domains. A simple kinetic model is used to analyze the competition between the removal and generation of particulate matter by ionization air purifiers under conditions of a typical residential building. This model predicts that certain widely used ionization air purifiers may actually increase the mass concentration of fine and ultrafine particulates in the presence of common unsaturated VOC, such as limonene contained in many household cleaning products. This prediction is supported by an explicit observation of ultrafine particle nucleation events caused by the addition of D-limonene to a ventilated office room equipped with a common ionization air purifier.  相似文献   

19.
Coal bed natural gas (CBNG) produced water is usually disposed into nearby constructed disposal ponds. Geochemistry of produced water, particularly trace elements interacting with a semiarid environment, is not clearly understood. The objective of this study was to collect produced water samples at outfalls and corresponding disposal ponds and monitor pH, iron (Fe), aluminum (Al), chromium (Cr), manganese (Mn), lead (Pb), copper (Cu), zinc (Zn), arsenic (As), boron (B), selenium (Se), molybdenum (Mo), cadmium (Cd), and barium (Ba). Outfalls and corresponding disposal ponds were sampled from five different watersheds including Cheyenne River (CHR), Belle Fourche River (BFR), Little Powder River (LPR), Powder River (PR), and Tongue River (TR) within the Powder River Basin (PRB), Wyoming from 2003 to 2005. Paired t tests were conducted between CBNG outfalls and corresponding disposal ponds for each watershed. Results suggest that produced water from CBNG outfalls is chemically different from the produced water from corresponding disposal ponds. Most trace metal concentrations in the produced water increased from outfall to disposal pond except for Ba. In disposal ponds, Ba, As, and B concentrations increased from 2003 to 2005. Geochemical modeling predicted precipitation and dissolution reactions as controlling processes for Al, Cu, and Ba concentrations in CBNG produced water. Adsorption and desorption reactions appear to control As, Mo, and B concentrations in CBNG water in disposal ponds. Overall, results of this study will be important to determine beneficial uses (e.g., irrigation, livestock/wildlife water, and aquatic life) for CBNG produced water in the PRB, Wyoming.  相似文献   

20.
Sulfur dioxide (SO2) and trace elements are pollutants derived from coal combustion. This study focuses on the simultaneous removal of S02 and trace arsenic oxide (As2O3) from flue gas by calcium oxide (CaO) adsorption in the moderate temperature range. Experiments have been performed on a thermogravimetric analyzer (TGA). The interaction mechanism between As2O3 and CaO is studied via XRD detection. Calcium arsenate [Ca3(AsO4)2] is found to be the reaction product in the range of 600-1000 degrees C. The ability of CaO to absorb As2O3 increases with the increasing temperature over the range of 400-1000 degrees C. Through kinetics analysis, it has been found that the rate constant of arsenate reaction is much higher than that of sulfate reaction. SO2 presence does not affect the trace arsenic capture either in the initial reaction stage when CaO conversion is relatively low or in the later stage when CaO conversion is very high. The product of sulfate reaction, CaS04, is proven to be able to absorb As2O3. The coexisting CO2 does not weaken the trace arsenic capture either.  相似文献   

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