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1.
用低浓度SO2诱导驯化方法获得高效脱硫菌群,并用分离培养与16S rRNA基因测序技术相结合的方法鉴定菌群种属,分析驯化过程中种群结构的动态变化,同时研究分离纯菌种的脱硫性能。结果表明,从诱导驯化7 d和14 d菌液中分别分离出23株菌和22株菌,16S rRNA序列分析发现这些菌归属于13个种,其中有6个种(Rhodococcus erythropolis、Pseudomonas putida、Microbacterium oxydans、Sphingomonas koreensis、Acinetobacter junii、Acinetobacter johnsonii)对SO2-3有较强的降解能力,并在持续驯化过程中稳定的生长传代,降解产物以硫酸根为主,还有极少量的单质硫。与含混合菌的驯化菌液降解SO2-3的能力相比,单一脱硫菌的脱硫性能较弱。脱硫功能菌株及其基本特性的研究为微生物处理SO2烟气提供了丰富的菌源信息和理论基础。  相似文献   

2.
A year-long field study to characterize the ionic species in PM2.5 was carried out in Shanghai and Beijing, China, in 1999–2000. Weekly samples of PM2.5 were collected using a special low flow rate (0.4 l min−1) sampler. In Shanghai, SO42− NO3 and NH4+ were the dominant ionic species, which accounted for 46%, 18% and 17% of the total mass of ions, respectively. Local SO2 emissions were an important source of SO42− in PM2.5 because the SO42− concentration was correlated with the SO2 concentration (r=0.66). The relatively stable SO42−/SO2 mass ratio over a large range of temperatures suggests that gas-phase oxidation of SO2 played a minor role in the formation of SO42−. The sum of SO42− and NO3 was highly correlated with NH4+ (r=0.96), but insufficient ammonium was present to totally neutralize the aerosol. In Beijing, SO42−, NO3 and NH4+ were also the dominant ionic species, constituting 44%, 25% and 16% of the total mass of water-soluble ions, respectively. Local SO2 emissions were an important source of SO42− in the winter since SO42− was correlated with SO2 (r=0.83). The low-mass SO42−/SO2 ratio (0.27) during winter, which had low humidity, suggests that gas-phase oxidation of SO2 was a major route of sulfate formation. In the summer, however, much higher mass ratios of SO42−/SO2 (5.6) were observed and were ascribed to in-cloud sulfate formation. The annual average ratio of NO3/SO42− was 0.4 and 0.6 in Shanghai and in Beijing, respectively, suggesting that stationary emissions were still a dominant source in these two cities.  相似文献   

3.
A steady state mesoscale model developed to predict primary SO2 concentrations from a single point source is presented. The model was validated with data from the Midwest Interstate Sulfur Transport and Transformation (MISTT) project, with root mean square errors of 9.69 μg m?3 and 0.42 μg m?3 for SO2 and SO4 respectively. Wet deposition (washout and rainout), eddy dispersivity, dry deposition of SO2 and mean wind speed were found to be the most important factors controlling sulfur dioxide and sulfate concentrations. Estimation of precipitation acidity was then carried out using scavenging theory. The greatest potential acidification occurred approximately 200 km from the source along plume centerllne, which indicates a rather local effect as opposed to a long distance effect. The cross-plume influence was up to 60 km in width at a distance of 400 km from the source.  相似文献   

4.
Sodium hypochlorite (NaClO) has been widely used as a chemical additive for enhancing nitrogen oxide (NOx; NO + NO2), sulfur dioxide (SO2), and mercury (Hg0) removals in a wet scrubber. However, they are each uniquely dependent on NaClO(aq) pH, hence making the simultaneous control difficult. In order to overcome this weakness, we sprayed low liquid-to-gas (L/G) ratio (0.1 L/Nm3) of NaClO(aq) to vaporize quickly at 165 °C. Results have shown that the maximized NOx, SO2, and Hg0 removals can be achieved at the pH range between 4.0 and 6.0. When NOx and Hg0 coexist with SO2, in addition, their removals are significantly enhanced by reactions with solid and gaseous by-products such as NaClO(s), NaClO2(s), OClO, ClO, and Cl species, originated from the reaction between SO2 and NaClO(aq). We have also demonstrated the feasibility of this approach in the real flue gases of a combustion plant and observed 50%, 80%, and 60% of NOx, SO2, and Hg0 removals, respectively. These findings led us to conclude that the spray of NaClO(aq) at a relatively high temperature at which the sprayed solution can vaporize quickly makes the simultaneous control of NOx, SO2, and Hg0 possible.

Implications: The simple spray of NaClO(aq) at temperatures above 165 °C can cause the simultaneous removal of gaseous NOx, SO2, and Hg0 by its quick vaporization. Their maximized removals are achieved at the pH range between 4.0 and 6.0. NOx and Hg0 removals are also enhanced by gaseous and solid intermediate products generated from the reaction of SO2 with NaClO(aq). The feasibility of this approach has been demonstrated in the real flue gases of a combustion plant.  相似文献   


5.
Abstract

A huge amount of inorganic acids can be produced and emitted with waste gases from integrated circuit manufacturing processes such as cleaning and etching. Emission of inorganic acids from selected semiconductor factories was measured in this study. The sampling of the inorganic acids was based on the porous metal denuders, and samples were then analyzed by ion chromatography. The amount of chemical usage was adopted from the data that were reported to the Environmental Protection Bureau in Hsin-chu County according to the Taiwan Environmental Protection Agency regulation. The emission factor is defined as the emission rate (kg/month) divided by the amount of chemical usage (L/month). Emission factors of three inorganic acids (i.e., hydrofluoric acid [HF], hydrochloric acid [HQ], and sulfuric acid [H2SO4]) were estimated by the same method. The emission factors of HF and HCl were determined to be 0.0075 kg/L (coefficient of variation [CV] = 60.7%, n = 80) and 0.0096 kg/L (CV = 68.2%, n = 91), respectively. Linear regression equations are proposed to fit the data with correlation coefficient square (R2) = 0.82 and 0.9, respectively. The emission factor of H2SO4, which is in the droplet form, was determined to be 0.0016 kg/L (CV = 99.2%, n = 107), and its R2 was 0.84. The emission profiles of gaseous inorganic acids show that HF is the dominant chemical in most of the fabricators.  相似文献   

6.

Efficient abatement of an iodinated X-ray contrast media iohexol by an emerging sulfite autoxidation advanced oxidation process is demonstrated, which is based on transition metal ion–catalyzed autoxidation of sulfite to form active oxidizing species. The efficacy of the combination of sulfite and transition metal ions (Ag(I), Mn(II), Co(II), Fe(II), Cu(II), Fe(III), or Ce(III)) was tested for iohexol abatement. Co(II) and Cu(II) are proven to show more pronounced catalytic activity than other metals at pH 8.0. According to the quenching studies, sulfate radical (SO4??) is identified to be the primary species for oxidation of iohexol. Increasing dosages of metal ion or sulfite and higher pH values are favorable for iohexol abatement. Inhibition of iohexol abatement is observed in the absence of dissolved oxygen, which is vital for the production of SO5?? and subsequent formation of SO4??. Overall, activation of sulfite to produce reactive radicals with extremely low Co(II) or Cu(II) concentrations (in the range of μg L?1) in circumneutral conditions is confirmed, which offers a potential SO4??-based advanced oxidation process in treatment of aquatic organic contaminants.

  相似文献   

7.
The rate constants for reactions of the SO4 radical anion with some low molecular weight monocarboxylic acids (MCAs) and dicarboxylic acids (DCAs) and their anions using the laser flash photolysis-long path laser absorption (LFP-LPLA) technique were determined. The present study contains the first measured rate constants for SO4 reactions with glycolic, lactic, malic and malonic acid. The rate constants are found to be in the range from 105 to 107 M−1 s−1, with the lower values found for acids and higher values for their respective anions. In addition, the rate constants for scavenging of SO4 by all investigated organics in the Mn(II)-catalyzed S(IV) autoxidation at pH 4.5 and T=25 °C were determined by means of the reversed rate method. The comparison between these rate constants and the rate constants obtained by direct measurements confirms the proposed inhibiting mechanism for the Mn(II)-catalyzed S(IV) autoxidation in the presence of monocarboxylic acids. In the case of formic acid, which causes the highest inhibition, this mechanism can explain the second part of kinetic traces (i.e. after the induction period). Surprisingly, although dicarboxylic acids are reactive toward SO4 they do not contribute to the inhibition of S(IV) oxidation (especially malic and malonic acids).  相似文献   

8.
低温选择性催化还原(SCR)脱硝是国内外脱硝技术研发的热点,但目前主要集中在实验室小试范围,无法完全反映催化剂在实际烟气中的运行状况。在30 t/h循环流化床燃煤锅炉脱硫除尘装置后建设了2 000~5 000 m3/h的SCR脱硝中试装置,经系统研究发现,中试使用的蜂窝式催化剂对SO2和NO具有很强的吸附能力,且反应温度、喷氨速率和气体空速均会影响催化脱硝效率。为期5 d的连续运行实验结果表明,催化剂的脱硝效率一直稳定在30%~50%,并未发现明显的失活,这证明设计除雾除尘器、较大的混合器、混合器与反应器间较长的管路均有利于缓解催化剂因SO2、H2O和飞灰中的碱性金属导致的失活。  相似文献   

9.
The microstructure of 1/10 and 1/20 atmosphere, lean H2S—O2—N2 flames is developed using the mass-spectrometric flame-sampling technique. The flame mechanism developed is in agreement with that determined from an earlier study on 1-atm H2S flames. The formation of SO2 appears to be primarily related to the production of SH and the ensuing oxidation steps SH + O2 = SO + OH and SO + O2 = SO2 + O. While there is some question whether SO2 formation occurs via an SO or an S2O intermediate, the present study does not give direct support to the role of S2O in the oxidation mechanism. However, the presence of significant quantities of free sulfur in the pre-flame zone may be indicative of S2O formation via SO + S → S2O, and, possibly, via the disproportionation of SO, 3SO → S2O + SO2. Kinetic analyses of some of the pre-flame reactions indicate an apparent activation energy of 17,300 calories/mole for the decomposition of H2S. The actual initiation process in the flame mechanism requires further examination. The specific rate for the reaction step H2S + O = OH + SH is given by k 6 = 1.45 × 1015 exp ( – 6600/RT) cm3 mole–1 sec–1, and the specific rate for the oxidation of SO, SO + O2 = SO2 + O, is given by k 5 = 5.2 × 1014 exp (—19,300/RT) cm3 mole–1 sec–1.  相似文献   

10.
ABSTRACT

Simultaneous removal of H2S and CS2 was studied with a peat biofilter inoculated with a Thiobacillus strain that oxidizes both compounds in an acidic environment. Both sulfurous gases at concentrations below 600 mg S/m3 were efficiently removed, and the removal efficiencies were similar, 99%, with an empty bed retention time (EBRT) of more than 60 sec. Concentrations greater than 1300-5000 mg S/m3 caused overloading of the filter material, resulting in high H2SO4 production, accumulation of elemental sulfur, and reduced removal efficiency. The highest sulfur removal rate achieved was 4500 g-S/day/m3 filter material. These results indicate that peat is suitable as a biofilter material for the removal of a mixture of H2S and CS2 when concentrations of gases to be purified are low (less than 600 mg/m3), but it is still odorous and toxic to the environment and humans.  相似文献   

11.
This paper reports the results of over 2 years of measurements of several of the species comprising atmospheric SOx (=SO2+SO42−) and NOy (=NO+NO2 + PAN + HNO3+NO3+ organicnitrates + HONO + 2N2O5 …) at Whiteface Mountain, New York. Continuous real-time measurements of SO2 and total gaseous NOy provided data for about 50% and 65% of the period, respectively, and 122 filter pack samples were obtained for HNO3, SO2 and aerosol SO42−, NO3, H+ and NH4+. Concentrations of SO2 and NOy were greatest in winter, whereas concentrations of the reaction products SO42− and HNO3were greatest in summer. The seasonal variation in SO42− was considerably more pronounced than that of HNO3and the high concentrations of SO42− aerosol present in summer were also relatively more acidic than SO42− aerosol in other seasons. As a result, SO42− aerosol was the predominant acidic species present in summer, HNO3was predominant in other seasons. Aerosol NO3 concentrations were low in all seasons and appeared unrelated to simultaneous NOy and HNO3concentrations. These data are consistent with seasonal variations in photochemical oxidation rates and with existing data on seasonal variations in precipitation composition. The results of this study suggest that emission reductions targeted at the summer season might be a cost-effective way to reduce deposition of S species, but would not be similarly cost-effective in reducing deposition of N species. kwAcid deposition, seasonal variation, sulfate, nitrate, nitric acid, sulfur dioxide, oxides of nitrogen, hydrogen peroxide, ozone, air pollution, Adirondack Mountains  相似文献   

12.
Measurements are reported of the chemical composition of the liquid water and interstitial air in warm (> 0°C), non-precipitating stratus and strato-cumulus clouds at various locations in the eastern United States. Inorganic ionic composition of the cloud water was generally dominated by H+, NH4+, NO3 and SO42−, similar to the composition of precipitation in this region of the U.S. Concentrations of the corresponding interstitial aerosol species and gaseous HNO3 were invariably low in comparison to concentrations of the respective ionic species in cloudwater. In contrast, the concentration of NOx (i.e. NO + NO2 + organic nitrates) was invariably comparable to or in excess of that of cloudwater nitrate. Sulfur dioxide was found at varying concentrations relative to cloudwater sulfate. In many cases, the SO2 concentration was quite low (< 0.2 ppb) even in the presence of substantial quantities of cloudwater SO42− (> 1 ppb equivalent gas-phase concentration), suggesting large fractional conversion and incorporation into cloudwater. In other cases, in which dilute SO2 plumes (pso, > 5 ppb) were observed in the cloud interstitial air, the gaseous SO2 concentration substantially exceeded the cloudwater sulfate concentration.Concentrations of H2O2 in cloudwater were found to exhibit strong inverse correlation with interstitial SO2. Appreciable concentrations of SO2 in cloud interstitial air and H2O2 in cloudwater were only rarely observed to coexist, for the most part only one or the other being present above the limit of detection. These observations are consistent with aqueous-phase oxidation of SO2 by H2O2, as has been inferred previously on the basis of laboratory kinetic studies, and with the hypothesis that depending on relative concentrations, either of these species can be a limiting reagent for in-cloud SO2 oxidation. The uptake of NOx as cloudwater nitrate is less complete than the uptake of SO2 as sulfate, and evidence for the occurrence of similar in-cloud processes causing the conversion of NO or NO2 to cloudwater nitrate has not been found.  相似文献   

13.
This paper presents the results of continuous measurements of trace atmospheric gases and aerosol composition made at the summit of Whiteface Mountain, New York, for 28 days in July 1982. The gas phase species NO, NOx ( = NO + NO2 + PAN), HNO3, SO2 and NH3 were measured, as well as aerosol SO42−, NO3, H+ and NH4+. Mean and median NOx concentrations were 1.1 and 1.0 ppb, respectively, with maximum and minimum values of 3.2 and 0.3 ppb. HNO3 concentrations were variable, occasionally exceeding the simultaneously measured NOx levels. Mean and median SO2 were 0.8 and 0.3 ppb, with concentrations up to 12 ppb in pollution episodes. Mean and median NH3 were both 2.2 ppb. Monthly mean SO42− was 5.3 μg m−3, with values in clean air of about 1.5 μg m−3, and in polluted air up to 80 μg m−3. Trajectory calculations indicate that episodes of high pollutant concentrations occur in air masses arriving at Whiteface from the southwest. These episodes contributed most of the SO42−, HNO3 and aerosol acidity, and about half the SO2 and NOx to which the site was exposed during the measurement period. Limited comparisons of air chemistry data with the composition of cloudwater collected during the program are also presented.  相似文献   

14.
A series of iron–manganese oxide catalysts supported on TiO2 and titanium nanotubes (TNTs) were studied for low temperature selective catalytic reduction (SCR) of NO with NH3 in the presence of SO2. The results showed that the specific surface area and the amount of Brønsted acid sites were highly correlated. The results also demonstrated that higher Mn4+/Mn3+ ratios and larger specific surface areas might be the main reasons for the excellent performance of MnFe-TNTs catalyst after SO2 poisoning. The SO2 poisoning effect could be minimized by reducing the GHSV, increasing the reaction temperature, or increasing the [NH3]/[NO] molar ratio. The results also indicated that the formation of ammonium sulfate had a stronger effect on the NO conversion efficiency as compared to the formation of metal sulfate. Thus operating the low temperature SCR at above 230 oC to avoid the formation of ammonium sulfate would be the priority choice when SO2 poisoning is a concerned issue.?Implications: Low-temperature selective catalytic reduction (SCR) has attracted increasing attention due to that it can reduce the energy consumption for the SCR process employed in industries such as steel plants and glass manufacturing plants. However, it also suffers from the sulfur dioxide (SO2) poisoning problem. This study investigates the possibility of using titania nanotubes (TNTs) as the support of Mn/Fe bimetal oxide catalysts for low-temperature SCR to reduce the SO2 poisoning. The results indicated that the MnFe-TNT catalyst can tolerate SO2 for a longer time as compared with the MnFe-TiO2 catalyst.  相似文献   

15.
EN 14791 is a European Standard Reference method for the measurement of SO2 in emissions. This standard is based on a wet-chemical method in which SO2 present in flue gases is absorbed into an absorption solution containing hydrogen peroxide, and analyzed as sulfates after sampling. This study presents the results obtained when three portable automated measuring systems (P-AMS), based on Fourier-transform infrared (FTIR) spectroscopy, non-dispersive infrared (NDIR) and ultraviolet-fluorescence (UV) techniques, were compared to the Standard Reference Method for SO2 (EN 14791) in order to verify whether they could be used as alternative methods (AM) to EN 14791. In the case of FTIR, the measurements were performed from hot and wet gas, without any conditioning. UV-fluorescence analyzers were equipped with dilution probes and one NDIR applied a permeation dryer, whereas the other had a chiller. Tests were carried out at concentration ranges from 0 to 200 mg/m3(n) and from 0 to 800 mg/m3(n) for testing of equivalency according to CEN/TS 14793 using a test bench. Equivalency test criteria were met for all tested P-AMS except for NDIR at the lower range. The SO2 results measured with NDIR and the chiller were lower compared to the set-up with NDIR and permeation. This was most probably due to the chiller causing absorption of SO2 in the condensate. Tests were also carried out at field conditions, measuring the SO2 emissions from a boiler combusting mainly bark. The same phenomena were observed in these tests as during the test bench study, i.e. the measurement set-up with NDIR and the chiller gave the lowest results. These data demonstrated that the tested alternative methods (FTIR, UV-fluorescence, and NDIR) could be used instead of the standard reference method EN 14791, thus providing real-time calibration of automated measuring systems. It must however be emphasized that when measuring water-soluble gases, such as SO2, the choice of suitable conditioning technique is critical in order to minimize losses of the studied component in the condensate.

Implications: Portable automated measuring systems (P-AMS) provide real-time information about emissions and their concentrations, thus offering significant advantages compared to wet-chemical methods. This study presents results which can be used as a validation protocol to show that the tested P-AMS techniques (FTIR, NDIR, UV-fluorescence) could be used instead of EN 14791 (CEN 2017a) as alternative methods (AM), when paying attention to the selection of an appropriate conditioning technique.  相似文献   

16.
A gas monitoring system based on broadband absorption spectroscopic techniques in the ultraviolet region is described and tested. The system was employed in real-time continuous concentration measurements of sulfur dioxide (SO2) and nitric oxide (NO) from a 220-ton h?1 circulating fluidized bed (CFB) boiler in Shandong province, China. The emission coefficients (per kg of coal and per kWh of electricity) and the total emission of the two pollutant gases were evaluated. The measurement results showed that the emission concentrations of SO2 and NO from the CFB boiler fluctuated in the range of 750–1300 mg m?3 and 100–220 mg m?3, respectively. Compared with the specified emission standards of air pollutants from thermal power plants in China, the values were generally higher for SO2 and lower for NO. The relatively high emission concentrations of SO2 were found to mainly depend on the sulfur content of the fuel and the poor desulfurization efficiency. This study indicates that the broadband UV spectroscopy system is suitable for industrial emission monitoring and pollution control.  相似文献   

17.
The techniques of Principal Component Analysis (PCA) and subsequent regression analysis were used in an attempt to describe local and upwind chemical and physical factors which affect the variability of SO4 –2 concentrations observed in a rural area of the northeastern U.S. The data used in the analyses included upwind and local O3 concentrations, temperature, relative humidity and other climatological information, SO2, and meteorological information associated with backward trajectories. The investigation identified five principal components, three major (eigenvalues >1) and two minor (eigenvalues < one), which accounted for 52% (r = 0.72) of the variability in the SO4 –2 regression model. These components can be described as representing local and upwind photochemistry, droplet growth, SO2 emissions, and air mass characteristics. The study also indicated that in future studies it will be necessary to a priori select air pollution and meteorological variables for measurement to potentially increase the sensitivity of this type of receptor model.  相似文献   

18.
SO2/O2 mixtures were photolyzed at 3130 Å and in the range 2500–4000 Å at room temperature. The only product of photolysis was SO3. Attempts to estimate ф(S03) using mass spectrometry, l.R. spectroscopy and pressure change measurements were unsuccessful, because it was not possible to obtain reproducible quantitative estimates of SO3. ф(SO2) values were determined by monitoring the 3130 Å absorption for its concentration measurements. ф(SO2) was independent of SO2 (11.6 to 50.4 torr) and O2 (50.0 to 390.6 torr) pressures. At 3130 Å, ф(SO2) varied between 1.5 × 10?2 and 2.2 X 10?2. Over the integrated range 2500–4000 Å ф(SO2) values of 2.1 X 10?3 to 2.9 X 10?3 were obtained. The differences in ф(SO2) values are explained in terms of wavelength dependence of the rate constants for the two primary reactions: 1SO2 + SO2 → 2SO2(1) and 1SO2 + SO23SO2 + SO2(2); (k2/k1) 3130 Å ≈ 10(k2/k1)2500–4000 Å.  相似文献   

19.
Calibration gas standards for H2S, CH3SH, CS2 and SO2, independently prepared by two separate research groups from the University of Idaho Department of Chemistry and the NOAA Aeronomy Laboratory, were directly intercompared using a gas chromatographic-flame photometric measurement procedure for all four species and a fluorimetric measurement procedure for H2S. The NOAA gas standard system used gravimetrically-calibrated ‘low loss’ permeation tubes in conjunction with a three-stage dynamic dilution system. The University of Idaho (UI) system used single-stage dilution of the effluent from ‘ultra-low loss’ permeation tubes, which were calibrated by a metal foil collection/flash desorption/flame photometric detection procedure using aqueous sulfate standards. Comparative measurements between UI and NOAA gas standards in the 1–2 ppbv range showed differences no greater than 12 % for CS2, SO2 and CH3SH, and 21 % for H2S.  相似文献   

20.
ABSTRACT

We conducted a multi-pollutant exposure study in Baltimore, MD, in which 15 non-smoking older adult subjects (>64 years old) wore a multi-pollutant sampler for 12 days during the summer of 1998 and the winter of 1999. The sampler measured simultaneous 24-hr integrated personal exposures to PM25, PM10, SO4 2-, O3, NO2, SO2, and exhaust-related VOCs.

Results of this study showed that longitudinal associations between ambient PM2.5 concentrations and corresponding personal exposures tended to be high in the summer (median Spearman's r = 0.74) and low in the winter (median Spearman's r = 0.25). Indoor ventilation was an important determinant of personal PM2.5 exposures and resulting personal-ambient associations. Associations between personal PM25 exposures and corresponding ambient concentrations were strongest for well-ventilated indoor environments and decreased with ventilation. This decrease was attributed to the increasing influence of indoor PM2 5 sources. Evidence for this was provided by SO4 2-measurements, which can be thought of as a tracer for ambient PM25. For SO4 2-, personal-ambient associations were strong even in poorly ventilated indoor environments, suggesting that personal exposures to PM2.5 of ambient origin are strongly associated with corresponding ambient concentrations. The results also indicated that the contribution of indoor PM2.5 sources to personal PM2.5 exposures was lowest when individuals spent the majority of their time in well-ventilated indoor environments.

Results also indicate that the potential for confounding by PM2.5 co-pollutants is limited, despite significant correlations among ambient pollutant concentrations. In contrast to ambient concentrations, PM2.5 exposures were not significantly correlated with personal exposures to PM2.5-10, PM2.5 of non-ambient origin, O3, NO2, and SO2. Since a confounder must be associated with the exposure of interest, these results provide evidence that the effects observed in the PM2.5 epidemiologic studies are unlikely to be due to confounding by the PM2.5 co-pollutants measured in this study.  相似文献   

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