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1.
Interactions between mercury and dissolved organic matter--a review   总被引:14,自引:0,他引:14  
Ravichandran M 《Chemosphere》2004,55(3):319-331
Dissolved organic matter (DOM) interacts very strongly with mercury, affecting its speciation, solubility, mobility, and toxicity in the aquatic environment. Strong binding of mercury by DOM is attributed to coordination of mercury at reduced sulfur sites within the organic matter, which are present at concentrations much higher than mercury concentrations found in most natural waters. The ability of organic matter to enhance the dissolution and inhibit the precipitation of mercuric sulfide, a highly insoluble solid, suggests that DOM competes with sulfide for mercury binding. This is confirmed by very high conditional stability constants for mercury-organic sulfur (RSHg+) complexes (10(25)-10(32)) recently reported in literature. DOM appears to play a key role in the photochemical reduction of ionic mercury to elemental mercury and subsequent reoxidation of elemental mercury to ionic mercury, thus affecting volatilization loss and bioavailability of mercury to organisms. DOM affects the production and bioaccumulation of methylmercury, the most bioaccumulative mercury species in fish.  相似文献   

2.
Injection of powdered activated carbon (PAC) upstream of particulate removal devices (such as electrostatic precipitator and baghouses) has been used effectively to remove hazardous air pollutants, particularly mercury-containing pollutants, emitted from combustors and incinerators. Compared with commercial PACs (CPACs), an alternative PAC derived from waste tires (WPAC) was prepared for this study. The equilibrium adsorptive capacity of mercury chloride (HgCl2) vapor onto the WPAC was further evaluated with a self-designed bench-scale adsorption column system. The adsorption temperatures investigated in the adsorption column were controlled at 25 and 150 degrees C. The superficial velocity and residence time of the flow were 0.01 m/sec and 4 sec, respectively. The adsorption column tests were run under nitrogen gas flow. Experimental results showed that WPAC with higher Brunauer-Emmett-Teller (BET) surface area could adsorb more HgCl2 at room temperature. The equilibrium adsorptive capacity of HgCl2 for WPAC measured in this study was 1.49 x 10(-1) mg HgCl2/g PAC at 25 degrees C with an initial HgCI2 concentration of 25 microg/m3. With the increase of adsorption temperature < or = 150 degrees C, the equilibrium adsorptive capacity of HgCl2 for WPAC was decreased to 1.34 x 10(-1) mg HgCl2/g PAC. Furthermore, WPAC with higher sulfur contents could adsorb even more HgCl2 because of the reactions between sulfur and Hg2+ at 150 degrees C. It was demonstrated that the mechanisms for adsorbing HgCl2 onto WPAC were physical adsorption and chemisorption at 25 and 150 degrees C, respectively. Experimental results also indicated that the apparent overall driving force model appeared to have the good correlation with correlation coefficients (r) > 0.998 for HgCl2 adsorption at 25 and 150 degrees C. Moreover, the equilibrium adsorptive capacity of HgCl2 for virgin WPAC was similar to that for CPAC at 25 degrees C, whereas it was slightly higher for sulfurized WPAC than for CPAC at 150 degrees C.  相似文献   

3.
Xia LY  Gu DH  Tan J  Dong WB  Hou HQ 《Chemosphere》2008,71(9):1774-1780
The photolysis of simulating low concentration of hydrogen sulfide malodorous gas was studied under UV irradiation emitted by self-made microwave discharge electrodeless lamps (i.e. microwave UV electrodeless mercury lamp (185/253.7 nm) and iodine lamp (178.3/180.1/183/184.4/187.6/206.2 nm)). Experiments results showed that the removal efficiency (eta H2S) of hydrogen sulfide was decreased with increasing initial H2S concentration and increased slightly with gas residence time; H2S removal efficiency was decreased dramatically with enlarged pipe diameter. Under the experimental conditions with pipe diameter of 36 mm, gas flow rate of 0.42 standard l s(-1), eta H2S was 52% with initial H2S concentration of 19.5 mg m(-3) by microwave mercury lamp, the absolute removal amount (ARA) was 4.30 microg s(-1), and energy yield (EY) was 77.3 mg kW h(-1); eta H2S was 56% with initial H2S concentration of 18.9 mg m(-3) by microwave iodine lamp, the ARA was 4.48 microg s(-1), and the EY was 80.5mg kW h(-1). The main photolysis product was confirmed to be SO4(2-) with IC.  相似文献   

4.
Kinetics and stoichiometry of aerobic chemical and biological sulfide oxidation in wastewater from sewer networks were studied. In this respect, the effects of temperature and pH were investigated in the ranges 10 to 20 degrees C and 5 to 9, respectively. The temperature dependency of sulfide oxidation kinetics was described using an Arrhenius relationship. The effect of pH on the rate of chemical sulfide oxidation is related to the dissociation of hydrogen sulfide (H2S) to hydrogen sulfide ion (HS(-)), with HS(-) being more readily oxidized than H2S. Biological sulfide oxidation exhibited the highest rates at ambient wastewater pH, and the reaction was inhibited at both low and high pH values. Chemical sulfide oxidation was found to produce thiosulfate and sulfate, while elemental sulfur was the main product of biological sulfide oxidation. Based on the investigations, general rate equations and stoichiometric constants were determined, enabling the processes to be incorporated to conceptual sewer process models.  相似文献   

5.
The objective of this work was to evaluate the effect of the initial sulfide concentration on the kinetics and metabolism of phenol and sulfide in batch bioassays using nitrate as electron acceptor. Complete oxidation of sulfide (20 mg L(-1) of S(2-)) and phenol (19.6 mg L(-1)) was linked to nitrate reduction when nitrate was supplemented at stoichiometric concentrations. At 32 mg L(-1) of sulfide, oxidation of sulfide and phenol by the organo-lithoautotrophic microbial culture was sequential; first sulfide was rapidly oxidized to elemental sulfur and afterwards to sulfate; phenol oxidation started once sulfate production reached a maximum. When the initial sulfide concentration was increased from 20 to 26 and finally to 32 mg L(-1), sulfide oxidation was inhibited. In contrast phenol consumption by the denitrifying culture was not affected. These results indicated that sulfide affected strongly the sulfide oxidation rate and nitrate reduction.  相似文献   

6.
研究了载硫温度、硫炭比(简称S/C),吸附温度等因素对载硫活性炭的硫含量、脱汞能力以及硫损失的影响,探讨载硫活性炭制备的工艺条件优化。结果表明,不同载硫温度下制备的载硫活性炭的气态Hg0吸附能力远强于原料活性炭;载硫温度不同时,负载到活性炭孔隙或表面上的硫的形态不同,导致了脱汞能力的差异,较合适的载硫温度为350℃;S/C为5%(质量分数,下同)时,随着吸附温度的升高,载硫活性炭的气态Hg0吸附量降低;在一定的载硫温度下,原料中S/C越高时,制备的载硫活性炭的硫含量越高、气态Hg0吸附能力越强,但其硫损失率也越高,从实际的使用效果来看,较合适的S/C为10%。  相似文献   

7.
Fourteen sulfur and/or sulfuric acid producing regenerate FGD processes were discussed at the 1974 FGD Symposium in Atlanta. During the period elapsed since then, considerable status change has occurred on many of these regenerable processes. Other regenerable processes which were not as well known during 1974 have surfaced in 1975. The problems of obtaining reducing gases (hydrogen sulfide, carbon monoxide, and hydrogen) for the reduction of sulfur dioxide product streams to elemental sulfur have become severe due to shortages of natural gas or other petroleum based feedstock. A new sulfur producing process which employs CO and H2 directly (rather than the H2S required for liquid and vapor base Claus reactions) is gaining attention. This paper discusses briefly: (1) the announced status of the many regenerable FGD processes, (2) the problem of reductant gas supply, and (3) the effect on FGD processes of using coal based reducing gas instead of reformed natural gas.  相似文献   

8.
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   

9.
Maas Pv  Brink Pv  Klapwijk B  Lens P 《Chemosphere》2009,75(2):243-249
BioDeNO(x), a novel technique to remove NO(x) from industrial flue gases, is based on absorption of gaseous nitric oxide into an aqueous Fe(II)EDTA(2-) solution, followed by the biological reduction of Fe(II)EDTA(2-) complexed NO to N(2). Besides NO reduction, high rate biological Fe(III)EDTA(-) reduction is a crucial factor for a succesful application of the BioDeNO(x) technology, as it determines the Fe(II)EDTA(2-) concentration in the scrubber liquor and thus the efficiency of NO removal from the gas phase. This paper investigates the mechanism and kinetics of biological Fe(III)EDTA(-) reduction by unadapted anaerobic methanogenic sludge and BioDeNO(x) reactor mixed liquor. The influence of different electron donors, electron mediating compounds and CaSO(3) on the Fe(III)EDTA(-) reduction rate was determined in batch experiments (21mM Fe(III)EDTA(-), 55 degrees C, pH 7.2+/-0.2). The Fe(III)EDTA(-) reduction rate depended on the type of electron donor, the highest rate (13.9mMh(-1)) was observed with glucose, followed by ethanol, acetate and hydrogen. Fe(III)EDTA(-) reduction occurred at a relatively slow (4.1mMh(-1)) rate with methanol as the electron donor. Small amounts (0.5mM) of sulfide, cysteine or elemental sulfur accelerated the Fe(III)EDTA(-) reduction. The amount of iron reduced significantly exceeded the amount that can be formed by the chemical reaction of sulfide with Fe(III)EDTA(-), suggesting that the Fe(III)EDTA(-) reduction was accelerated via an auto-catalytic process with an unidentified electron mediating compound, presumably polysulfides, formed out of the sulfur additives. Using ethanol as electron donor, the specific Fe(III)EDTA(-) reduction rate was linearly related to the amount of sulfide supplied. CaSO(3) (0.5-100mM) inhibited Fe(III)EDTA(-) reduction, probably because SO(3)(2-) scavenged the electron mediating compound.  相似文献   

10.
Direct mercury (Hg) speciation was assessed for soil samples with a Hg concentration ranging from 7 up to 240 mg kg−1. Hg chemical forms were identified and quantified by sequential extractions and bulk- and micro-analytical techniques exploiting synchrotron generated X-rays. In particular, microspectroscopic techniques such as μ-XRF, μ-XRD and μ-XANES were necessary to solve bulk Hg speciation, in both soil fractions <2 mm and <2 μm. The main Hg-species found in the soil samples were metacinnabar (β-HgS), cinnabar (α-HgS), corderoite (Hg3S2Cl2), and an amorphous phase containing Hg bound to chlorine and sulfur. The amount of metacinnabar and amorphous phases increased in the fraction <2 μm. No interaction among Hg-species and soil components was observed. All the observed Hg-species originated from the slow weathering of an inert Hg-containing waste material (K106, U.S. EPA) dumped in the area several years ago, which is changing into a relatively more dangerous source of pollution.  相似文献   

11.
Mercury removal from incineration flue gas by organic and inorganic adsorbents   总被引:11,自引:0,他引:11  
Jurng J  Lee TG  Lee GW  Lee SJ  Kim BH  Seier J 《Chemosphere》2002,47(9):907-913
Experiments were performed to investigate various adsorbents for their mercury removal capabilities from incineration flue gases. Four different materials were tested; Zeolite, Bentonite, activated carbon (AC), and wood char. Real incineration off-gas and in-lab simulated combustion flue gases (N2 + Hg) were used. Three cylindrical-shaped sorbent columns with 5 cm in diameter and 20 cm in length were used. The gas flow rate was fixed at 660 l/h at all times. Concentrations of NO, CO, O2, CO2, SO2, H2O, HCl, and mercury were continuously monitored. Mercury removal efficiencies of natural Zeolite and Bentonite were found to be much lower than those of the referenced AC. Amount of Hg removed were 9.2 and 7.4 microg/g of Zeolite and Bentonite, respectively. Removal efficiencies of each layer consisted of inorganic adsorbents were no higher than 7%. No significant improvement was observed with sulfur impregnation onto the inorganic adsorbents. Organic adsorbents (wood char and AC) showed much higher mercury removal efficiencies than those of inorganic ones (Zeolite and Bentonite). Mercury removal efficiency of wood char reached over 95% in the first layer, showing almost same effectiveness as AC which currently may be the most effective adsorbents for mercury. Amount of mercury captured by wood char was approximately 0.6 mg/g of wood char, close to the amount captured by AC tested in this study. Hence, wood char, made from the waste woods through a gasification process, should be considered as a possible alternative to relatively expensive AC.  相似文献   

12.
Aspects of the core-shell model of nanoscale zero-valent iron (nZVI) and their environmental implications were examined in this work. The structure and elemental distribution of nZVI were characterized by X-ray energy-dispersive spectroscopy (XEDS) with nanometer-scale spatial resolution in an aberration-corrected scanning transmission electron microscope (STEM). The analysis provides unequivocal evidence of a layered structure of nZVI consisting of a metallic iron core encapsulated by a thin amorphous oxide shell. Three aqueous environmental contaminants, namely Hg(II), Zn(II) and hydrogen sulfide, were studied to probe the reactive properties and the surface chemistry of nZVI. High-resolution X-ray photoelectron spectroscopy (HR-XPS) analysis of the reacted particles indicated that Hg(II) was sequestrated via chemical reduction to elemental mercury. On the other hand, Zn(II) removal was achieved via sorption to the iron oxide shell followed by zinc hydroxide precipitation. Hydrogen sulfide was immobilized on the nZVI surface as disulfide (S(2)(2-)) and monosulfide (S(2-)) species. Their relative abundance in the final products suggests that the retention of hydrogen sulfide occurs via reactions with the oxide shell to form iron sulfide (FeS) and subsequent conversion to iron disulfide (FeS(2)). The results presented herein highlight the multiple reactive pathways permissible with nZVI owing to its two functional constituents. The core-shell structure imparts nZVI with manifold functional properties previously unexamined and grants the material with potentially new applications.  相似文献   

13.
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   

14.
A number of activated carbons derived from waste tires were further impregnated by gaseous elemental sulfur at temperatures of 400 and 650 degrees C, with a carbon and sulfur mass ratio of 1:3. The capabilities of sulfur diffusing into the micropores of the activated carbons were significantly different between 400 and 650 degrees C, resulting in obvious dissimilarities in the sulfur content of the activated carbons. The sulfur-impregnated activated carbons were examined for the adsorptive capacity of gas-phase mercuric chloride (HgC1) by thermogravimetric analysis (TGA). The analytical precision of TGA was up to 10(-6) g at the inlet HgCl2 concentrations of 100, 300, and 500 microg/m3, for an adsorption time of 3 hr and an adsorption temperature of 150 degrees C, simulating the flue gas emitted from municipal solid waste (MSW) incinerators. Experimental results showed that sulfur modification can slightly reduce the specific surface area of activated carbons. High-surface-area activated carbons after sulfur modification had abundant mesopores and micropores, whereas low-surface-area activated carbons had abundant macropores and mesopores. Sulfur molecules were evenly distributed on the surface of the inner pores after sulfur modification, and the sulfur content of the activated carbons increased from 2-2.5% to 5-11%. After sulfur modification, the adsorptive capacity of HgCl2 for high-surface-area sulfurized activated carbons reached 1.557 mg/g (22 times higher than the virgin activated carbons). The injection of activated carbons was followed by fabric filtration, which is commonly used to remove HgCl2 from MSW incinerators. The residence time of activated carbons collected in the fabric filter is commonly about 1 hr, but the time required to achieve equilibrium is less than 10 min. Consequently, it is worthwhile to compare the adsorption rates of HgCl2 in the time intervals of < 10 and 10-60 min.  相似文献   

15.
The carpophores of Parasol Mushroom and underlying soil substrate collected from several unpolluted and spatially distant sites across Poland were examined to know content and bioconcentration potential of mercury by this species. The total mercury content of the caps of Parasol Mushroom for the particular sites ranged from 1.1 +/- 1.0 to 8.4 +/- 7.4 microg/g dry matter (total range from 0.05 to 22 microg/g dm), while in the stalks were from 0.53 +/- 0.27 to 6.8 +/- 7.1 microg/g dm (total range from 0.078 to 20 microg/g dm). A top soil layer (0-10 cm) showed baseline mercury concentration from 0.022 +/- 0.011 to 0.36 +/- 0.16 microg/g dm (total range from 0.010 to 0.54 microg/g dm). Parasol Mushroom is an effective mercury accumulator in the carpophores and bioconcentration factor (BCF) values of this element in the caps and depending on the sampling site ranged from 16 +/- 6 to 220 +/- 110 (total range from 0.52 to 470), while for the stalks were from 7.6 +/- 2.6 to 130 +/- 96 (total range from 0.52 to 340). It seems reasonable to state that tolerance (maximum allowable concentration) of the total mercury in a single cap of Parasol Mushroom at unpolluted areas should not exceed 25 microg/g dm. A value greater then 25 mu g/g dm will imply an elevated content due to site pollution problems. Nevertheless, knowledge on highly toxic methylmercury content and its fraction in the total mercury content of Parasol Mushroom is lacking.  相似文献   

16.
In this study, removing sulfur dioxide (SO2), nitrogen oxides (NO(x)), and mercury (Hg) from simulated flue gas was investigated in two laboratory-sized bubbling reactors that simulated an oxidizing reactor (where the NO and Hg(0) oxidation reactions are expected to occur) and a wet limestone scrubber, respectively. A sodium chlorite solution was used as the oxidizing agent. The sodium chlorite solution was an effective additive that enhanced the NO(x), Hg, and SO2 capture from the flue gas. Furthermore, it was discovered that the location of the sodium chlorite application (before, in, or after the wet scrubber) greatly influences which pollutants are removed and the amount removed. This effect is related to the chemical conditions (pH, absence/presence of particular gases) that are present at different positions throughout the flue gas cleaning system profile. The research results indicated that there is a potential to achieve nearly zero SO2, NO(x), and Hg emissions (complete SO2, NO, and Hg removals and -90% of NO(x) absorption from initial values of 1500 ppmv of SO2, 200 ppmv of NO(x), and 206 microg/m3 of Hg(0)) from the flue gas when sodium chlorite was applied before the wet limestone scrubber. However applying the oxidizer after the wet limestone scrubber was the most effective configuration for Hg and NO(x) control for extremely low chlorite concentrations (below 0.002 M) and therefore appears to be the best configuration for Hg control or as an additional step in NO(x) recleaning (after other NO(x) control facilities). The multipollutant scrubber, into which the chlorite was injected simultaneously with the calcium carbonate slurry, appeared to be the least expensive solution (when consider only capital cost), but exhibited the lowest NO(x) absorption at -50%. The bench-scale test results presented can be used to develop performance predictions for a full- or pilot-scale multipollutant flue gas cleaning system equipped with wet flue gas desulfurization scrubber.  相似文献   

17.
Stabilization of mercury-containing wastes using sulfide   总被引:1,自引:0,他引:1  
This paper summarizes the findings of our studies on mercury stabilization using sulfide. Primary stabilization variables such as stabilization pH and sulfide/mercury molar ratio were tested. Mercury stabilization effectiveness was evaluated using the Toxicity Characteristic Leaching Procedure (TCLP) and the constant pH leaching tests. The influence of interfering ions on mercury immobilization was also tested. The experimental results indicate that the sulfide-induced treatment technology is an effective way to minimize mercury leaching. It was found that the most effective mercury stabilization occurs at pH 6 combined with a sulfide/mercury molar ratio of 1. The combined use of increased dosage of sulfide and ferrous ions ([S]/[Hg]=2 and [Fe]/[Hg]=3 at pH=6) can significantly reduce interferences by chloride and/or phosphate during sulfide-induced mercury immobilization. The sulfide-treated waste stabilization efficiency reached 98%, even with exposure of the wastes to high pH leachants.  相似文献   

18.
Long-term operation of a biofilter for simultaneous removal of H2S and NH3   总被引:5,自引:0,他引:5  
Simultaneous removal of NH3 and H2S was investigated using two types of biofilters--one packed with wood chips and the other with granular activated carbon (GAC). Experimental tests and measurements included analyses of removal efficiency (RE), metabolic products, and results of long-term operation (around 240 days). The REs for NH3 and H2S were 92 and 99.9%, respectively, before deactivation. After deactivation, the RE for NH3 and H2S were decreased to 30-50% and 75%, respectively. The activity of nitrifying bacteria was inhibited by high concentrations of H2S (over 200 ppm) but recovered gradually after H2S addition was ceased. However, the Thiobacillus thioparus as sulfur oxidizing bacteria did not show inhibition at the NH3 concentration under 150-ppm conditions. The deactivation of the biofilter was caused by metabolic products [elemental sulfur and (NH4)2SO4] accumulating on the packing materials during the extended operation. The removal capacities for NH3 and H2S were 6.0-8.0 and 45-75 mg N, S/L/hr, respectively.  相似文献   

19.
Application of riverbed sand for the adsorptive separation of cadmium(II) from aqueous solutions has been investigated. Removal increased from 26.8 to 56.4% by decreasing the initial concentration of cadmium from 7.5 x 10(-5) to 1.0 x 10(-5)M at pH 6.5, 25 degrees C temperature, agitation speed of 100 rpm, 100 microm particle size and 1.0 x 10(-2) NaClO4 ionic strength. Process of separation is governed by first order rate kinetics. The value of rate constant of adsorption, k(ad), was found to be 2.30 x 10(-2)per min at 25 degrees C. Values of coefficient of mass transfer, beta L, were calculated and its value at 25 degrees C was found to be 1.92 x 10(-2)cm/s. Values of Langmuir constant were calculated. Values of thermodynamic parameters delta G0, delta H0 and delta S0 were also calculated and were recorded as -0.81 kcal/mol, -9.31 kcal/mol and -28.10 cal/mol at 25 degrees C. pH has been found to affect the removal of cadmium significantly and maximum removal, 58.4%, has been found at pH 8.5. Process can be used for treatment of cadmium(II) rich wastewaters.  相似文献   

20.
用于气态零价汞转化的催化剂研究   总被引:4,自引:0,他引:4  
零价汞的高效去除是燃煤烟气汞污染控制过程中的关键环节。为了促进烟气中的零价汞转化为易于去除的氧化态汞,分别考察了在有HCl存在时,几种过渡金属氧化物(Cu、Fe、Mn、Co和Zr)对零价汞氧化的催化作用,以筛选出性能较好的催化组分;为提高催化剂的抗SO2性能,分别尝试了利用几种金属元素(Sr、Ce、W和Mo)对催化剂进行掺杂改性的方法。结果表明,锰氧化物的催化作用最好,其最佳使用温度在573 K左右;SO2对零价汞的催化氧化有明显抑制作用,在无SO2及1 400 mg/m3SO2时锰催化剂对零价汞催化氧化效率分别为93%和78%。而Mo改性的锰氧化物催化剂的抗硫性能大幅提高,在1 400 mg/m3SO2存在的情况下其对零价汞的催化氧化效率可达到90%以上,较其他改性元素高。  相似文献   

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