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1.
Speciation of methylmercury in rice grown from a mercury mining area   总被引:1,自引:0,他引:1  
Monomethylmercury (CH3Hg+ and its complexes; MeHg hereafter) is a known developmental neurotoxin. Recent studies have shown that rice (Oryza sativa L.) grain grown from mercury (Hg) mining areas may contain elevated MeHg concentrations, raising concerns over the health of local residents who consume rice on a daily basis. An analytical method employing high performance liquid chromatography (HPLC) - inductively coupled plasma mass spectrometry (ICP-MS) following enzymatic hydrolysis was developed to analyze the speciation of MeHg in uncooked and cooked white rice grain grown from the vicinity of a Hg mine in China. The results revealed that the MeHg in the uncooked rice is present almost exclusively as CH3Hg-l-cysteinate (CH3HgCys), a complex that is thought to be responsible for the transfer of MeHg across the blood-brain and placental barriers. Although cooking does not change the total Hg or total MeHg concentration in rice, no CH3HgCys is measurable after cooking, suggesting that most, if not all, of the CH3HgCys is converted to other forms of MeHg, the identity and toxicity of which remain elusive.  相似文献   

2.
Abstract

This paper is particularly related to elemental mercury (Hg0) oxidation and divalent mercury (Hg2+) reduction under simulated flue gas conditions in the presence of nitric oxide (NO) and sulfur dioxide (SO2). As a powerful oxidant and chlorinating reagent, Cl2 has the potential for Hg oxidation. However, the detailed mechanism for the interactions, especially among chlorine (Cl)-containing species, SO2, NO, as well as H2O, remains ambiguous. Research described in this paper therefore focused on the impacts of SO2 and NO on Hg0 oxidation and Hg2+ reduction with the intent of unraveling unrecognized interactions among Cl species, SO2, and NO most importantly in the presence of H2O. The experimental results demonstrated that SO2 and NO had pronounced inhibitory effects on Hg0 oxidation at high temperatures when H2O was also present in the gas blend. Such a demonstration was further confirmed by the reduction of Hg2+ back into its elemental form. Data revealed that SO2 and NO were capable of promoting homogeneous reduction of Hg2+ to Hg0 with H2O being present. However, the above inhibition or promotion disappeared under homogeneous conditions when H2O was removed from the gas blend.  相似文献   

3.
To investigate the chemical characteristics of precipitation in the polluted coastal atmosphere, a total of 46 event-based precipitation samples were collected using a wet-only automatic precipitation collector from September 2006 to October 2007 at metropolitan Newark, New Jersey in the US East Coast. Samples were analyzed by ion chromatography for the concentrations of major inorganic ions (Cl, NO3, SO42−, F, NH4+, Ca2+, Mg2+, Na+, K+) and organic acid species (CH3COO, HCOO, CH2(COO)22−, C2O42−). Selected trace metals (Sb, Pb, Al, V, Fe, Cr, Co, Ni, Cu, Zn, Cd) in samples were determined by ICPMS. Mass concentration results show that SO42− was the most dominant anion accounting for 51% of the total anions, controlling the acidity of the precipitation. NH4+ accounted for 48.6% of the total cations, dominating the precipitation neutralization. CH3COO and HCOO were the two dominant water-soluble organic acid species, accounting for 42% and 40% of the total organic acids analyzed, respectively. Al, Zn and Fe were the three major trace metals in precipitation, accounting for 34%, 27%, and 25% of the total mass of metals analyzed. The pH values in precipitation ranged from 4.4 to 4.9, indicating an acidic nature. Enrichment Factor (EF) Analysis showed that Na+, Cl, Mg2+ and K+ in the precipitation were primarily of marine origin, while most of the Fe, Co and Al were from crust sources. Pb, V, Cr, Ni were moderately enriched with EFs ranging 43–410, while Zn, Sb, Cu, Cd and F were highly enriched with EFs > 700, indicating significant anthropogenic influences. Factor analysis suggests 6 major sources contributing to the observed composition of precipitation at this location: (1) nitrogen-enriched soil, (2) secondary pollution processes, (3) marine sources, (4) incinerations, (5) oil combustions, and (6) malonate–vanadium enriched sources. To further explore the source–precipitation event relationships and seasonality, cluster analysis was performed for all precipitation events. Results show that about half of the precipitation events were characterized by mixed sources. Significant influences of nitrogen-enriched soil and marine sources were associated with precipitation events in spring and autumn, while secondary pollution processes, incineration and oil combustion contributed greatly in summer.  相似文献   

4.
ABSTRACT

Analysis of Hg speciation in combustion flue gases is often accomplished in standardized sampling trains in which the sample is passed sequentially through a series of aqueous solutions to capture and separate oxidized Hg (Hg2+) and elemental Hg (Hg0). Such methods include the Ontario Hydro (OH) and the Alkaline Mercury Speciation (AMS) methods, which were investigated in the laboratory to determine whether the presence of Cl2 and other common flue gas species can bias the partitioning of Hg0 to front impingers intended to isolate Hg2+ species. Using only a single impinger to represent the front three impingers for each method, it was found that as little as 1-ppm Cl2 in a simulated flue gas mixture led to a bias of approximately 10-20% of Hg0 misreported as Hg2+ for both the OH and the AMS methods. Experiments using 100-ppm Cl2 led to a similar bias in the OH method, but to a 30-60% bias in the AMS method. These false readings are shown to be due to liquid-phase chemistry in the impinger solutions, and not necessarily to the gas-phase reactions between Cl2 and Hg as previously proposed. The pertinent solution chemistry causing the interference  相似文献   

5.
In a laboratory study we investigated 1) the potential production of nitrous oxide (N2O), methane (CH4) and carbon dioxide (CO2) and 2) the effect of nitrate (NO3?) and anaerobic N2O development on CH4 production in sediment from a recently recreated free surface water wetland (FSWW) and in soil from an adjacent meadow. We designed an experiment where production of greenhouse gases was registered at the time of maximum net development of N2O. We made additions of biodegradable carbon (glucose) and/or NO3? to sediment and soil slurries and incubated them at four temperatures (4, 13, 20, 28 °C). Gas production from both substrates was positively correlated with temperature. We also found that the sediment produced more N2O than the soil. N2O production in sediment was NO3? limited, whereas in soil carbon availability was lower and only combined additions of NO3? and glucose supported increased N2O development. CH4 production was generally low and did not differ between soil and sediment. Nor did glucose addition increase CH4 rates. The results suggest that neither soil nor sediment environment did support development of methanogenic populations. There were no clear effects of NO3? on CH4 production. However, the highest records of CH4 were found in incubations with low N2O production, which indicates that N2O might be toxic to methanogens. In summary, our study showed that transforming meadows into FSWWs implies a risk of increased N2O emissions. This does not seem to be valid for CH4. However, since N2O is almost always produced wherever NO3? is denitrified, increased N2O production in wetlands leads to reduced rates in downstream environments. Hence, we conclude that when balancing NO3? retention and global warming aspects, we find no reason to discourage future creation or restoration of wetlands.  相似文献   

6.
The influences of different kinds of anthropogenic activities on rainwater chemistry in a tropical area were studied during one uninterrupted year at Piracicaba River Basin (Southeast Brazil). A total of 272 rainwater samples collected continuously from August 1997 to July 1998 at four different sites were analyzed for F, CH3COO, HCOO, MSA, Cl, NO2, Br, NO3, SO42−, C2O42−, PO43−, Na+, NH4+, K+, Mg2+, Ca2+, DOC (dissolved organic carbon), DIC (dissolved inorganic carbon), pH and conductivity. The most abundant ion was H+ and rain acidity was significant at all sampling sites (average pH of 4.4–4.5). The sources of this free acidity differ among sites and appear to be correlated to the different land-uses. The composition of rainwater appeared to be controlled mostly by three sources: soil dust, sugar cane burning and industrial emissions.  相似文献   

7.
Different land uses in subtropics play an important role in regulating the global environmental changes. To reduce uncertainties of greenhouse gas (GHG) emissions of agricultural soils in subtropical ecosystem, a four years campaign was started to determine the temporal GHG (CO2 and CH4) fluxes from seven sites of four land use types (1 vegetable field, 3 uplands, 2 orchards, 1 pine forest). The mean annual budgets of CO2, and CH4 were 6.5~10.5 Mg CO2 ha?1 yr?1, and +0.47 ~ ?2.37 kg CH4 ha?1 yr?1, respectively. Pine forest had significantly lower CO2 emission and higher CH4 uptake than agriculture land uses. Tilled orchard emitted more CO2 and oxidized less CH4 than non-tilled orchard. Upland crops had higher CO2 emissions than orchards, while abrupt differences of CH4 uptake were observed between upland crops and orchards. Every year, the climate was warm and wet from April to September (the hot–humid season) and became cool and dry from October to March (the cool–dry season). Driven by seasonality of temperature and WFPS, CO2 fluxes were significantly higher in the hot–humid season than in cool–dry season. Soil temperature, WFPS, NO3?–N and NH4+–N contents interactively explained CH4 uptake which was significantly higher in cool–dry season than in hot–humid season. We conclude that soil C fluxes from different land uses are strongly under control of different climatic predictors along with soil nutrient status, which interact in conjunction with each other to supply the readily available substrates.  相似文献   

8.
Fe2O3 and CeO2 modified activated coke (AC) synthesized by the equivalent-volume impregnation were employed to remove elemental mercury (Hg0) from simulated flue gas at a low temperature. Effects of the mass ratio of Fe2O3 and CeO2, reaction temperature, and individual flue gas components including O2, NO, SO2, and H2O (g) on Hg0 removal efficiency of impregnated AC were investigated. The samples were characterized by Brunauer–Emmett–Teller (BET), X-ray diffraction (XRD), scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS). Results showed that with optimal mass percentage of 3 % Fe2O3 and 3 % CeO2 on Fe3Ce3/AC, the Hg0 removal efficiency could reach an average of 88.29 % at 110 °C. Besides, it was observed that O2 and NO exhibited a promotional effect on Hg0 removal, H2O (g) exerted a suppressive effect, and SO2 showed an insignificant inhibition without O2 to some extent. The analysis of XPS indicated that the main species of mercury on used Fe3Ce3/AC was HgO, which implied that adsorption and catalytic oxidation were both included in Hg0 removal. Furthermore, the lattice oxygen, chemisorbed oxygen, and/or weakly bonded oxygen species made a contribution to Hg0 oxidation.  相似文献   

9.
Knowing the fraction of methane (CH4) oxidized in landfill cover soils is an important step in estimating the total CH4 emissions from any landfill. Predicting CH4 oxidation in landfill cover soils is a difficult task because it is controlled by a number of biological and environmental factors. This study proposes an artificial neural network (ANN) approach using feedforward backpropagation to predict CH4 oxidation in landfill cover soil in relation to air temperature, soil moisture content, oxygen (O2) concentration at a depth of 10 cm in cover soil, and CH4 concentration at the bottom of cover soil. The optimum ANN model giving the lowest mean square error (MSE) was configured from three layers, with 12 and 9 neurons at the first and the second hidden layers, respectively, log-sigmoid (logsig) transfer function at the hidden and output layers, and the Levenberg-Marquardt training algorithm. This study revealed that the ANN oxidation model can predict CH4 oxidation with a MSE of 0.0082, a coefficient of determination (R 2) between the measured and predicted outputs of up to 0.937, and a model efficiency (E) of 0.8978. To conclude, further developments of the proposed ANN model are required to generalize and apply the model to other landfills with different cover soil properties.

Implications:

To date, no attempts have been made to predict the percent of CH4 oxidation within landfill cover soils using an ANN. This paper presents modeling of CH4 oxidation in landfill cover soil using ANN based on field measurements data under tropical climate conditions in Malaysia. The proposed ANN oxidation model can be used to predict the percentage of CH4 oxidation from other landfills with similar climate conditions, cover soil texture, and other properties. The predicted value of CH4 oxidation can be used in conjunction with the Intergovernmental Panel on Climate Change (IPCC) First Order Decay (FOD) model by landfill operators to accurately estimate total CH4 emission and how much it contributes to global warming.  相似文献   


10.
《Chemosphere》2011,82(11):1469-1476
Soil metabolism of sulfonamides is largely unknown. Hence the sulfonamides sulfanilamide (SAA), sulfadimethoxine (SDT) and sulfapyridine (SPY) were reacted in model experiments with a fungal laccase from Trametes versicolor. Enzymatic transformation after a reaction time of 15 d ranged from 10.0% for SAA up to 95.6% for SPY and the difference was attributed to the different molecular substituents. Metabolites were first tentatively assigned after LC–ESI+–MS full-scan analysis. Secondly, the proposed metabolites were further confirmed employing either multiple reaction monitoring in comparison with standard substances or precursor ion scan LC–ESI+–MS/MS experiments striving for the precursor and two to three product ions. Aniline was confirmed as a breakdown product of SPY and further metabolites of SPY and of SDT were identified as rearranged SO2 extrusion products. Thirdly, some of the metabolites matched those that were previously reported for sulfonamide photodegradation and degradation in soil. It was concluded that enzymatic metabolism as investigated here also occurs in soil.  相似文献   

11.

In this work, biochar (BC), activated carbon (AC), and graphene oxide (GO) were thiol-functionalized using 3-mercaptopropyltrimethoxysilane (3-MPTS) (named as BCS, ACS, and GOS, respectively). BCS, ACS, and GOS were synthesized mainly via the interaction between hydrolyzed 3-MPTS and surface oxygen-containing functional groups (e.g., –OH, O–C=O, and C=O) and π-π interaction. The materials before and after modification were characterized and tested for mercury removal, including sorption kinetics and isotherms, the effects of adsorbent dosage, initial pH, and ionic strength. Pseudo-second-order sorption kinetic model (R2 = 0.992~1.000) and Langmuir sorption isotherm model (R2 = 0.964~0.998) fitted well with the sorption data of mercury. GOS had the most –SH groups with the largest adsorption capacity for Hg2+ and CH3Hg+ (449.6 and 127.5 mg/g), followed by ACS (235.7 and 86.7 mg/g) and BCS (175.6 and 30.3 mg/g), which were much larger than GO (96.7 and 4.9 mg/g), AC (81.1 and 24.6 mg/g), and BC (95.6 and 9.4 mg/g). GOS and ACS showed stable mercury adsorption properties at a wide pH range (2~9) and ionic strength (0.01~0.1 mol/L). Mercury maybe removed by ligand exchange, surface complexation, and electrostatic attraction.

  相似文献   

12.
To investigate whether wind is a significant driving force in the diffusion of CO and CH4 from the atmosphere into soil, we measured the concentrations of these two gases at two heights above a temperate grass field in Japan and estimated their deposition velocities using micrometeorological techniques. The concentrations were inversely correlated with wind speed, indicating that the local concentrations were influenced by ground sources. The CO and CH4 concentrations at 0.33 m were usually lower than those at 1.3 m. Although nocturnal data are suspected to be non-stationary, by selecting several periods when the changes of the concentrations were small but larger than analytical precision, we obtained a CO velocity of 2.9 and 3.9×10−2 cms−1, agreeing with a CO deposition velocity, 3.4×10−2 cms−1, obtained by applying a method using CO2 as a tracer. The CH4 influx obtained by the method using CO2 as a tracer was 13 ngm−2 s−1. The ranges of the CO deposition velocity and CH4 influx were similar to those obtained in previous studies in grassfields and in a nearby arable field using a closed-chamber technique. This shows that light winds do not greatly accelerate CO and CH4 uptake by soil.  相似文献   

13.
Due to the intense microbial oxidation of organic soils in the Florida Everglades, approximately 1400 kg N/ha are mineralized annually. Most of this nitrogen is lost to the atmosphere through denitrification in the soil. Nitrous oxide is one of the gaseous products of denitrification, therefore the objectives of this study were to determine the quantities of N2O emitted from these soils and to measure the effect of this N2O on ambient mixing ratios in the Everglades. Nitrous oxide fluxes from these soils ranged from 4 g N/ha/day, during dry periods, to 4500 g N/ha/day following rainfall events. Nitrous oxide emissions increased with increasing soil moisture. From April through the end of December 1979, a total of 165, 97, and 48 kg N2O-N/ha were emitted from fallow, St. Augustine grass, and sugarcane fields, respectively. There was a diurnal variation in the N2O mixing ratios of air 8 m above the soil in the Everglades. This diurnal fluctuation was affected by wind speed. There was a significant linear correlation between the average daily mixing ratio and the flux of N2O from the soil.  相似文献   

14.
1,2-Dichloroethane (1,2-DCA) is one of the most hazardous pollutant of soil and groundwater, and is produced in excess of 5.44 × 109 kg annually. Owing to their toxicity, persistence and potential for bioaccumulation, there is a growing interest in technologies for their removal. Heavy metals are known to be toxic to soil microorganisms at high concentrations and can hinder the biodegradation of organic contaminants. In this study, the inhibitory effect of heavy metals, namely; arsenic, cadmium, mercury and lead, on the aerobic biodegradation of 1,2-DCA by autochthonous microorganisms was evaluated in soil microcosm setting. The presence of heavy metals was observed to have a negative impact on the biodegradation of 1,2-DCA in both soil samples tested, with the toxic effect being more pronounced in loam soil, than in clay soil. Generally, 75 ppm As3+, 840 ppm Hg2+, and 420 ppm Pb2+ resulted in 34.24%, 40.64%, and 45.94% increase in the half live (t½) of 1,2-DCA, respectively, in loam soil, while concentrations above 127.5 ppm Cd2+, 840 ppm Hg2+ and 420 ppm of Pb2+ and less than 75 ppm As3+ was required to cause a >10% increase in the t½ of 1,2-DCA in clay soil. A dose-dependent relationship between degradation rate constant (k1) of 1,2-DCA and metal ion concentrations was observed for all the heavy metals tested, except for Hg2+. This study demonstrated that different heavy metals have different impacts on the degree of 1,2-DCA degradation. Results also suggest that the degree of inhibition is metal specific and is also dependent on several factors including; soil type, pH, moisture content and available nutrients.  相似文献   

15.
Das S  Ghosh A  Adhya TK 《Chemosphere》2011,84(1):54-62
Combination of divergent active principles to achieve broad-spectrum control is gaining popularity to manage the weed menace in intensive agriculture. However, such application could have non-target impacts on the soil processes affecting soil ecology and environmental interactions. A field experiment was conducted to investigate the impact of separate and combined applications of herbicides bensulfuron methyl and pretilachlor on the emission of N2O and CH4, and related soil and microbial parameters in a flooded alluvial field planted to rice cv Lalat. Single application of the herbicide bensulfuron methyl or pretilachlor resulted in a significant reduction of N2O and CH4 emissions while the combination of these two herbicides distinctly increased N2O and CH4 emissions. Cumulative N2O emissions (kg N2O-N) followed the order of bensulfuron methyl (0.35 kg ha−1) < pretilachlor (0.36 kg ha−1) < control (0.45 kg ha−1) < bensulfuron methyl 0.6% + pretilachlor 6.0% single dose (0.49 kg ha−1) < bensulfuron methyl 0.6% + pretilachlor 6.0% double dose (0.54 kg ha−1). Cumulative CH4 emissions (kg CH4), on the other hand, followed the order of bensulfuron methyl (47.89 kg ha−1) < pretilachlor (73.17 kg ha−1) < bensulfuron methyl 0.6% + pretilachlor 6.0% single dose (93.50 kg ha−1) < control (106.54 kg ha−1) < bensulfuron methyl 0.6% + pretilachlor 6.0% double dose (124.67 kg ha−1). The inhibitory effect of separate application of herbicides bensulfuron methyl 0.6% and pretilachlor 6.0% on N2O emission was linked to lower mineral N, lower denitrifying and nitrifying activity and low denitrifier and nitrifier populations. Inhibitory effect on CH4 emission, on the contrary, was linked to prevention in the drop of redox potential, lower readily mineralizable carbon (RMC) and microbial biomass carbon (MBC) contents as well as lower methanogenic and higher methanotrophic bacterial population. Admittedly, stimulatory effect of combined application of herbicides bensulfuron methyl 0.6% and pretilachlor 6.0% at double dose on N2O and CH4 emission was related to reversal of the identified indicators of inhibition. Results indicate that while individual application of herbicides bensulfuron methyl 0.6% or pretilachlor 6.0% can reduce N2O and CH4 emission from flooded soil planted to rice, their combined application at normal dose can keep the emission at a comparatively lower level with significantly higher grain yield as compared to the herbicides applied alone.  相似文献   

16.
A previously proposed technology incorporating TiO2 into common household fluorescent lighting was further tested for its Hg0 removal capability in a simulated flue-gas system. The flue gas is simulated by the addition of O2, SO2, HCl, NO, H2O, and Hg0, which are frequently found in combustion facilities such as waste incinerators and coal-fired power plants. In the O2 + N2 + Hg0 environment, a Hg0 removal efficiency (ηHg) greater than 95% was achieved. Despite the tendency for ηHg to decrease with increasing SO2 and HCl, no significant drop was observed at the tested level (SO2: 5–300 ppmv, HCl: 30–120 ppmv). In terms of NO and moisture, a significant negative effect on ηHg was observed for both factors. NO eliminated the OH radical on the TiO2 surface, whereas water vapor caused either the occupation of active sites available to Hg0 or the reduction of Hg0 by free electron. However, the negative effect of NO was minimized (ηHg > 90%) by increasing the residence time in the photochemical reactor. The moisture effect can be avoided by installing a water trap before the flue gas enters the Hg0 removal system.

Implications: This paper reports a novel technology for a removal of gas-phase elemental mercury (Hg0) from a simulated flue gas using TiO2-coated glass beads under a low-cost, easily maintainable household fluorescent light instead of ultraviolet (UV) light. In this study, the effects of individual chemical species (O2, SO2, HCl, NO, and water vapor) on the performance of the proposed technology for Hg0 removal are investigated. The result suggests that the proposed technology can be highly effective, even in real combustion environments such as waste incinerators and coal-fired power plants.  相似文献   

17.
ABSTRACT

This article presents the results of an industrial-scale study (on 400 MWe lignite fired unit) of simultaneous NOx, SO2, and HgT removal in FGD absorber with oxidant injection (NaClO2) into flue gas. It was confirmed that the injection of sodium chlorite upstream the FGD (Flue Gas Desulfurization) absorber oxidize NO to NO2, Hg0 to Hg2+, and enhancing NOx and HgT removal efficiency from exhaust gas in FGD absorber. Mercury removal efficiency grows with the rise of degree of oxidation NO to NO2 and was limited by the phenomenon of re-emission. For NOx removal the most critical parameters is slurry pH and temperature. There was no negative effect on sulfur dioxide removal efficiency caused by oxidant injection in tested FGD absorber. Based on the data provided, NOx and HgT emissions can be reduced by adjusting the FGD absorber operating parameters combined with oxidant injection.  相似文献   

18.
Manure-based soil amendments (herein “amendments”) are important fertility sources, but differences among amendment types and management can significantly affect their nutrient value and environmental impacts. A 6-month in situ decomposition experiment was conducted to determine how protection from wintertime rainfall affected nutrient losses and greenhouse gas (GHG) emissions in poultry (broiler chicken and turkey) and horse amendments. Changes in total nutrient concentration were measured every 3 months, changes in ammonium (NH4+) and nitrate (NO3?) concentrations every month, and GHG emissions of carbon dioxide (CO2), methane (CH4), and nitrous oxide (N2O) every 7–14 days. Poultry amendments maintained higher nutrient concentrations (except for K), higher emissions of CO2 and N2O, and lower CH4 emissions than horse amendments. Exposing amendments to rainfall increased total N and NH4+ losses in poultry amendments, P losses in turkey and horse amendments, and K losses and cumulative N2O emissions for all amendments. However, it did not affect CO2 or CH4 emissions. Overall, rainfall exposure would decrease total N inputs by 37% (horse), 59% (broiler chicken), or 74% (turkey) for a given application rate (wet weight basis) after 6 months of decomposition, with similar losses for NH4+ (69–96%), P (41–73%), and K (91–97%). This study confirms the benefits of facilities protected from rainfall to reduce nutrient losses and GHG emissions during amendment decomposition.

Implications: The impact of rainfall protection on nutrient losses and GHG emissions was monitored during the decomposition of broiler chicken, turkey, and horse manure-based soil amendments. Amendments exposed to rainfall had large ammonium and potassium losses, resulting in a 37–74% decrease in N inputs when compared with amendments protected from rainfall. Nitrous oxide emissions were also higher with rainfall exposure, although it had no effect on carbon dioxide and methane emissions. Overall, this work highlights the benefits of rainfall protection during amendment decomposition to reduce nutrient losses and GHG emissions.  相似文献   

19.

Activated carbon was one of the main adsorptions utilized in elemental mercury (Hg0) removal from coal combustion flue gas. However, the high cost and low physical adsorption efficiency of activated carbon injection (ACI) limited its application. In this study, an ultra-high efficiency (nearly 100%) catalyst sorbent-Sex/Activated carbon (Sex/AC) was synthesized and applied to remove Hg0 in the simulated flue gas, which exhibited 120 times outstanding adsorption performance versus the conventional activated carbon. The Sex/AC reached 17.98 mg/g Hg0 adsorption capacity at 160 °C under the pure nitrogen atmosphere. Moreover, it maintained an excellent mercury adsorption tolerance, reaching the efficiency of Hg0 removal above 85% at the NO and SO2 conditions in a bench-scale fixed-bed reactor. Characterized by the multiple methods, including BET, XRD, XPS, kinetic and thermodynamic analysis, and the DFT calculation, we demonstrated that the ultrahigh mercury removal performance originated from the activated Se species in Sex/AC. Chemical adsorption plays a dominant role in Hg0 removal: Selenium anchored on the surface of AC would capture Hg0 in the flue gas to form an extremely stable substance-HgSe, avoiding subsequent Hg0 released. Additionally, the oxygen-containing functional groups in AC and the higher BET areas promote the conversion of Hg0 to HgO. This work provided a novel and highly efficient carbon-based sorbent -Sex/AC to capture the mercury in coal combustion flue gas.

Selenium-modified porous activated carbon and the interface functional group promotes the synergistic effect of physical adsorption and chemical adsorption to promote the adsorption capacity of Hg0.

  相似文献   

20.
The status of the current knowledge concerning the dry deposition of atmospheric mercury, including elemental gaseous mercury (Hg0), reactive gaseous mercury (RGM), and particulate mercury (Hgp), is reviewed. The air–surface exchange of Hg0 is commonly bi-directional, with daytime emission and nighttime deposition over non-vegetated surfaces and vegetated surfaces with small leaf area indices under low ambient Hg0 conditions. However, daytime deposition has also been observed, especially when the ambient Hg0 is high. Typical dry deposition velocities (Vd) for Hg0 are in the range of 0.1–0.4 cm s?1 over vegetated surfaces and wetlands, but substantially smaller over non-vegetated surfaces and soils below canopies. Meteorological, biological, and soil conditions, as well as the ambient Hg0 concentrations all play important roles in the diurnal and seasonal variations of Hg0 air–surface exchange processes. Measurements of RGM deposition are limited and are known to have large uncertainties. Nevertheless, all of the measurements suggest that RGM can deposit very quickly onto any type of surface, with its Vd ranging from 0.5 to 6 cm s?1. The very limited data for Hgp suggest that its Vd values are in the range of 0.02–2 cm s?1.A resistance approach is commonly used in mercury transport models to estimate Vd for RGM and Hgp; however, there is a wide range of complexities in the dry deposition scheme of Hg0. Although resistance-approach based dry deposition schemes seem to be able to produce the typical Vd values for RGM and Hg0 over different surface types, more sophisticated air–surface exchange models have been developed to handle the bi-directional exchange processes. Both existing and newly developed dry deposition schemes need further evaluation using field measurements and intercomparisons within different modelling frameworks.  相似文献   

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