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1.
Long-term mercury dynamics in UK soils   总被引:1,自引:0,他引:1  
A model assuming first-order losses by evasion and leaching was used to evaluate Hg dynamics in UK soils since 1850. Temporal deposition patterns of Hg were constructed from literature information. Inverse modelling indicated that 30% of 898 rural sites receive Hg only from the global circulation, while in 51% of cases local deposition exceeds global. Average estimated deposition is 16 μg Hg m−2 a−1 to rural soils, 19 μg Hg m−2 a−1 to rural and non-rural soils combined. UK soils currently hold 2490 tonnes of reactive Hg, of which 2140 tonnes are due to anthropogenic deposition, mostly local in origin. Topsoil currently releases 5.1 tonnes of Hg0 per annum to the atmosphere, about 50% more than the anthropogenic flux. Sorptive retention of Hg in the lower soil exerts a strong control on surface water Hg concentrations. Following decreases in inputs, soil Hg concentrations are predicted to decline over hundreds of years.  相似文献   

2.
The first attempt to systematically investigate the atmospheric mercury (Hg) in the MBL of the Augusta basin (SE Sicily, Italy) has been undertaken. In the past the basin was the receptor for Hg from an intense industrial activity which contaminated the bottom sediments of the Bay, making this area a potential source of pollution for the surrounding Mediterranean. Three oceanographic cruises have been thus performed in the basin during the winter and summer 2011/2012, where we estimated averaged Hgatm concentrations of about 1.5 ± 0.4 (range 0.9–3.1) and 2.1 ± 0.98 (range 1.1–3.1) ng m−3 for the two seasons, respectively. These data are somewhat higher than the background Hgatm value measured over the land (range 1.1 ± 0.3 ng m−3) at downtown Augusta, while are similar to those detected in other polluted regions elsewhere. Hg evasion fluxes estimated at the sea/air interface over the Bay range from 3.6 ± 0.3 (unpolluted site) to 72 ± 0.1 (polluted site of the basin) ng m−2 h−1. By extending these measurements to the entire area of the Augusta basin (∼23.5 km2), we calculated a total sea–air Hg evasion flux of about 9.7 ± 0.1 g d−1 (∼0.004 t yr−1), accounting for ∼0.0002% of the global Hg oceanic evasion (2000 t yr−1). The new proposed data set offers a unique and original study on the potential outflow of Hg from the sea–air interface at the basin, and it represents an important step for a better comprehension of the processes occurring in the marine biogeochemical cycle of this element.  相似文献   

3.
The median total mercury concentration in 898 UK rural topsoils, sampled between 1998 and 2008, was 0.095 μg g−1. Approximate adjustment for unreactive metal produced an estimate of 0.052 μg g−1 for reactive Hg. The highest concentrations were in the north and west, where organic-rich soils with low bulk densities dominate, but the spatial pattern was quite different if soil Hg pools (mg m−2) were considered, the highest values being near to the industrial north of England and London. Possible toxic effects of Hg were best evaluated by comparison with soil Critical Limits expressed as ratios of Hg to soil organic matter, or soil solution Hg2+ concentrations, estimated by chemical speciation modelling. Only a few percent of the rural UK soils showed exceedance, and this also applied to rural soils from the whole of Europe. UK urban and industrial soils had higher Hg concentrations and more cases of exceedance.  相似文献   

4.
Mt. Gongga area in southwest China was impacted by Hg emissions from industrial activities and coal combustion, and annual means of atmospheric TGM and PHg concentrations at a regional background station were 3.98 ng m−3 and 30.7 pg m−3, respectively. This work presents a mass balance study of Hg in an upland forest in this area. Atmospheric deposition was highly elevated in the study area, with the annual mean THg deposition flux of 92.5 μg m−2 yr−1. Total deposition was dominated by dry deposition (71.8%), and wet deposition accounted for the remaining 28.2%. Forest was a large pool of atmospheric Hg, and nearly 76% of the atmospheric input was stored in forest soil. Volatilization and stream outflow were identified as the two major pathways for THg losses from the forest, which yielded mean output fluxes of 14.0 and 8.6 μg m−2 yr−1, respectively.  相似文献   

5.
Seasonal patterns of atmospheric mercury (Hg) fluxes measured over vegetated terrestrial systems can provide insight into the underlying process controlling emission and deposition of Hg to vegetated surfaces. Gaseous elemental Hg fluxes were measured for week-long periods in each season (spring, summer, fall, and winter) over an uncontaminated high-elevation wetland meadow in Shenandoah National Park, Virginia using micrometeorological methods. Mean net deposition was observed in the spring (?4.8 ng m?2 h?1), emission in the summer (2.5 ng m?2 h?1), near zero flux in the fall (0.3 ng m?2 h?1), and emission in the winter (4.1 ng m?2 h?1). Nighttime deposition (when stomata are closed) and the poor correlation between Hg fluxes and canopy conductance during periods of active vegetation growth suggest that stomatal processes are not the dominant mechanism for ecosystem-level GEM exchange at this site. The strong springtime deposition relative to summer implies that young vegetation is better at scavenging Hg, with the highest deposition occurring at night possibly via a cuticular pathway. These results suggest that spring is a period of GEM deposition while other seasons exhibit net emission, emphasizing the importance of capturing GEM flux seasonality when determining total Hg budgets.  相似文献   

6.
Si L  Ariya PA 《Chemosphere》2011,84(8):1079-1084
Mercury is a global environmental contaminant with severe toxicity impact. The chemical processes resulting in the transformation of oxidized mercury species (Hg2+) to elemental mercury (Hg0), greatly affects the fate and transport of mercury in the natural environment. We hereby provide the first study on the photochemistry of Hg2+ with selected alkanethiols (R-SH) as model compounds to represent thiols and thiol-type binding sites on humic substances in natural waters because of the common sulfhydryl functional group (-SH). Kinetic studies were performed using cold vapor atomic fluorescence spectroscopy (CVAFS), the formation of Hg2+-thiol complexes (Hg(SR)2) were confirmed by UV-visible spectrometry and Atmospheric Pressure Chemical Ionization-Mass Spectrometry (APCI-MS), and the reaction products were analyzed using Electron Impact-Mass Spectrometry (EI-MS) and Solid Phase Microextraction coupled with Gas Chromatography-Mass Spectrometry (SPME/GC-MS). Our results indicated that the photoreduction of Hg2+ by selected alkanethiols may be mediated by Hg2+-thiol complexes to produce Hg0. Under our experimental conditions, the apparent first order rate constants obtained for 1-propanethiol, 1-butanethiol, and 1-pentanethiol were (2.0 ± 0.2) × 10−7 s−1, (1.4 ± 0.1) × 10−7 s−1, (8.3 ± 0.5) × 10−8 s−1, respectively. The effects of ionic strength, dissolved oxygen or chloride ion on reaction rates were found to be minimal under our experimental conditions. The identified products of the reaction between oxidized mercury species with selected alkanethiols (C3-C5) were Hg0 and disulfides (RS-SR). The potential environmental implications are herein discussed.  相似文献   

7.
Accumulation of total and methyl-Hg by mushrooms and earthworms was studied in thirty-four natural forest soils strongly varying in soil physico-chemical characteristics. Tissue Hg concentrations of both receptors did hardly correlate with Hg concentrations in soil. Both total and methyl-Hg concentrations in tissues were species-specific and dependent on the ecological groups of receptor. Methyl-Hg was low accounting for less than 5 and 8% of total Hg in tissues of mushrooms and earthworms, respectively, but with four times higher concentrations in earthworms than mushrooms. Total Hg concentrations in mushrooms averaged 0.96 mg Hg kg−1 dw whereas litter decomposing mushrooms showed highest total Hg and methyl-Hg concentrations. Earthworms contained similar Hg concentrations (1.04 mg Hg kg−1 dw) whereas endogeic earthworms accumulated highest amounts of Hg and methyl-Hg.  相似文献   

8.
To investigate the characteristics of mercury exchange between soil and air in the heavily air-polluted area, total gaseous mercury (TGM) concentration in air and Hg exchange flux were measured in Wanshan Hg mining area (WMMA) in November, 2002 and July–August, 2004. The results showed that the average TGM concentrations in the ambient air (17.8–1101.8 ng m−3), average Hg emission flux (162–27827 ng m−2 h−1) and average Hg dry deposition flux (0–9434 ng m−2 h−1) in WMMA were 1–4 orders of magnitude higher than those in the background area. It is said that mercury-enriched soil is a significant Hg source of the atmosphere in WMMA. It was also found that widely distributed roasted cinnabar banks are net Hg sources of the atmosphere in WMMA. Relationships between mercury exchange flux and environmental parameters were investigated. The results indicated that the rate of mercury emission from soil could be accelerated by high total soil mercury concentration and solar irradiation. Whereas, highly elevated TGM concentrations in the ambient air can restrain Hg emission from soil and even lead to strongly atmospheric Hg deposition to soil surface. A great amount of gaseous mercury in the heavily polluted atmosphere may cycle between soil and air quickly and locally. Vegetation can inhibit mercury emission from soil and are important sinks of atmospheric mercury in heavily air-polluted area.  相似文献   

9.
Szopka K  Karczewska A  Kabała C 《Chemosphere》2011,83(11):1507-1512
The study was aimed to examine total concentrations and pools of Hg in surface layers of soils in the Karkonosze Mountains, dependent on soil properties and site locality. Soil samples were collected from a litter layer and the layers 0-10 cm and 10-20 cm, at 68 sites belonging to the net of a monitoring system, in two separate areas, and in three altitudinal zones: below 900 m, 900-1100 m, and over 1100 m. Air-borne pollution was the major source of mercury in soils. Hg has accumulated mainly in the litter (where its concentrations were the highest), and in the layer 0-10 cm. Hg concentrations in all samples were in the range 0.04-0.97 mg kg−1, with mean values 0.38, 0.28, and 0.14 mg kg−1 for litter and the layers 0-10 cm and 10-20 cm, respectively. The highest Hg concentrations in the litter layer were found in the intermediate altitudinal zone, whereas Hg concentrations in the layer 0-10 cm increased with increasing altitude. Soil quality standard for protected areas (0.50 mg kg−1) was exceeded in a few sites. The pools of Hg accumulated in soils were in the range: 0.8-84.8 mg m−2, with a mean value of 16.5 mg m−2, and they correlated strongly with the pools of stored organic matter.  相似文献   

10.
Five weeks of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particle bound mercury (Hgp) concentrations as well as fluxes of GEM were measured at Maryhill, Ontario, Canada above a biosolids amended field. The study occurred during the autumn of 2004 (October–November) to capture the effects of cool weather conditions on the behaviour of mercury in the atmosphere. The initial concentration of total mercury (Hg) in the amended soil was relatively low (0.4 μg g−1±10%).A micrometeorological approach was used to infer the flux of GEM using a continuous two-level sampling system with inlets at 0.40 and 1.25 m above the soil surface to measure the GEM concentration gradient. The required turbulent transfer coefficients were derived from meteorological parameters measured on site. The average GEM flux over the study was 0.1±0.2 ng m−2 h−1(±one standard deviation). The highest averaged hourly GEM fluxes occurred when the averaged net radiation was highest, although the slight diurnal patterns observed were not statistically significant for the complete flux data series. GEM emission fluxes responded to various local events including the passage of a cold front when the flux increased to 2 ng m−2 h−1 and during a biosolids application event at an adjacent field when depositional fluxes peaked at −3 ng m−2 h−1. Three substantial rain events during the study kept the surface soil moisture near field capacity and only slightly increased the GEM flux. Average concentrations of RGM (2.3±3.0 pg m−3), Hgp (3.0±6.2 pg m−3) and GEM (1.8±0.2 ng m−3) remained relatively constant throughout the study except when specific local events resulted in elevated concentrations. The application of biosolids to an adjacent field produced large increases in Hgp (25.8 pg m−3) and RGM (21.7 pg m−3) concentrations only when the wind aligned to impact the experimental equipment. Harvest events (corn) in adjacent fields also corresponded to higher concentrations of GEM and Hgp but with no elevated peaks in RGM concentrations. Diurnal patterns were not statistically significant for RGM and Hgp at Maryhill.  相似文献   

11.
Critical Limits for Hg(II) in soils, derived from chronic toxicity data   总被引:1,自引:0,他引:1  
Published chronic toxicity data for Hg(II) added to soils were assembled and evaluated to produce a data set comprising 52 chronic end-points, five each for plants and invertebrates and 42 for microbes. With end-points expressed in terms of added soil Hg(II) contents, Critical Limits were derived from the 5th percentiles of species sensitivity distributions, values of 0.13 μg (g soil)−1 and 3.3 μg (g soil organic matter)−1 being obtained. The latter value exceeds the currently recommended Critical Limit, used to determine Hg(II) Critical Loads in Europe, of 0.5 μg (g soil organic matter)−1. We also applied the WHAM/Model VI chemical speciation model to estimate concentrations of Hg2+ in soil solution, and derived an approximate Critical Limit Function (CLF) that includes pH; log [Hg2+]crit = −2.15 pH −17.10. Because they take soil properties into account, the soil organic matter-based limit and the CLF provide the best assessment of toxic threat for different soils. For differing representative soils, each predicts a range of up to 100-fold in the dry weight-based content of mercury that corresponds to the Critical Limit.  相似文献   

12.
Daily ozone deposition flux to a Norway spruce forest in Czech Republic was measured using the gradient method in July and August 2008. Results were in good agreement with a deposition flux model. The mean daily stomatal uptake of ozone was around 47% of total deposition. Average deposition velocity was 0.39 cm s−1 and 0.36 cm s−1 by the gradient method and the deposition model, respectively. Measured and modelled non-stomatal uptake was around 0.2 cm s−1. In addition, net ecosystem production (NEP) was measured by using Eddy Covariance and correlations with O3 concentrations at 15 m a.g.l., total deposition and stomatal uptake were tested. Total deposition and stomatal uptake of ozone significantly decreased NEP, especially by high intensities of solar radiation.  相似文献   

13.
Atmospheric elemental, reactive and particulate mercury (Hg) concentrations were measured north of downtown Reno, Nevada, USA from November 2004 to November 2007. Three-year mean and median concentrations for gaseous elemental Hg (Hg0) were 1.6 and 1.5 ng m−3 (respectively), similar to global mean Hg0 concentrations. The three-year mean reactive gaseous Hg (RGM) concentration (26 pg m−3) was higher than values reported for rural sites across the western United States. Well defined seasonal and daily patterns in Hg0 and RGM concentrations were observed, with the highest Hg0 concentrations measured in winter and early morning, and RGM concentrations being greatest in the summer and mid-afternoon. Elevated Hg0 concentrations in winter were associated with periods of cold, stagnant air; while a regularly observed early morning increase in concentration was due to local source and surface emissions. The observed afternoon increase and high summer values of RGM can be explained by in situ oxidation of gaseous Hg0 or mixing of RGM derived from the free troposphere to the surface. Because both of these processes are correlated with the same environmental conditions it is difficult to assess their overall contribution to the observed trends.  相似文献   

14.
The study of mercury (Hg) cycle in Arctic regions is a major subject of concern due to the dramatic increases of Hg concentrations in ecosystem in the last few decades. The causes of such increases are still in debate, and an important way to improve our knowledge on the subject is to study the exchanges of Hg between atmosphere and snow during springtime. We organized an international study from 10 April to 10 May 2003 in Ny-Ålesund, Svalbard, in order to assess these fluxes through measurements and derived calculations.Snow-to-air emission fluxes of Hg were measured using the flux chamber technique between ∼0 and 50 ng m−2 h−1. A peak in Gaseous Elemental Mercury (GEM) emission flux from the snow to the atmosphere has been measured just few hours after an Atmospheric Mercury Depletion Event (AMDE) recorded on 22 April 2004. Surprisingly, this peak in GEM emitted after this AMDE did not correspond to any increase in Hg concentration in snow surface. A peak in GEM flux after an AMDE was observed only for this single event but not for the four other AMDEs recorded during this spring period.In the snow pack which is seasonal and about 40 cm depth above permafrost, Hg is involved in both production and incorporation processes. The incorporation was evaluated to ∼5–40 pg m2 h. Outside of AMDE periods, Hg flux from the snow surface to the atmosphere was the consequence of GEM production in the air of snow and was about ∼15–50 ng m−2 h−1, with a contribution of deeper snow layers evaluated to ∼0.3–6.5 ng m−2 h−1. The major part of GEM production is then mainly a surface phenomenon. The internal production of GEM was largely increasing when snow temperatures were close to melting, indicating a chemical process occurring in the quasi-liquid layer at the surface of snow grains.  相似文献   

15.
Atmospheric mercury (Hg) species, including gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particulate-bound mercury (Hgp), were monitored near three sites, including a cement plant (monitored in 2007 and 2008), an urban site and a rural site (both monitored in 2005 and 2008). Although the cement plant was a significant source of Hg emissions (for 2008, GEM: 2.20 ± 1.39 ng m?3, RGM: 25.2 ± 52.8 pg m?3, Hgp 80.8 ± 283 pg m?3), average GEM levels and daytime average dry depositional RGM flux were highest at the rural site, when all three sites were monitored sequentially in 2008 (rural site, GEM: 2.37 ± 1.26 ng m?3, daytime RGM flux: 29 ± 40 ng m?2 day?1). Photochemical conversion of GEM was not the primary RGM source, as highest net RGM gains (75.9 pg m?3, 99.0 pg m?3, 149 m?3) occurred within 3.0–5.3 h, while the theoretical time required was 14–23 h. Instead, simultaneous peaks in RGM, Hgp, ozone (O3), nitrogen oxides, and sulfur dioxide in the late afternoon suggested short-range transport of RGM from the urban center to the rural site. The rural site was located more inland, where the average water vapor mixing ratio was lower compared to the other two sites (in 2008, rural: 5.6 ± 1.4 g kg?1, urban: 9.0 ± 1.1 g kg?1, cement plant: 8.3 ± 2.2 g kg?1). Together, these findings suggested short-range transport of O3 from an urban area contributed to higher RGM deposition at the rural site, while drier conditions helped sustain elevated RGM levels. Results suggested less urbanized environments may be equally or perhaps more impacted by industrial atmospheric Hg emissions, compared to the urban areas from where Hg emissions originated.  相似文献   

16.
Four seasonal sampling campaigns were carried out in the Florida Everglades to measure elemental Hg vapor (Hg°) fluxes over emergent macrophytes using a modified Bowen ratio gradient approach. The predominant flux of Hg° over both invasive cattail and native sawgrass stands was emission; mean day time fluxes over cattail ranged from ∼20 (winter) to ∼40 (summer) ng m−2 h−1. Sawgrass fluxes were about half those over cattail during comparable periods. Emission from vegetation significantly exceeded evasion of Hg° from the underlying water surface (∼1–2 ng m−2 h−1) measured simultaneously using floating chambers. Among several environmental factors (e.g. CO2 flux, water vapor flux, wind speed, water, air and leaf temperature, and solar radiation), water vapor exhibited the strongest correlation with Hg° flux, and transpiration is suggested as an appropriate term to describe this phenomenon. The lack of significant Hg° emissions from a live, but uprooted (floating) cattail stand suggests that a likely source of the transpired Hg° is the underlying sediments. The pattern of Hg° fluxes typically measured indicated a diel cycle with two peaks, possibly related to different gas exchange dynamics: one in early morning related to lacunal gas release, and a second at midday related to transpiration; nighttime fluxes approached zero.  相似文献   

17.
The estimated annual throughfall deposition flux of Hg in a northern mixed-hardwood forest in the Lake Huron Watershed was 10.5±1.0 μg m−2 compared to an annual precipitation Hg flux of 8.7±0.5 μg m−2 (June 1996–June 1997). The source of this additional Hg in throughfall is often attributed to wash-off of dry deposition, but foliar leaching of Hg may also be important. To determine the influence of both dry deposition and foliar leaching of Hg and other elements in throughfall, we measured a suite of trace elements (Hg, Al, Mg, V, Mn, Cu, Zn, As, Rb, Sr, Cd, Ba, La, Ce, and Pb) in throughfall, precipitation, and ambient air samples from a northern mixed-hardwood forest. Based on a multiple linear regression model, dry deposition had the most important influence on Hg, Al, La, Ce, V, As, Cu, Zn, Cd, and Pb fluxes while foliar leaching strongly influenced Mg, Mn, Rb, Sr, and Ba fluxes in net throughfall. The Hg dry deposition flux was estimated using gaseous and aerosol Hg measurements and modeled deposition velocities. The calculated dry deposition flux (∼12–14 μg m−2) of Hg to the canopy indicated that atmospheric deposition of Hg could easily account for all of the Hg deposited in net throughfall (1.9±0.1 μg m−2). Although there is a large uncertainty associated with these techniques, the modeling estimates indicate that atmospheric Hg may account for all of the Hg deposited in litterfall (11.4±2.8 μg m−2).  相似文献   

18.
Lake-sediment records across the Northern Hemisphere show increases in atmospheric deposition of anthropogenic mercury (Hg) over the last 150 years. Most of the previous studies have examined remote lakes affected by the global atmospheric Hg reservoir. In this study, we present Hg flux records from lakes in an urban/suburban setting of central New York affected also by local and regional emissions. Sediment cores were collected from the Otisco and Skaneateles lakes from the Finger Lakes region, Cross Lake, a hypereutrophic lake on the Seneca River, and Glacial Lake, a small seepage lake with a watershed that corresponds with the lake area. Sediment accumulation rates and dates were established by 210Pb. The pre-anthropogenic regional atmospheric Hg flux was estimated to be 3.0 μg m−2 yr−1 from Glacial Lake, which receives exclusively direct atmospheric deposition. Mercury fluxes peaked during 1971–2001, and were 3 to more than 30 times greater than pre-industrial deposition. Land use change and urbanization in the Otisco and Cross watersheds during the last century likely enhanced sediment loads and Hg fluxes to the lakes. Skaneateles and Glacial lakes have low sediment accumulation rates, and thus are excellent indicators for atmospheric Hg deposition. In these lakes, we found strong correlations with emission records for the Great Lakes region that markedly increased in the early 1900s, and peaked during WWII and in the early 1970s. Declines in modern Hg fluxes are generally evident in the core records. However, the decrease in sediment Hg flux at Glacial Lake was interrupted and has increased since the early 1990s probably due to the operation of new local emission sources. Assuming the global Hg reservoir tripled since the pre-industrial period, the contribution of local and regional emission sources to central New York lakes was estimated to about 80% of the total atmospheric Hg deposition.  相似文献   

19.
The composition of landfill gas (LFG) was analyzed for vapor-phase mercury (Hg) (primarily in its elemental form, Hg0) and relevant environmental parameters from 42 out of 106 ventpipes placed across two different sectors of the Nan-Ji-Do (NJD) landfill site in Seoul, Korea during September/October 2000. Results of our studies showed that large quantities of Hg emanated through these ventpipes which were infiltrated deep into the waste layer. The mean concentration of Hg, computed using the data sets collected from 42 ventpipes, was 420 ng m−3 with a range of 3.45–2952 ng m−3. Because large differences were apparent in its concentration levels not only between the two sectors of 1 and 2 but also between the plain and slope areas, evaluation of the data was made by dividing them into four different categories, namely plain areas of sectors 1 and 2 and slope areas of sectors 1 and 2. By categorizing the data in such a manner, the emission fluxes of ventilated Hg were estimated for each data group at the NJD site. The flux values of Hg for each data group were distinguished so that the enhanced fluxes were observed in plain compared to slope areas. The computed LFG fluxes of Hg from the whole NJD site were on the order of 23 g on an annual basis. The overall results of our study suggest that the vent emission of Hg from the study site is comparable in magnitude to those reported previously (e.g., the Florida landfill sites in US), while the LFG emissions of Hg may not necessarily be the most dominant source in the NJD site.  相似文献   

20.
Changes in deposition of gaseous divalent mercury (Hg(II)) and particulate mercury (Hg(p)) in New Hampshire due to changes in local sources from 1996 to 2002 were assessed using the Industrial Source Complex Short Term (ISCST3) model (regional and global sources and Hg atmospheric reactions were not considered). Mercury (Hg) emissions in New Hampshire and adjacent areas decreased significantly (from 1540 to 880 kg yr−1) during this period, and the average annual modeled deposition of total Hg also declined from 17 to 7.0 μg m−2 yr−1 for the same period. In 2002, the maximum amount of Hg deposition was modeled to be in southern New Hampshire, while for 1996 the maximum deposition occurred farther north and east. The ISCST3 was also used to evaluate two future scenarios. The average percent difference in deposition across all cells was 5% for the 50% reduction scenario and 9% for the 90% reduction scenario.  相似文献   

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