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1.
The aim of this study was to investigate the geochemical characteristics of arsenic in the solid material samples of the Mae Moh Mine and also the Mae Moh power plants fly ash samples were systematically studied. Arsenic concentration in overburden, coal lignite and fly ash are variable (depending on source of solid samples). The results show that the strata of overburden, J seam of coal and fly ash are rich in arsenic and also relatively soluble from fly ash; it occurs as a surface precipitate on the ash particle. The experimental study on speciation in the strata also indicates that the arsenic speciation of Mae Moh solid samples are mainly arsenate, As (V), which are approaching exceed 80%. Arsenic content in the main of overburden is in the range of 14.3–888.8 mg/kg, which is larger than the arsenic background soil values. Solid materials polluted wastewater; the arsenic speciation was present predominantly as arsenate in the surface water of a series of Mae Moh solid materials basins.  相似文献   

2.
An overview is presented on possible mechanisms that control the leaching behaviour of the oxyanion forming elements As, Cr, Mo, Sb, Se, V and W in cementituous systems and alkaline solid wastes, such as municipal solid waste incinerator bottom ash, fly ash and air pollution control residues, coal fly ash and metallurgical slags. Although the leachability of these elements generally depends on their redox state, speciation measurements are not common. Therefore, experimental observations available in the literature are combined with a summary of the thermal behaviour of these elements to assess possible redox states in freshly produced alkaline wastes, given their origin at high temperature. Possible redox reactions occurring at room temperature, on the other hand, are reviewed because these may alter the initial redox state in alkaline wastes and their leachates. In many cases, precipitation of oxyanions as a pure metalate cannot provide a satisfactory explanation for their leaching behaviour. It is therefore highly likely that adsorption and solid solution formation with common minerals in alkaline waste and cement reduce the leachate concentration of oxyanions below pure-phase solubility.  相似文献   

3.
砷在自然界中广泛存在,近年来砷污染对人类健康造成的危害越来越引人关注。微生物在自然界中长期与砷共存,进化出不同的生物转化机制,在自然水体中微生物主要参与砷的不同氧化价态之间的转化过程,即As(V)和As(III)之间的氧化还原作用。砷酸盐异化还原菌（Dissimilatory Arsenate Respiring Prokaryote, DARP）可以将As(V)还原为As(III),化能自养亚砷酸盐氧化菌（Chemoautotrophic Arsenite Oxidizer, CAO）和异养亚砷酸盐氧化菌（Heterotrophic Arsenite Oxidizer, HAO）可以将As(III)氧化为As(V)。这些砷代谢微生物在分类和代谢能力上都具有很大的多样性,它们广泛参与了砷的生物地球化学循环的关键步骤,对特定环境条件下砷的地球化学行为产生重要影响,进而参与了砷的全球循环。在盐碱湖莫诺（Mono）湖中砷的不同价态分层存在,CAO与DARP的紧密偶联共同参与了莫诺湖中的砷的地球化学循环。在孟加拉三角洲的地下含水层中,微生物参与了将砷从固相迁移到水相的关键步骤,最终导致了地下水中的砷污染。  相似文献   

4.
Anthropogenic sources of carbon from landfill or waste leachate can promote reductive dissolution of in situ arsenic (As) and enhance the mobility of As in groundwater. Groundwater from residential-supply wells in a fractured crystalline-rock aquifer adjacent to a Superfund site in Raymond, New Hampshire, USA, showed evidence of locally enhanced As mobilization in relatively reducing (mixed oxic-anoxic to anoxic) conditions as determined by redox classification and other lines of evidence. Redox classification was determined from geochemical indicators based on threshold concentrations of dissolved oxygen (DO), nitrate (NO 3 – ), iron (Fe2+), manganese (Mn2+), and sulfate (SO 4 2– ). Redox conditions were evaluated also based on methane (CH4), excess nitrogen gas (N2) from denitrification, the oxidation state of dissolved As speciation (As(III) and As(V)), and several stable isotope ratios. Samples from the residential-supply wells primarily exhibit mixed redox conditions, as most have long open boreholes (typically 50–100?m) that receive water from multiple discrete fractures with contrasting groundwater chemistry and redox conditions. The methods employed in this study can be used at other sites to gauge redox conditions and the potential for As mobilization in complex fractured crystalline-rock aquifers where multiple lines of evidence are likely needed to understand As occurrence, mobility, and transport.  相似文献   

5.
Systematic changes in mineralogy, enrichment and depletion of selected elements, and mineralogical speciation of selected elements in fly ash and bottom ash samples from the Lingan Power Plant were compared to run-of-mine and pulverized feed coal from the Sydney coalfield, Nova Scotia, eastern Canada. The analytical techniques used were an electron microprobe equipped with energy and wavelength X-ray dispersive spectrometers, X-ray diffraction, neutron activation, scanning electron microscopy with energy dispersive X-ray and incident light petrography. Three types of glasses (Fe/O-rich, Fe/Al/Si/O-rich and or Al/Si/O-rich) were identified in the combustion residues; they were formed as a result of the interaction of melted pyrite and clay minerals. Compared to the feed coal, most elements were enriched 10 to20 times in the fly ash. The concentration of the elements in both the fly ash and bottom ash are comparable to coal ash that is generated by the low temperature asher in the laboratory. Some chalcophile elements such as arsenic and lead occurred as a solid solution in pyrite in the feed coal and were concentrated in the float fraction (density: <2.81 g/cm3) of the fly ash with non-crystalline Fe-oxides. X-ray mapping of arsenic in the fly ash and bottom ash indicates that arsenic was evenly distributed as oxide within the Fe/O- and Fe/Al/Si/O-rich glass and crystalline phases in the fly ash, possibly in solid solution. Arsenic is associated with Fe/O and Fe/S crystalline phases in the bottom ash.  相似文献   

6.
Interplay of S and As in Mekong Delta sediments during redox oscillations   总被引：1，自引：1，他引：0  
The cumulative effects of periodic redox cycling on the mobility of As,Fe,and S from alluvial sediment to groundwater were investigated in bioreactor experiments.Two particular sediments from the alluvial floodplain of the Mekong Delta River were investigated:Matrix A(14 m deep)had a higher pyrite concentration than matrix B(7 m deep)sediments.Gypsum was present in matrix B but absent in matrix A.In the reactors,the sediment suspensions were supplemented with As(Ⅲ)and SO_4~(2-),and were subjected to three full-redox cycles entailing phases of nitrogen/CO_2,compressed air sparging,and cellobiose addition.Major differences in As concentration and speciation were observed upon redox cycling.Evidences support the fact that initial sediment composition is the main factor controlling arsenic release and its speciation during the redox cycles.Indeed,a high pyrite content associated with a low SO_4~(2-)content resulted in an increase in dissolved As concentrations,mainly in the form of As(Ⅲ),after anoxic half-cycles;whereas a decrease in As concentrations mainly in the form of As(Ⅴ),was instead observed after oxic half-cycles.In addition,oxic conditions were found to be responsible for pyrite and arsenian pyrite oxidation,increasing the As pool available for mobilization.The same processes seem to occur in sediment with the presence of gypsum,but,in this case,dissolved As were sequestered by biotic or abiotic redox reactions occurring in the Fe—S system,and by specific physico-chemical condition(e.g.pH).The contrasting results obtained for two sediments sampled from the same core show that many complexes and entangled factors are at work,and further refinement is needed to explain the spatial and temporal variability of As release to groundwater of the Mekong River Delta(Vietnam).  相似文献   

7.
The tailings dam breach at the Ajka alumina plant, western Hungary in 2010 introduced ∼1 million m3 of red mud suspension into the surrounding area. Red mud (fine fraction bauxite residue) has a characteristically alkaline pH and contains several potentially toxic elements, including arsenic. Aerobic and anaerobic batch experiments were prepared using soils from near Ajka in order to investigate the effects of red mud addition on soil biogeochemistry and arsenic mobility in soil–water experiments representative of land affected by the red mud spill. XAS analysis showed that As was present in the red mud as As(V) in the form of arsenate. The remobilisation of red mud associated arsenate was highly pH dependent and the addition of phosphate to red mud suspensions greatly enhanced As release to solution. In aerobic batch experiments, where red mud was mixed with soils, As release to solution was highly dependent on pH. Carbonation of these alkaline solutions by dissolution of atmospheric CO2 reduced pH, which resulted in a decrease of aqueous As concentrations over time. However, this did not result in complete removal of aqueous As in any of the experiments. Carbonation did not occur in anaerobic experiments and pH remained high. Aqueous As concentrations initially increased in all the anaerobic red mud amended experiments, and then remained relatively constant as the systems became more reducing, both XANES and HPLC–ICP-MS showed that no As reduction processes occurred and that only As(V) species were present. These experiments show that there is the potential for increased As mobility in soil–water systems affected by red mud addition under both aerobic and anaerobic conditions.  相似文献   

8.
Disposal of saline subsurface drainage waters from croplands into evaporation basins (or ponds) in the San Joaquin Valley of California causes excessive accumulation of salts and elevated concentrations of arsenic (As), a potentially high risk element with little information about its fate, in the agricultural evaporation ponds. We examined dissolved As concentration, speciation, and distribution in waters as well as As fractionation in sediments in the 10-cell South Evaporation Basin for better understanding of processes and conditions affecting As transformations and fate in a specific drainage disposal facility. The increase of total dissolved As concentrations were observed with higher Cl− and electric conductivity along flow path indicating that evaporation was an important factor regulating total dissolved As concentration. The increases of reduced As species such as arsenite [As(III)] and organic As (monomethylarsonic acid and dimethylarsinic acid) were found towards the terminal flow pathway. However, arsenate [As(V)], the oxidized species remained greater than 67% of total dissolved As in all cell waters. Sequential extractions of sediments indicated that reducing conditions may influence As behavior in sediments to be more soluble and exchangeable. Arsenic association with oxides was appreciable only under oxidizing condition. Carbonate minerals played an important role in immobilizing As into the sediments under alkaline condition and a broad range of redox conditions. However, these sink mechanisms did not significantly reduce As concentrations in the cell waters. The reducing condition facilitated by high concentration of organic matter might be a major factor for the increase in As mobility.  相似文献   

9.
Analytical methods of dissolved Se species in river water and seawater were established and applied to study dissolved Se speciation in the Kaoping and Erhjen rivers and estuaries, southwestern Taiwan. The Kaoping and Erhjen rivers and estuaries were respectively in relatively oxygenated and oxygen-deficient conditions as revealed from the distributions of dissolved oxygen, DOC, nutrients, and dissolved Mn. Concentrations of dissolved total Se increased downstream in the riverine sections, ranging from 0.6 nM to 1.2 nM for the Kaoping River and from 0.8 nM to 1.05 nM for the Erhjen River. The dissolved total Se was only slightly higher in the Erhjen middle estuary than in the Kaoping middle estuary in spite of heavier pollution in the former. The dissolved total Se behaved rather conservatively in the Kaoping estuary but nonconservatively in the Erhjen estuary resulting from anthropogenic inputs, and in this respect showed similarities with the behavior of redox-sensitive Mn. The predominant species of selenium were Se(VI) and organic Se in the Kaoping River and Se(VI) in the Kaoping estuary. The elevated concentration of Se(VI) in the Kaoping estuary may stem from the degradation of organic Se and oxidation of Se(IV). On the other hand, Se(IV) and organic Se were equally dominant in the Erhjen River, and Se(IV) was predominant through most of the Erhjen estuary. The elevated distribution of Se(IV) in the Erhjen middle estuary may result mostly from partial decomposition of organic Se, but further oxidation of Se(IV) was inhibited in reducing waters. However, Se(VI) became dominant at Erhjen outer estuary where water was oxygenated by the replacement of intruded coastal seawater. Apparently, the speciation of dissolved Se was mainly controlled by the biological and redox processes in the Kaoping and Erhjen rivers and estuaries.  相似文献   

10.
Incubation studies were carried out using 5 freshly collected sediments from shallow aquifers of the Hetao Basin, Inner Mongolia. The aquifer sediments covering a range of redox conditions, as indicated by their deep grey to yellow color were mixed with degassed artificial As solution or degassed deionized water at a ratio of solid to water of about 1:10 (wt./wt.). Suspensions which were either amended with glucose or autoclaved, were incubated in parallel with unamended suspensions. Five microcosm cultures of unamended sediments gradually release the equivalent of 0.03–0.30 μg/g As to the dissolved phase. The addition of glucose as a potential electron donor results in a marked stimulation in the mobilization of As (0.71–3.81 μg/g) in the amended incubations for all sediments. The quantity of As released accounts for 60–70% of As bound to Fe/Mn oxides in the original sediments. The microbially mediated mobilization of As with the organic nutrient as an electron donor is strongly associated with the As bound to Fe/Mn oxides, as well as the exchangeable As. During the incubations amended with glucose, 2–4% of the sediment Fe is released. The results suggest that the introduction of labile dissolved organic C into the yellowish sediment aquifers with As-free groundwater would reduce a significant proportion of the Fe(III) oxyhydroxides mediated by anaerobic bacteria respiration and increase groundwater As concentrations.  相似文献   

11.
Generation of dust particles from the Owens Lake playa creates a severe air pollution hazard in the western United States. Much of the dust produced from the dry lakebed is derived from salts formed by evaporation of saline groundwater that often contains high concentrations of dissolved arsenic (As). The objectives of this research were to study the spatial distribution of dissolved arsenic in the shallow groundwater, and to examine factors affecting arsenic solubility and speciation. Evapoconcentration, redox potential, pH, and mineral solubility were examined as factors regulating arsenic biogeochemistry. Dissolved arsenic concentrations ranged from 0.1 to 96 mg L−1 and showed a general increase from the shoreline to the center of the lakebed. Arsenic concentrations were strongly correlated to electrical conductivity (EC) and δD suggesting that evapoconcentration is an important process regulating total As concentrations. Arsenite [As(III)] was the dominant form of inorganic arsenic at Eh values less than about −170 mV while arsenate [As(V)] was predominant at higher Eh values. Organic arsenic was negligible (<0.21%) in all shallow groundwater samples. Dissolved arsenic concentrations do not appear to be strongly regulated by solid-phase reactions. Solid-phase arsenic concentrations generally ranged between 4.0 and 42.6 mg kg−1 and a maximum concentration range (20 to 40 mg kg−1) was reached as solution concentration increased up to 80 mg L−1, indicating minimal sorption and/or precipitation of arsenic. Chemical equilibrium modeling indicated that orpiment (As2S3) was the only solid phase with a positive saturation index (indicating over-saturation), but only at high arsenic and sulfide concentrations. The findings of this research are important for assessing the potential environmental impacts of elevated arsenic concentrations on dust mitigation efforts taking place at Owens Dry Lake.  相似文献   

12.
The accumulation of selenium in evaporation basins (or ponds) in the San Joaquin Valley, California is of a great concern due to its potential hazards to environments. In this study, the accumulation, speciation and concentrations of Se were examined in waters as well as sediments in a system of the evaporation ponds. A significant decrease in the total dissolved Se concentration in Cell 1 in which drainage water with higher Se concentration was pumped from Inlet Channels indicated that the immobilization of Se was active in the Cell 1 and resulted in the higher Se concentration in sediments compared to the terminal cell such as Cell 9. The percentage of reduced Se species such as selenite [Se(IV)] and org-Se of total Se in drainage waters was also found increased in Cell 1 compared to Inlet Channels. The total dissolved Se concentrations in water along flow paths from Cell 1 were relatively constant except for terminal cells such as Cells 9 and 10, which showed higher total dissolved Se concentrations due to evapoconcentration. The percentage of reduced Se forms of total Se was inversely proportional to the percentage of Se(VI) depending on the redox condition of evaporation ponds along the flow paths. Sequential extractions of Se species in sediments indicated that organic associated Se and elemental Se were prevalent forms in sediments in the ponds system. The higher concentrations of elemental Se and organic associated Se in sediments in Cell 1 indicated that the immobilization of Se was active in the sediments compared to Cell 9, while the percentage of both fractions of total Se in sediments in Cells 1 and 9 was relatively constant. The organic materials from algae might provide carbon sources for Se reduction and Se sink in sediments in its elemental and organic associated forms.  相似文献   

13.
We examined the hypothesis that sulfide drives arsenic mobilization from pyritic black shale by a sulfide-arsenide exchange and oxidation reaction in which sulfide replaces arsenic in arsenopyrite forming pyrite, and arsenide (As−1) is concurrently oxidized to soluble arsenite (As+3). This hypothesis was tested in a series of sulfide-arsenide exchange experiments with arsenopyrite (FeAsS), homogenized black shale from the Newark Basin (Lockatong formation), and pyrite isolated from Newark Basin black shale incubated under oxic (21% O2), hypoxic (2% O2, 98% N2), and anoxic (5% H2, 95% N2) conditions. The oxidation state of arsenic in Newark Basin black shale pyrite was determined using X-ray absorption-near edge structure spectroscopy (XANES). Incubation results show that sulfide (1 mM initial concentration) increases arsenic mobilization to the dissolved phase from all three solids under oxic and hypoxic, but not anoxic conditions. Indeed under oxic and hypoxic conditions, the presence of sulfide resulted in the mobilization in 48 h of 13-16 times more arsenic from arsenopyrite and 6-11 times more arsenic from isolated black shale pyrite than in sulfide-free controls. XANES results show that arsenic in Newark Basin black shale pyrite has the same oxidation state as that in FeAsS (−1) and thus extend the sulfide-arsenide exchange mechanism of arsenic mobilization to sedimentary rock, black shale pyrite. Biologically active incubations of whole black shale and its resident microorganisms under sulfate reducing conditions resulted in sevenfold higher mobilization of soluble arsenic than sterile controls. Taken together, our results indicate that sulfide-driven arsenic mobilization would be most important under conditions of redox disequilibrium, such as when sulfate-reducing bacteria release sulfide into oxic groundwater, and that microbial sulfide production is expected to enhance arsenic mobilization in sedimentary rock aquifers with major pyrite-bearing, black shale formations.  相似文献   

14.
To understand the mechanism of arsenic mobilization from sediment to groundwater mediated by microorganism, vertical distribution of bacterial populations in aquifer sediments of the Hetao plain, Inner Mongolia was investigated by a two-step nested PCR-DGGE and 16S rRNA gene clone libraries, combined with sediment geochemistry. A borehole to 30 m depth was drilled and 11 sediment samples were collected. Lithological profile and different geochemical characteristics of sediments indicated a distinct transition of oxidizing–reducing environment along the depth of the sediment core. As(III) and Fe(II) concentrations elevated progressively from 10 m, simultaneously coupling with decrease of As(V) and Fe(III) concentrations, implying that reductive dissolution of arsenic-rich Fe(III) oxyhydroxides led to arsenic release. Results of DGGE displayed that sediment samples with higher concentrations of total arsenic and total organic carbon had lower population diversity, which suggested total arsenic concentrations were important to determine the population diversity of sediments. Bacterial communities of a sediment sample with the highest diversity and ratio of As(III) to total As were dominated by aerobic and facultative anaerobic bacteria and belonged to Alpha-, Beta-, and Gammaproteobacteria and Firmicutes group. Most of the retrieved sequences were closely related to high arsenic-resistance organisms, sulfide/thiosulfate oxidizers, denitrifiers, and aromatic hydrocarbon degraders. Thiobacillus distinctly predominated in clone library, which suggested that arsenic might be released by oxidized dissolution of sulfide minerals coupled to arsenate reduction or nitrate reduction in anaerobic condition. These data have important implications for understanding the microbially mediated arsenic mobilization in aquifers.  相似文献   

15.
李梦娣  周炼  王焰新  吴潇  王帅 《地球科学》2014,39(1):99-107
砷在天然环境中的迁移富集与氧化还原状态密切相关.盆地环境地下水中砷的活化迁移机制主要为沉积物中铁/锰氢氧化物由氧化还原条件变化导致发生还原性溶解进而释放吸附在其表面的砷.钼及钼同位素为氧化还原环境的重要指示参数, 且铁/锰氢氧化物对钼同位素分馏有着重要的控制作用.将地下水的钼同位素应用于砷的活化迁移规律研究.大同盆地地下水中钼同位素比值(δ98Mo)范围为-0.12‰~+2.17‰, 相比于淡水中钼同位素组成偏重.桑干河河水的δ98Mo为+0.72‰, 与文献报道的河水平均钼同位素比值+0.7‰相当.大同盆地地下水中δ98Mo与硫化物之间存在正相关关系, 表明Mo-Fe-S复合物可能形成于特定条件下, 并优先利用水溶液中轻的钼使地下水中δ98Mo比值升高.砷浓度与钼浓度之间的微弱负相关以及砷浓度与钼同位素之间的正相关说明, Mo-Fe-S的形成过程可能与同环境中As-Fe-S的复合物的形成存在竞争关系, 进而使得地下水中砷富集.地下水中相对偏高的δ98Mo可能来源于铁的氢氧化物对溶液中轻的钼的吸附速率高于先前吸附在铁的氢氧化物的钼的释放, 且铁的氢氧化物对水溶液中钼的再吸附这一循环过程会导致地下水中钼浓度降低及钼同位素比值的升高.钼同位素指示的循环性的铁的氢氧化物的还原溶解及再氧化过程对砷的富集也有重要影响.   相似文献   

16.
A laboratory investigation was carried out to examine the mechanism of arsenic (As) mobilization under flooded conditions (24 and 240 h) in 18 alluvial soils of Punjab, North–West India. Total dissolved As increased from a range of 3–16 μg L?1 (mean 9 μg L?1) to a range of 33–1,761 μg L?1 (mean 392 μg L?1) with the increase in flooding period from 24 to 240 h. The amount of As mobilization varied depending upon redox potential (pe) created by flooding conditions. After 24 h of flooded conditions, pe of soil water suspension ranged from ?1.75 to 0.77 (mean ?0.24). Increasing the flooding period to 240 h, pe of soil water suspension decreased in the range of ?4.49 to ?2.74 (mean ?3.29). Pourbaix diagram identified arsenate (HAsO4 2?) as predominant species in most of the alluvial soil–water suspensions under oxidized conditions, after 24 h of equilibration period, which ultimately transformed to arsenite (H3AsO3 0) after 240 h of anaerobic condition due to more reduced status. The solid phase identified was orpiment (As2S3). Identification of iron and manganese species in alluvial soil water suspension by Pourbaix diagram indicated decline in both soluble Fe2+ and SO4 2? concentration due to the formation of iron sulfide mineral phase after 240 h under anaerobic conditions. In these soils, decline in soluble Fe was also due to the precipitation of vivianite [Fe3(PO4)2·8H2O]. Elevated arsenic content and low pe value were measured in aquifers located in paddy growing fields comparative to aquifers of other sites. Large degree of variability in As concentrations was recorded in aquifers located at same sites. Thus, it is better to analyze each aquifer for their As content rather than to depends on the prediction on As content of neighbouring wells. The present investigation elucidates that flood irrigation practices in Punjab for growing paddy crop could induce the geochemical conditions favorable to mobilize arsenic from surface soils which could eventually elevate its content in the underlying shallow aquifers. Water abstracted from these aquifers by hand pumps or tube wells for drinking purposes could create hazards for local population due to loading with arsenic concentration above the safe limits. Thus, to avoid further contamination of shallow aquifers with arsenic, it is advisable to shift the flooded rice cultivation to other upland crops having lesser water requirement.  相似文献   

17.
煤中As的赋存状态及其在燃烧过程中的转化   总被引：1，自引：0，他引：1  
对煤中砷的赋存状态进行了综述,总结了砷在燃煤过程中的迁移转化行为。从飞灰演化的角度探讨了飞灰对砷的富集机制,认为飞灰对砷的富集是伴随飞灰的演化过程进行的。飞灰对砷的富集主要有4种形式,即发生化学反应生成含砷稳定化合物,进入粘土矿物晶格内部,飞灰对砷及其化合物的吸附和冷凝   相似文献   

18.
Wetlands are significant sources and sinks for arsenic (As), yet the geochemical conditions and processes causing a release of dissolved arsenic and its association with the solid phase of wetland soils are poorly known. Here we present experiments in which arsenic speciation was determined in peatland mesocosms in high spatiotemporal resolution over 10 months. The experiment included a drought/rewetting treatment, a permanently wet, and a defoliated treatment. Soil water content was determined by the TDR technique, and arsenic, iron and sulfate turnover from mass balancing stocks and fluxes in the peat, and solid phase contents by sequential extractions. Arsenic content ranged from 5 to 25 mg kg−1 and dissolved concentrations from 10 to 300 μg L−1, mainly in form of As(III), and secondarily of As(V) and dimethylated arsenic (DMA). Total arsenic was mainly associated with amorphous iron hydroxides (R2 > 0.95, α < 0.01) and deeper into the peat with an unidentified residual fraction. Arsenic release was linked to ferrous iron release and primarily occurred in the intensely rooted uppermost soil. Volumetric air contents of 2-13 % during drought eliminated DMA from the porewater and suppressed its release after rewetting for >30 d. Dissolved As(III) was oxidized and immobilized as As(V) at rates of up to 0.015 mmol m−3 d−1. Rewetting mobilized As(III) at rates of up to 0.018 mmol m−3 d−1 within days. Concurrently, Fe(II) was released at depth integrated rates of up 20 mmol m−3 d−1. The redox half systems of arsenic, iron, and sulfur were in persistent disequilibrium, with H2S being a thermodynamically viable reductant for As(V) to As(III). The study suggests that rewetting can lead to a rapid release of arsenic in iron-rich peatlands and that methylation is of lesser importance than co-release with iron reduction, which was largely driven by root activity.  相似文献   

19.
为探析长江口沉积物-水界面砷的迁移转化机制,本文分析了2019年夏季长江口4个站位上覆水和间隙水中总As浓度及形态的剖面变化特征,耦合氧化还原敏感元素(Fe、Mn和S)的剖面变化剖析了沉积物-水界面砷循环的Fe-Mn-S控制机制,同时结合砷相关功能基因探讨了沉积物-水界面砷迁移转化的微生物调控过程,估算了沉积物-水界面总As的扩散通量。结果表明,除A7-4站位外,长江口其他3个站位间隙水总As以As3+为主要存在形态,且总As浓度均在上覆水中为最低值(0.748~1.57 μg·L-1),而在间隙水中随着深度增加而逐渐增加并在6~9 cm深度达到峰值(7.14~26.9 μg·L-1)。间隙水总As及As3+浓度的剖面变化趋势与溶解态Fe2+、Mn2+相似,其均在中间层出现高值,说明沉积物Fe/Mn还原带砷的释放可能是随固相Fe(Ⅲ)或Mn(Ⅳ)的还原而转移到间隙水中的。氧化层和Fe/Mn还原带过渡区间隙水砷浓度与砷异化还原菌功能基因arrA和arsC丰度存在对应关系(除A1-3站外),说明砷异化还原菌将溶解As5+或固相As5+还原为溶解As3+可能是该过渡层砷迁移转化的另一重要过程。硫酸盐还原带的间隙水总As和As3+浓度降低,但由于间隙水的低S2-浓度不利于砷硫化物生成,因此深层间隙水砷可能与铁硫矿物结合而被移除。底层环境氧化还原条件是影响沉积物-水界面砷迁移转化的重要因素,随底层水DO浓度的降低,砷迁移转化更倾向于微生物还原控制。长江口沉积物-水界面总As的扩散通量为1.18×10-7~2.07×10-7 μmol·cm-2·s-1,均表现为沉积物间隙水中总As向上覆水释放,即沉积物是研究区域水体总As的来源之一。  相似文献   

20.
Radiolabelled assays and compound-specific stable isotope analysis (CSIA) were used to assess methyl tert-butyl ether (MTBE) biodegradation in an unleaded fuel plume in a UK chalk aquifer, both in the field and in laboratory microcosm experiments. The 14C-MTBE radiorespirometry studies demonstrated widespread potential for aerobic and anaerobic MTBE biodegradation in the aquifer. However, δ13C compositions of MTBE in groundwater samples from the plume showed no significant 13C enrichment that would indicate MTBE biodegradation at the field scale. Carbon isotope enrichment during MTBE biodegradation was assessed in the microcosms when dissolved O2 was not limiting, compared with low in situ concentrations (2 mg/L) in the aquifer, and in the absence of O2. The microcosm experiments showed ubiquitous potential for aerobic MTBE biodegradation in the aquifer within hundreds of days. Aerobic MTBE biodegradation in the microcosms produced an enrichment of 7‰ in the MTBE δ13C composition and an isotope enrichment factor (ε) of −1.53‰ when dissolved O2 was not limiting. However, for the low dissolved O2 concentration of up to 2 mg/L that characterizes most of the MTBE plume fringe, aerobic MTBE biodegradation produced an enrichment of 0.5-0.7‰, corresponding to an ε value of −0.22‰ to −0.24‰. No anaerobic MTBE biodegradation occurred under these experimental conditions. These results suggest the existence of a complex MTBE-biodegrading community in the aquifer, which may consist of different aerobic species competing for MTBE and dissolved O2. Under low O2 conditions, the lower fractionating species have been shown to govern overall MTBE C-isotope fractionation during biodegradation, confirming the results of previous laboratory experiments mixing pure cultures. This implies that significant aerobic MTBE biodegradation could occur under the low dissolved O2 concentration that typifies the reactive fringe zone of MTBE plumes, without producing detectable changes in the MTBE δ13C composition. This observed insensitivity of C isotope enrichment to MTBE biodegradation could lead to significant underestimation of aerobic MTBE biodegradation at field scale, with an unnecessarily pessimistic performance assessment for natural attenuation. Site-specific C isotope enrichment factors are, therefore, required to reliably quantify MTBE biodegradation, which may limit CSIA as a tool for the in situ assessment of MTBE biodegradation in groundwater using only C isotopes.  相似文献   

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