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1.
The build-up of methane in the hypolimnion of the eutrophic Lake Rotsee (Lucerne, Switzerland) was monitored over a full year. Sources and sinks of methane in the water column were characterized by measuring concentrations and carbon isotopic composition. In fall, high methane concentrations (up to 1 mM) were measured in the anoxic water layer. In the oxic layer, methane concentrations were much lower and the isotopic composition shifted towards heavy carbon isotopes. Methane oxidation rates peaked at the interface between oxic and anoxic water layers at around 8–10 m depth. The electron balance between the oxidants oxygen, sulphate, and nitrate, and the reductants methane, sulphide and ammonium, matched very well in the chemocline during the stratified season. The profile of carbon isotopic composition of methane showed strong indications for methane oxidation at the chemocline (including the oxycline). Aerobic methane oxidizing bacteria were detected at the interface using fluorescence in situ hybridization. Sequencing the responsible organisms from DGGE bands revealed that aerobic methanotrophs type I closely related to Methylomonas were present. Sulphate consumption occurred at the sediment surface and, only towards the end of the stagnation period, matched with a zone of methane consumption. In any case, the flux of sulphate below the chemocline was not sufficient to oxidize all the methane and other oxidants like nitrate, iron or manganese are necessary for the observed methane oxidation. Although most of the methane was oxidized either aerobically or anaerobically, Lake Rotsee was still a source of methane to the atmosphere with emission rates between 0.2 mg CH4 m?2 day?1 in February and 7 mg CH4 m?2 day?1 in November.  相似文献   

2.
The biogeochemistry of methane in the sediments of Lake Caviahue was examined by geochemical analysis, microbial activity assays and isotopic analysis. The pH in the water column was 2.6 and increased up to a pH of 6 in the deeper sediment pore waters. The carbon isotope composition of CH4 was between − 65 and − 70‰ which is indicative for the biological origin of the methane. The enrichment factor ε increased from − 46‰ in the upper sediment column to more than − 80 in the deeper sediment section suggesting a transition from acetoclastic methanogenesis to CO2 reduction with depth. In the most acidic surface layer of the sediment (pH < 4) methanogenesis is inhibited as suggested by a linear CH4 concentration profile, activity assays and MPN analysis. The CH4 activity assays and the CH4 profile indicate that methanogenesis in the sediment of Lake Caviahue was active below 40 cm depth. At that depth the pH was above 4 and sulfate reduction was sulfate limited. Methane was diffusing with a flux of 0.9 mmol m− 2 d− 1 to the sediment surface where it was probably oxidized. Methanogenesis contributed little to the sediments carbon budget and had no significant impact on lake water quality. The high biomass content of the sediment, which was probably caused by the last eruption of Copahue Volcano, supported high rates of sulfate reduction which probably raised the pH and created favorable conditions for methanogens in deeper sediment layers.  相似文献   

3.
Kosolapov  D. B. 《Water Resources》2002,29(2):174-180
Concentrations of CH4 and the rates of processes of its transformation and oxidation are evaluated in the littoral zone of a large polimictic reservoir in the open-water period. The production of CH4 in bottom sediment was found to vary within 0.07 to 17.32 mmol/(m2 day) and attain its maximum in the late summer. The main factors to control the activity of methanogens were found to be the temperature and the availability of substrates (acetate and H2/CO2). The newly formed methane was oxidized in the top soil layer with a rate of 0.09–17.15 mmol/(m2 day). The rates of processes of biogenic production and consumption of CH4 in silts of screened coast were higher than those in sands of the open coastal zone. Methanotrophs were found to consume >87% of the methane produced. These bacteria accounted for 20 and 8% of the total oxygen consumption by bottom sediment in the screened and open littoral zones, respectively.  相似文献   

4.
This paper focuses on the chemical and isotopic features of dissolved gases (CH4 and CO2) from four meromictic lakes hosted in volcanic systems of Central–Southern Italy: Lake Albano (Alban Hills), Lake Averno (Phlegrean Fields), and Monticchio Grande and Piccolo lakes (Mt. Vulture). Deep waters in these lakes are characterized by the presence of a significant reservoir of extra-atmospheric dissolved gases mainly consisting of CH4 and CO2. The δ13C-CH4 and δD-CH4 values of dissolved gas samples from the maximum depths of the investigated lakes (from ?66.8 to ?55.6?‰ V-PDB and from ?279 to ?195?‰ V-SMOW, respectively) suggest that CH4 is mainly produced by microbial activity. The δ13C-CO2 values of Lake Grande, Lake Piccolo, and Lake Albano (ranging from ?5.8 to ?0.4?‰ V-PDB) indicate a significant CO2 contribution from sublacustrine vents originating from (1) mantle degassing and (2) thermometamorphic reactions involving limestone, i.e., the same CO2 source feeding the regional thermal and cold CO2-rich fluid emissions. In contrast, the relatively low δ13C-CO2 values (from ?13.4 to ?8.2?‰ V-PDB) of Lake Averno indicate a prevalent organic CO2. Chemical and isotopic compositions of dissolved CO2 and CH4 at different depths are mainly depending on (1) CO2 inputs from external sources (hydrothermal and/or anthropogenic); (2) CO2–CH4 isotopic exchange; and (3) methanogenic and methanotrophic activity. In the epilimnion, vertical water mixing, free oxygen availability, and photosynthesis cause the dramatic decrease of both CO2 and CH4 concentrations. In the hypolimnion, where the δ13C-CO2 values progressively increase with depth and the δ13C-CH4 values show an opposite trend, biogenic CO2 production from CH4 using different electron donor species, such as sulfate, tend to counteract the methanogenesis process whose efficiency achieves its climax at the water–bottom sediment interface. Theoretical values, calculated on the basis of δ13C-CO2 values, and measured δ13CTDIC values are not consistent, indicating that CO2 and the main carbon-bearing ion species (HCO3 ?) are not in isotopic equilibrium, likely due to the fast kinetics of biochemical processes involving both CO2 and CH4. This study demonstrates that the vertical patterns of the CO2/CH4 ratio and of δ13C-CO2 and δ13C-CH4 are to be regarded as promising tools to detect perturbations, related to different causes, such as changes in the CO2 input from sublacustrine springs, that may affect aerobic and anaerobic layers of meromictic volcanic lakes.  相似文献   

5.
The expanding use of horizontal drilling and hydraulic fracturing technology to produce oil and gas from tight rock formations has increased public concern about potential impacts on the environment, especially on shallow drinking water aquifers. In eastern Kentucky, horizontal drilling and hydraulic fracturing have been used to develop the Berea Sandstone and the Rogersville Shale. To assess baseline groundwater chemistry and evaluate methane detected in groundwater overlying the Berea and Rogersville plays, we sampled 51 water wells and analyzed the samples for concentrations of major cations and anions, metals, dissolved methane, and other light hydrocarbon gases. In addition, the stable carbon and hydrogen isotopic composition of methane (δ13C‐CH4 and δ2H‐CH4) was analyzed for samples with methane concentration exceeding 1 mg/L. Our study indicates that methane is a relatively common constituent in shallow groundwater in eastern Kentucky, where methane was detected in 78% of the sampled wells (40 of 51 wells) with 51% of wells (26 of 51 wells) exhibiting methane concentrations above 1 mg/L. The δ13C‐CH4 and δ2H‐CH4 ranged from ?84.0‰ to ?58.3‰ and from ?246.5‰ to ?146.0‰, respectively. Isotopic analysis indicated that dissolved methane was primarily microbial in origin formed through CO2 reduction pathway. Results from this study provide a first assessment of methane in the shallow aquifers in the Berea and Rogersville play areas and can be used as a reference to evaluate potential impacts of future horizontal drilling and hydraulic fracturing activities on groundwater quality in the region.  相似文献   

6.
Oxygen uptake rates by the sediment have been determined in a natural stratified sediment-water system from Lake Constance (Obersee, max. depth). After oxic preconditioning of the system the uptake rates ranged between 855 and 1,062 mg·m?2·d?1; after anoxic preconditioning of the system they ranged between 3,405 and 3,794 mg·m?2·d?1. These data, and the electron activity buffer capacity and oxygen consumption intensity as found in Lake Constance profundal water, show that the oxic-anoxic transition will happen here at the earliest after 142 days (about 4.5 months) of total oxygen isolation. Reoxygenation requires at least 3.7 times higher O2 input than supposed for a ‘normal’ winter circulation in Obersee.  相似文献   

7.
Four field campaigns are carried out to quantify the methane (CH4) oxidation rate in Xiangxi Bay (XXB) of the Three Gorges Reservoir (TGR), China. The water depth of the sampling site varied from 13 to 30 m resulting from the water level fluctuation of the TGR. The CH4 oxidation rates are measured in situ as the decline of dissolved CH4 concentration versus time in incubated, and those rates. The CH4 oxidation rates range from 1.18 × 10?3 to 3.69 × 10?3 µmol L?1 h?1, with higher values and stronger variation during summer. A static floating chamber method is used to measure CH4 emitted to the atmosphere resulting in an annual mean flux of 4.79 µmol m?2 h?1. The CH4 emission rate is significantly negatively correlated with the water level. The results show that a large fraction of CH4 is consumed in the water column with a range of 28.97–55.90 µmol m?2 h?1, accounting for ≈69–98% of the total CH4 input into the water column, and more than 90% is consumed outside the summer, when the water level is lowest. Water depth, which is dominated by water level of the TGR, is a potentially important driver for CH4 oxidation and atmospheric emission in the tributary bay.  相似文献   

8.
We investigated greenhouse gas emissions (CO2, CH4, and N2O) from reservoirs located across an altitude gradient in Switzerland. These are the first results of greenhouse gas emissions from reservoirs at high elevations in the Alps. Depth profiles were taken in 11 reservoirs located at different altitudes between the years 2003 and 2006. Diffusive trace gas emissions were calculated using surface gas concentrations, wind speeds and transfer velocities. Additionally, methane entering with the inflowing water and methane loss at the turbine was assessed for a subset of the reservoirs. All reservoirs were emitters of carbon dioxide and methane with an average of 970?±?340?mg?m?2?day?1 (results only from four lowland and one subalpine reservoir) and 0.20?±?0.15?mg?m?2?day?1, respectively. One reservoir (Lake Wohlen) emitted methane at a much higher rate (1.8?±?0.9?mg?m?2?day?1) than the other investigated reservoirs. There was no significant difference in methane emissions across the altitude gradient, but average dissolved methane concentrations decreased with increasing elevation. Only lowland reservoirs were sources for N2O (72?±?22???g?m?2?day?1), while the subalpine and alpine reservoirs were in equilibrium with atmospheric concentrations. These results indicate reservoirs from subalpine/alpine regions to be only minor contributors of greenhouse gases to the atmosphere compared to other reservoirs.  相似文献   

9.
Gaining streams can provide an integrated signal of relatively large groundwater capture areas. In contrast to the point‐specific nature of monitoring wells, gaining streams coalesce multiple flow paths. Impacts on groundwater quality from unconventional gas development may be evaluated at the watershed scale by the sampling of dissolved methane (CH4) along such streams. This paper describes a method for using stream CH4 concentrations, along with measurements of groundwater inflow and gas transfer velocity interpreted by 1‐D stream transport modeling, to determine groundwater methane fluxes. While dissolved ionic tracers remain in the stream for long distances, the persistence of methane is not well documented. To test this method and evaluate CH4 persistence in a stream, a combined bromide (Br) and CH4 tracer injection was conducted on Nine‐Mile Creek, a gaining stream in a gas development area in central Utah. A 35% gain in streamflow was determined from dilution of the Br tracer. The injected CH4 resulted in a fivefold increase in stream CH4 immediately below the injection site. CH4 and δ13CCH4 sampling showed it was not immediately lost to the atmosphere, but remained in the stream for more than 2000 m. A 1‐D stream transport model simulating the decline in CH4 yielded an apparent gas transfer velocity of 4.5 m/d, describing the rate of loss to the atmosphere (possibly including some microbial consumption). The transport model was then calibrated to background stream CH4 in Nine‐Mile Creek (prior to CH4 injection) in order to evaluate groundwater CH4 contributions. The total estimated CH4 load discharging to the stream along the study reach was 190 g/d, although using geochemical fingerprinting to determine its source was beyond the scope of the current study. This demonstrates the utility of stream‐gas sampling as a reconnaissance tool for evaluating both natural and anthropogenic CH4 leakage from gas reservoirs into groundwater and surface water.  相似文献   

10.
Increased ultraviolet-B radiation (UV-B) in aquatic ecosystems brought about by stratospheric ozone depletion may result in increased formation rates of photochemical reaction products in the surface waters of aquatic ecosystems. In this study, the potential impact of increases in lower wave-length radiation on the formation of hydrogen peroxide (H2O2) and singlet oxygen (1O2) was modelled for lakes over a range of dissolved organic carbon (DOC) concentrations. The impact of increased UV-B radiation on the production of carbon monoxide (CO) was also calculated for two humic stained systems. The relative increases of H2O2 and1O2 production were greater in the clear lakes (70% increase in photochemical reaction rates near the surface) than the coloured systems (25%). Production of CO in the study sites also increased under depleted ozone conditions implying increased DOC losses to the overlying atmosphere.  相似文献   

11.
In the process of methane oxidation by nitrite ion, the latter, when in high concentration, inhibits the oxidation process. The effect of inhibition is incorporated in the proposed model, describing the dynamics of anaerobic oxidation of methane and its heavy fractions δ13CH4 and δC2H1H3 by nitrite ion. Two substrates—methane and nitrite—are considered in a modified Monod function, describing the oxidation rate. The model is calibrated against experimental data given in [8]. The dynamic behavior of the system under a deficiency of methane or nitrite ion is described. The dynamics of δ13CH4 and δC2H1H3 are shown to be governed by the oxidation dynamics of total methane CH4. By contrast to the conventional opinion that Rayleigh equation corresponds to 1st-order kinetics in terms of substrate concentration, this study shows that Rayleigh equation can be derived from dynamic equations for methane with heavy isotopes (13C and 2H), whatever the kinetic type of total methane oxidation.  相似文献   

12.
  相似文献   

13.
Data of hydrological and hydrochemical observations conducted in August 2000 at Lake Seliger and its major tributaries are presented. The analyzed characteristics included: O2, H2S, CH4, microelements; mineral and organic compounds of P and N, ionic composition components (HCO3 –, Cl–, Na+, K+, dry residue, pH; color index, electrical conductivity. Bottom sediment samples were analyzed for microelement concentrations, CH4, oil hydrocarbons. The influence of the basin on the ecological state of the lake was assessed, and tendencies in the evolution of its ecosystem are analyzed. It is shown that the ecological conditions of the lake has not changed significantly since 1960–1991, however, nutrient concentrations in the lake water was found to increase.  相似文献   

14.
Discrimination of abiogenic and biogenic alkane gases   总被引：5，自引：0，他引：5  
We have combined the analytical data of the carbon isotope distribution pattern, R/Ra and CH4/3He values of abiogenic and biogenic (referring to the thermogenic and bacterial or microbial) alkane gases in China with those of alkane gases from USA, Russia, Germany, Australia and other countries. Four discrimination criteria are derived from this comparative study: 1) Carbon isotopic composition is generally greater than -30‰ for abiogenic methane and less than -30‰ for biogenic methane; 2) Abiogenic alkane gases have a carbon isotopic reversal trend (δ 13C1> δ 13C2> δ 13C3> δ 13C4) with δ 13C1>-30‰ in general; 3) Gases with R/Ra >0.5 and δ 13C11 δ 13C2>0 are of abiogenic origin; 4) Gases (meth- ane) with CH4/3He≤106 are of abiogenic origin, whereas gases with CH4/3He≥1011 are of biogenic origin.  相似文献   

15.
It have been measured the denitrification rates (DR) of sediment in Saginaw Bay, Lake Huron, by N2 production method. Triplicate samples of sediment core were collected at two GLERL long-term monitoring sites of the Bay in July and August of 1995. The DR are 48.81 -24.99 and 32.81-40.51 micromol N2 -2h-1 in the Inner and Outer regions of Saginaw Bay, respectively.The characters of DR in Saginaw Bay were studied also in this paper. The DR were influenced by the interactions between the Saginaw River as a main pollution source and the Lake Huron as a reservoir of high quality water. The impacts of zebra mussels (Dreissena Polymorpha) on denitrification in Saginaw Bay, Lake Huron, were discussed, Significant differences in NH4+ exchange fluxes were detected in the inner and outer bays. The molar ratios of N2:TIN were similar at both sampling sites. Measured DR were positively correlated to O2 consumption rates in the headspace. Additionally, a negative correlation between NH4+ and NO3- concentrations in the overlying water was found.  相似文献   

16.
肖启涛  胡正华  张弥  王伟  肖薇 《湖泊科学》2021,33(2):561-570
外源引水等水力调控措施常用于湖泊水环境综合整治中,作为人类施加到湖泊显著的外界活动,其对湖泊甲烷(CH4)扩散通量的影响鲜有报道.贡湖湾作为"引江济太"工程长江来水进入太湖的第一站,其CH4通量变化是对水力调控的最好响应.基于2011年11月至2013年8月逐月的野外观测表明,贡湖湾平均CH4扩散排放量为0.073 mmol/(m2·d),显著高于参考水域(湖心区) CH4排放量(均值:0.017 mmol/(m2·d)).贡湖湾不同站点间CH4通量也表现出显著差异,但湖心区域无此现象.贡湖湾和湖心2个区域的CH4扩散通量均有明显的时间变化,且与水温呈显著正相关.但因受到外源来水的影响,贡湖湾CH4通量时间变化的温度依赖性相对较低.总体上外源引水显著提高了湖体CH4排放量,考虑到湖泊CH4通量受内部因子和外部因子的综合协调影响,其潜在的控制机制还需要进一步探讨.  相似文献   

17.
Large lakes enclosures were used to examine the influence of nutrient (P, N) enrichment and planktivorous fish (1 + yellow perch) predation on hypolimnetic oxygen depletion. Results were compared to similar data for lakes with high (Lake St. George) and low (Haynes Lake) abundances of planktivorous fish. In both the unfertilized and fertilized enclosures, fish predation on large cladocerans increased the biomasses of pico- and nanoplankton (0.2–20 µm), phytoplankton (chlorophyll a) and total phosphorus (TP), reduced sedimentation, water clarity, and hypolimnetic oxygen concentrations (AHO). Fertilized enclosures without fish had highest TP and sedimentation rates, but the AHO were low. The high planktivore lake had higher pico- and nanoplankton, higher chlorophyll a, reduced water clarity, and lower AHO than the low planktivore lake. Areal hypolimnetic oxygen depletion (AHOD) rates were strongly related with Secchi depth and plankton size-distribution (r 2 = 0.77, and 0.79, respectively), but not as strongly with TP, chlorophyll a, and sedimentation rates (r 2 = 0.25, 0.53, and 0.02, respectively). Such observations are useful in forming a generalized hypothesis that lakes with low planktivory and high water clarity have lower oxygen depletion because 1) plankton that are settling are larger and spend less time in the hypolimnetic water column before reaching the sediment, and therefore undergo less decomposition, and 2) the euphotic depth extends into the hypolimnion and production of oxygen can take place.  相似文献   

18.
Enhanced reductive bioremediation (ERB) is effective for treating a broad range of groundwater contaminants, but does result in secondary water quality impacts (SWQIs). Monitoring data from 47 ERB projects were analyzed to gain a better understanding of the formation and extent of SWQIs. The database analysis revealed that SWQIs occur at virtually every site, including reduced levels of background aqueous electron acceptors (O2, NO3?, and SO42?), increases in dissolved‐phase metals (Fe and Mn), and the production of CH4. However, the SWQI “plume” that is produced is usually confined within the original contaminant plume. As a result, SWQIs from ERB are unlikely to adversely impact potable water supplies. SWQIs do attenuate with distance downgradient, with concentrations often returning to near background levels. The results of the database analysis were combined with previous research to develop a general conceptual model (CM) of SWQI production, mobilization, and attenuation. This CM can assist in identifying conditions where SWQIs may pose a concern. These can include sites with low iron/high sulfate (H2S mobilization), high groundwater velocity (SWQIs at distances far downgradient), and sites with low CH4 anaerobic oxidation rates (CH4 migration).  相似文献   

19.
Methane emissions from hydroelectric reservoirs can comprise a considerable portion of anthropogenic methane. However, lack of data on CH4 emissions in different geographical regions and high spatial‐temporal variability in the emission rates of reservoirs has led to uncertainties regarding regional emission estimates of CH4. In the subtropical plateau climate region, we used the Ertan hydroelectric reservoir as a study area. The CH4 flux at the air‐water interface was assessed by floating chambers and factors influencing emissions, including the distance from the dam, water depth, seasonal variation in wet and dry season, air‐water temperature gradient and wind speed, and was also studied through a year‐long systematic sampling and monitoring experiment. The results showed that the surface of the reservoir was a source of CH4 during the sampling period and the annual average CH4 flux was 2·80 ± 1·52 mg m?2 d?1. CH4 flux (and its variation) was higher in the shallow water areas than in the deep‐water areas. CH4 flux near the dam was significantly higher than that of other locations farther from the dam in the dry season. The seasonal variations of CH4 emission in wet and dry seasons were minor and significant diurnal variations were observed in wet and dry seasons. Exponential relationships between the CH4 flux and air‐water temperature gradient were found. Air‐water temperature gradient was an important factor influencing diurnal variations of CH4 flux in the Ertan hydroelectric reservoir. These results indicate that systematic sampling is needed to better estimate CH4 flux through coverage of the spatial variation of different water depths, measuring‐point distance from the dam, seasonal variation in wet and dry seasons and changes in climate factors (such as air‐water temperature gradient). Our results also provide a fundamental parameter for CH4 emission estimation of global reservoirs. Copyright © 2010 John Wiley & Sons, Ltd.  相似文献   

20.
城市景观湖泊对温室气体的收支发挥着重要作用。本文以南京市莫愁湖为研究对象,采用静态箱-温室气体分析仪法实时监测湖泊水-气界面CH4通量,分析湖泊主要温室气体CH4在日尺度和季节尺度上因冒泡和扩散排放方式不同对其通量的影响,探究影响湖泊CH4通量的因素。结果表明:(1)在日尺度上,四季24 h内CH4均呈排放状态,受白天冒泡影响,四季CH4总通量均存在白天高于夜间的日变化特征。(2)在季节尺度上,莫愁湖CH4排放通量呈现显著的时空异质性,受冒泡通量的影响夏季CH4通量明显高于春、秋、冬三季;B区的CH4总通量(6.04 nmol/(m2·s))显著高于A区(3.82 nmol/(m2·s)),水体的营养化程度和离岸距离是空间变化的主要影响因素。A、B两区CH4排放夏季以冒泡排放为主,春、秋、冬以扩散排放为主。(3)在日尺度上,CH4通量受气温、水温、辐射和风速等气象要素影响,与水质参数间的关系不显著;在季节尺度上,CH4通量与温度(气温、水温)、水体营养盐水平、叶绿素a浓度及富营养化程度的时间变化相一致,也随着水体透明度、pH和氧化还原电位的减小而呈增加的趋势。本研究为准确估算城市湖泊CH4排放量提供重要的数据基础。  相似文献   

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