River network travel time is correlated with dissolved organic matter composition in rivers of the contiguous United States

Most terrestrial allochthonous organic matter enters river networks through headwater streams during high flow events. In headwaters, allochthonous inputs are substantial and variable, but become less important in streams and rivers with larger watersheds. As allochthonous dissolved organic matter (DOM) moves downstream, the proportion of less aromatic organic matter with autochthonous characteristics increases. How environmental factors converge to control this transformation of DOM at a continental scale is less certain. We hypothesized that the amount of time water has spent travelling through surface waters of inland systems (streams, rivers, lakes, and reservoirs) is correlated to DOM composition. To test this hypothesis, we used established river network scaling relationships to predict relative river network flow-weighted travel time (FWTT) of water for 60 stream and river sites across the contiguous United States (3090 discrete samples over 10 water years). We estimated lentic contribution to travel times with upstream in-network lake and reservoir volume. DOM composition was quantified using ultraviolet and visible absorption and fluorescence spectroscopy. A combination of FWTT and lake and reservoir volume was the best overall predictor of DOM composition among models that also incorporated discharge, specific discharge, watershed area, and upstream channel length. DOM spectral slope ratio (R² = 0.77) and Freshness Index (R² = 0.78) increased and specific ultraviolet absorbance at 254 nm (R² = 0.68) and Humification Index (R² = 0.44) decreased across sites as a function of FWTT and upstream lake volume. This indicates autochthonous-like DOM becomes continually more dominant in waters with greater FWTT. We assert that river FWTT can be used as a metric of the continuum of DOM composition from headwaters to rivers. The nature of the changes to DOM composition detected suggest this continuum is driven by a combination of photo-oxidation, biological processes, hydrologically varying terrestrial subsidies, and aged groundwater inputs.     

Characteristics and role of groundwater dissolved organic matter on arsenic mobilization and poisoning in Bangladesh

The fluorescence and molecular weight characteristics of dissolved organic matter (DOM) in groundwater of Bangladesh were investigated to evaluate its multiple roles on arsenic (As) mobilization and poisoning. Fluorescence properties of DOM were measured in groundwater samples collected from two As contaminated areas of Bangladesh (Faridpur at the Ganges floodplain and Sonargaon at the Meghna floodplain) from different locations and depths. The three dimensional excitation–emission matrix (3DEEM) fluorescence spectra of groundwater samples showed two characteristic peaks around Ex/Em = 335–365 nm/435–480 nm for fulvic-like peaks and peak at around Ex/Em = 275–290 nm/310–335 nm for the protein-like materials. The similarity of fluorescence spectra of groundwater and surface water of both the study areas with high intensity of fluorescence and its strong correlation with DOC reflect the in situ generation of fluorescent DOM from sedimentary organic matter (SOM) and recent recharge of terrestrial labile organic carbon into shallow aquifer. High performance size-exclusion chromatography (HPSEC) analysis of DOM shows positive correlations between fluorescence intensities (FI) of small molecular fractions (0.65 kDa) and As concentrations, with the signatures of protein-like peaks of DOM in groundwater. This result provides new evidence that small molecular weight fraction of DOM in groundwater of Bangladesh can play an important role on As mobilization and toxicity. In addition, high concentration of fluorescence materials in DOM of As contaminated groundwater of Bangladesh may pose a threat to public health.     

草源型可溶性有机物降解过程中活性氧物种产生过程

活性氧物种(ROS)参与天然水体系统中的光化学反应、氧化还原反应,是影响水体中有机污染物的迁移、转化、环境归宿及生态效应的重要因素.然而目前对草源型可溶性有机物(DOM)分解过程中ROS的产生过程并不清楚.本文通过室内模拟实验首先构建了室内测定3种ROS(~3CDOM~*、~1O_2、·OH)的方法,进而分析草源植物——苔草(Carex tristachya)残体浸出液中DOM光降解过程中ROS的产生过程.结果表明:ROS累积含量的产生随着DOM的降解逐渐升高在3种自由基含量中,~3CDOM*的产生含量最多,·OH产生含量低于另外2种ROS两个数量级.CDOM含量与~3CDOM~*、~1O2、·OH浓度呈现正相关关系,尤其与~3CDOM~*和~1O_2浓度的显著性水平最高,·OH次之.ROS浓度与水质指标呈现出不同的线性相关关系,与硝态氮浓度呈负相关关系,而与亚硝态氮浓度呈现正相关关系,并且亚硝态氮对ROS浓度影响效果极显著.同时类蛋白荧光峰值强度的衰减与ROS累积含量呈现极显著负相关关系,脱明在DOM的光降解过程中蛋白质小分子的降解是产生ROS很重要的一个部分.综上通过对草源型DOM光降解过程中ROS产生过程的研究,增加了对湖泊生态系统中水生植物产生ROS的过程、迁移、转化、归宿及其作用机制的认识.     

青海湖泉湾镭同位素的空间分布与沿岸地下水排放评价

青海湖是青藏高原的重要组成部分,它是维系青藏高原东北部生态安全的重要水体.其沿岸地下水的排放直接影响了青海湖的水文生物地球化学过程,然而对该问题的研究仍然不充分.本研究于2014年对青海湖泉湾湖水、河水和地下水进行223Ra和224Ra活度的测定分析,并对泉湾湖水水平向和垂直向的Ra活度分布进行深入分析,最后估算并探讨了泉湾水体的停留时间和布哈河口沿岸地下水的排放通量.表层湖水、河水、地下水不同端元的水体223Ra和224Ra活度值分别为0.441和0.026 dpm/100 L、0.22和0.016 dpm/100 L以及0.061和1.30 dpm/100 L,最高值为地下水,其次湖水,河水最小;总体上泉湾湖水223Ra和224Ra活度随离岸距离增加分别由0.047到0.011 dpm/100 L和1.4到0.2 dpm/100 L的减小,垂向上Ra活度呈楔形分布,Ra活度在不同方向上的非保守性分布主要受到悬浮颗粒物解析的影响;通过水体滞留时间模型计算获得青海湖泉湾水体的平均停留时间为1.8天,进一步分析泉湾水体Ra的源汇项,应用镭同位素质量平衡模型获得泉湾布哈河口沿岸地下水排放通量为0.054～0.109 m3/(m2·d).     

Preconditioning of an underflow during ice-breakup in a subarctic lake

The fate of inflows into lakes has been extensively studied during summer stratification but has seen relatively little focus during the weak winter stratification, with or without ice-cover. Field observations are presented of groundwater inflow into a shallow bay of a subarctic lake. Atmospheric forcing of the bay during the study period was extremely variable and coincided with spring ice-cover break-up. Two dominant wind regimes were identified; (1) weak wind-forcing (wind speed <5 m s⁻¹ or land-fast ice-cover), and (2) strong wind-forcing (wind speed >5 m s⁻¹ and open water). At a relatively constant temperature of ~3.3°C, the groundwater inflow was closer to the temperature of maximum density than the water in the main body of the lake, which during the observed winter stratification is ~1.2°C. During weak wind-forcing, the stratification within Silfra Bay approximated two-layers as this denser groundwater formed a negatively buoyant underflow. A calculated underflow entrainment rate of 2.8 × 10⁻³ agrees well with other underflow studies. During strong wind-forcing, the water column out to the mouth of the bay became weakly stratified as the underflow was entrained vertically by wind-stirring. Observed periods of mixing can be predicted to occur when turbulent kinetic energy (TKE) production by wind stirring integrated over the underflow hydraulic residence time in the bay exceeds the potential energy associated with the stratification. A decrease of ice cover, as observed in the studied subarctic lake over the last decade, will result in the underflow being more frequently exposed to the strong wind-forcing regime during winter, thereby altering the winter distribution of groundwater inflow within the lake.     

Variation in the photochemical lability of dissolved organic matter in a large boreal watershed

Boreal watersheds contain a vast quantity of terrestrially derived dissolved organic matter (DOM) originating from wetland and forest soils, yet variation in the potential for photochemical transformation of boreal aquatic DOM sources remains poorly understood. Laboratory solar radiation exposure experiments were conducted on DOM samples collected in three seasons, across nine sites, representing contrasting catchment composition and watershed position to assess variation in the photochemical lability of boreal DOM source and stable carbon isotopic signature (δ¹³C) of photomineralized DOM. Dissolved organic carbon (DOC) loss rates during laboratory exposure were lowest in summer, suggesting that DOM may have been more photo-degraded during summer. DOM from upstream portions of forested stream sites and wetland-influenced sites was more photolabile relative to downstream portions and the river DOM, suggesting potential losses in photolabile DOM downstream and in the lower reaches of the watershed. Increased a₂₅₄:a₃₅₀ and spectral slope following sample exposure suggest photoproduction of low molecular weight (LMW) CDOM and/or a higher photoreactivity of high molecular weight versus LMW compounds. Photomineralization of nitrogen was regulated by organic nitrogen concentration and resulted in NH₄ ⁺-photoproduction rates between 0.01 and 0.3?μM N?h^?1 and ecologically significant increases in NH₄ ⁺ for these waters. The δ¹³C of the photomineralized DOM was positively correlated to initial DOC concentration and generally lower when initial DOC concentrations were lower, suggesting variation in photomineralized DOM δ¹³C may be a result of kinetic isotope fractionation. Results from this study demonstrate significant variation in the photochemical lability of boreal watershed sources of DOM. Such variation suggests landscape and environmental change has the potential to alter the biogeochemical role photochemical transformations play in downstream portions of boreal watersheds.     

基于氡同位素的平原湖荡枯水期湖水地下水补排通量

水是人类生存之源,而湖荡被称为地球之“肾”,是河湖水系连接的关键缓冲节点,与人类生存和发展息息相关。长三角平原水系众多,河流纵横,天然湖泊与人工沟渠遍布,平原湖荡湖水与周边地下水的水力联系较为频繁,而地下水对湖泊水均衡贡献尚不明确,对平原湖荡地下水赋存和运移规律的认识不足。本研究以苏州吴江区元荡湖为研究对象,选取氡同位素作为湖水和地下水水力交换过程的示踪剂,建立氡箱模型,揭示元荡湖不同区段与地下水的水力联系过程和补给关系,并通过水位动态验证分析湖水—地下水交互关系。枯水期元荡湖水位和氡浓度空间分布特征指示研究区内地下水向湖水排泄,其中以湖泊西侧较为明显,地下水入流补给的氡为7.137×10⁶ Bq/d,输入量源项占比为90%,地下水流入量为4540.801 m³/d,地下水每日流入量对元荡湖水量的贡献率为2.551%。参数敏感性分析结果表明,风速与地下水²²²Rn活度为特别敏感参数,取值差异较大时会导致计算误差急剧增大,改善测点布置和提高模型参数精度能有效提高模型计算结果的准确性和可靠程度。借助氡同位素示踪方法,建立湖泊...     

A stable isotope study of the Garda lake, northern Italy: Its hydrological balance

Discontinuous measurements of the isotopic composition of surface water samples of the Garda lake carried out between 1998 and 2006 showed almost constant δ¹⁸O, δD and d-excess values through time. During 2006 and 2007 monthly vertical profiles of water samples were collected in the northernmost section of the lake, not far from the main inflow (Sarca river) to check whether there was any detectable influence from this inflowing river and whether there was a vertical isotopic stratification of the lake water. The isotopic measurement of water samples from the vertical profiles yielded isotopic values which were almost equal to those obtained from surface waters showing no detectable effect of the inflowing river water and no isotopic vertical stratification. The attempt to evaluate the evaporation rate of lake water by means of current models was totally unsuccessful. Despite the marked summer warming of the surface layer no isotopic fractionation related to evaporation processes could be detected. This anomalous behaviour may be related to the large amount of spring and summer precipitation characteristic of this area. The water balance of the lake calculated according to the amount of the inflowing water (Sarca river water plus rain water on the lake plus 20% of the precipitations on the whole catchment basin) and to the amount of outflowing water (Mincio river) showed a large imbalance, the river outflow alone resulting on average, during the last decade, at least double the inflow. To explain this imbalance of the lake, a large recharge by concealed groundwater is suggested: its isotopic composition should be quite close to the mean isotopic composition of precipitations over that area. This would be in agreement with the almost constant isotopic composition of both surface and deep waters and with the lack of vertical isotopic stratification. A few measurements of the tritium concentration carried out on lake water show values that are considerably higher than modern tritium values either in precipitation or in the Sarca river water: these results are in good agreement with the hypothesis of a recharge of the lake by deep aquifers.     

柴达木盆地尕斯库勒盐湖地表水-地下水的转化与铀的补给通量

流域范围内地表水和地下水转化对盐湖成盐元素的运移和富集具有十分重要的意义.本文通过尕斯库勒盐湖盆地内流域水体的水化学和B同位素特征识别了地表水和地下水之间的定量转化关系,在此基础上估算了流域中铀的补给通量.结果表明,流域水体中离子的分异除了蒸发浓缩作用之外,还受重力分异及掺杂作用的影响;上游库拉木勒克萨伊河和阿特阿特坎河水体在出山口附近转入地下并在中游补给地表水和地下水,其补给率分别占48.8%和51.2%,年均补给量分别为1.08×108和1.13×108m3/a;在中游至尾闾盐湖段,阿拉尔河和侧向补给对盐湖卤水的补给率占55.2%,深部水体的补给占44.8%;至少从5.7 ka以来,上游水体对盐湖卤水中铀的补给通量为4.11×103t,在湖积平原黏土沉积带以及祁漫塔格山前局部还原带可能具有较大规模的铀矿.研究结果有助于建立盐湖盆地水循环模式、揭示卤水资源形成机制;同时为尕斯库勒盐湖盆地水资源的高效利用和寻找铀矿提供理论依据和技术支持.     

Determination of groundwater discharge rates and water residence time of groundwater‐fed lakes by stable isotopes of water (18O, 2H) and radon (222Rn) mass balances

Lacustrine groundwater discharge (LGD) and the related water residence time are crucial parameters for quantifying lake matter budgets and assessing its vulnerability to contaminant input. Our approach utilizes the stable isotopes of water (δ¹⁸O, δ²H) and the radioisotope radon (²²²Rn) for determining long‐term average and short‐term snapshots in LGD. We conducted isotope balances for the 0.5‐km² Lake Ammelshainer See (Germany) based on measurements of lake isotope inventories and groundwater composition accompanied by good quality and comprehensive long‐term meteorological and isotopic data (precipitation) from nearby monitoring stations. The results from the steady‐state annual isotope balances that rely on only two sampling campaigns are consistent for both δ¹⁸O and δ²H and suggested an overall long‐term average LGD rate that was used to infer the water residence time of the lake. These findings were supported by the good agreement of the simulated LGD‐driven annual cycles of δ¹⁸O and δ²H lake inventories with the observed lake isotope inventories. However, radon mass balances revealed lower values that might be the result of seasonal LGD variability. For obtaining further insights into possible seasonal variability of groundwater–lake interaction, stable water isotope and radon mass balances could be conducted more frequently (e.g., monthly) in order to use the derived groundwater discharge rates as input for time‐variant isotope balances.     

Gravitational effect of water circulation in the northwest Yunnan

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