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.     

Nitrogen retention in a floodplain backwater of the upper Mississippi River (USA)

Backwaters connected to large rivers retain nitrate and may play an important role in reducing downstream loading to coastal marine environments. A summer nitrogen (N) inflow-outflow budget was examined for a flow-regulated backwater of the upper Mississippi River in conjunction with laboratory estimates of sediment ammonium and nitrate fluxes, organic N mineralization, nitrification, and denitrification to provide further insight into N retention processes. External N loading was overwhelmingly dominated by nitrate and 54% of the input was retained (137 mg m⁻² day⁻¹). Ammonium and dissolved organic N were exported from the backwater (14 and 9 mg m⁻² day⁻¹, respectively). Nitrate influx to sediment increased as a function of increasing initial nitrate concentration in the overlying water. Rates were greater under anoxic versus oxic conditions. Ammonium effluxes from sediment were 26.7 and 50.6 mg m⁻² day⁻¹ under oxic and anoxic conditions, respectively. Since anoxia inhibited nitrification, the difference between ammonium anoxic–oxic fluxes approximated a nitrification rate of 29.1 mg m⁻² day⁻¹. Organic N mineralization was 64 mg m⁻² day⁻¹. Denitrification, estimated from regression relationships between oxic nitrate influx versus initial nitrate concentration and a summer lakewide mean nitrate concentration of 1.27 mg l⁻¹, was 94 mg m⁻² day⁻¹. Denitrification was equivalent to only 57% of the retained nitrate, suggesting that another portion was assimilated by biota. The high sediment organic N mineralization and ammonium efflux rate coupled with the occurrence of ammonium export from the system suggested a possible link between biotic assimilation of nitrate, mineralization, and export.     

An isotopic model for the origin of autochthonous organic matter contained in the bottom sediments of a reservoir

Geochemical analysis of surface sediment samples collected in 2005 and 2006 was used to evaluate the potential sources of the organic matter present in sediments of southeast Poland's Solina Reservoir.Statistical analysis of sediment variables(carbon to nitrogen ratio, and the carbon 13 and nitrogen 15 isotope ratios) determined for the organic fraction indicated significant spatial variability with respect to sources of organic matter. A binary mixing model was developed from literature sources to predict the relative contributions of allochthonous and autochthonous production to sediment organic matter.Autochthonous production was shown to account for 60-75% of bulk sedimentation in the lacustrine parts of the reservoir, near the dam. In contrast, autochthonous production accounted for only 25% of sedimentation in the riverine zone receiving stream inputs. Statistical analysis identified the δ~(15)N of organic matter as the best predictor of the source of organic matter. Multiple regression analysis indicated that two water-quality variables(nitrate and dissolved silica) were significantly related to the δ~(15)N signature of organic matter. This led to a conclusion that limnetic nitrate and dissolved silica concentrations were regulating organic matter production in the Solina Reservoir.     

基于植物昼夜释氧变化规律的复合垂直流人工湿地氮形态

为了研究植物根系释氧规律对人工湿地中硝化与反硝化作用的影响,采用传统连续运行方式及根据释氧规律调节的新型运行方式(白天连续进水、夜间停水),在复合垂直流人工湿地小试系统中进行实验,采用代表性的挺水植物香蒲作为湿地植物,水力负荷为0.71 m3/(m2.d).结果表明:系统内白天以好氧的硝化作用为主,夜间以厌氧、缺氧的反硝化作用为主,且在新型运行方式下,系统内白天亚硝酸盐氮累积量为传统运行方式的5倍,硝酸盐氮累积量为其2倍,夜间亚硝酸盐氮和硝酸盐氮减少量又分别比传统运行方式高64%和26%.这说明在新型运行方式下,人工湿地脱氮效果优于传统运行方式.     

Nitrogen isotopic geochemical characteristics of crude oils in several basins of China

Nitrogen occupies a high content in crust and in atmospheric circle. It is one of the main elements in organism and an important element in sedimentary circle. Although nitrogen is little in crude oil, to a cer-tain degree, it influences the physical and chemical properties of oil, such as viscosity and density[1]. In reservoir the nitrogen-bearing compounds can form ion bonds or hydrogen bonds with substances on rock and form van der Vaals’ force among moleculae so they affect and alter the …     

Nutrient flux, uptake, and transformation in a spring-fed stream in the Missouri Ozarks, USA

We examined nutrient flux, uptake, and transformation along a spring-fed stream in the Ozark region of Missouri, USA, over the year 2006. Water in Mill Creek originates from several springs, with a single spring contributing over 90% of the stream discharge during much of the year of study. Soluble reactive phosphate concentrations were usually low (<10 μg L⁻¹) along Mill Creek, but peaked during high discharge. Concentrations of dissolved inorganic nitrogen (DIN) were relatively high in the spring water, mainly as nitrate, but usually declined across a small pond and the 10-km length of Mill Creek. During low flows in summer and early autumn, the stream removed over 300 μg L⁻¹ of DIN over its 10-km length, or about 80% of the initial amount. DIN retention along the stream, as a percentage of the DIN upstream, was related mainly to discharge, with higher flows having much higher DIN concentrations. The net uptake rate of DIN uptake was 0.91 μg m⁻² s⁻¹ in the stream during summer baseflow. The uptake rate declined downstream for different reaches and was closely related to DIN concentration. In experimental channels, uptake by epilithic algae was one significant sink for nitrate-N in Mill Creek. In 2006, inorganic nutrient export during a single day after a spring storm was similar to export during 40–100 days of low flow conditions in summer and early autumn. Our results suggest that significant nutrient retention can occur during baseflow periods via biological uptake, whereas substantial export occurs during high flow conditions.     

Contributions of phytoplankton and nitrifying bacteria to ammonium and nitrite dynamics in coastal waters

Ammonium and nitrite dynamics in coastal waters off Washington were examined using stable nitrogen isotope methods. Assimilation rates of ammonium into particulate nitrogen exhibited maxima (up to 500 nmol l⁻¹d⁻¹ at shallow depths and were negligible below the photic zone. Rates of ammonium oxidation by nitrifying bacteria showed surface minima and increased with depth (up to 35 nmol l⁻¹ d⁻¹). Both processes showed evidence of control by light intensity: light stimulated assimilation and inhibited oxidation. Ammonium turnover was dominated by phytoplankton assimilation at shallow depths and at inshore stations, while the relative contribution of bacterial oxidation of ammonium to turnover increased with increasing depth and increasing distance from shore. Nitrite turnover due to ammonium oxidation approached 60% per day in the primary nitrite maximum at the outer stations.     

Continuing inflation at Three Sisters volcanic center,central Oregon Cascade Range,USA, from GPS,leveling, and InSAR observations

Uplift of a broad area centered ~6 km west of the summit of South Sister volcano started in September 1997 (onset estimated from model discussed in this paper) and was continuing when surveyed in August 2006. Surface displacements were measured whenever possible since August 1992 with satellite radar interferometry (InSAR), annually since August 2001 with GPS and leveling surveys, and with continuous GPS since May 2001. The average maximum displacement rate from InSAR decreased from 3–5 cm/yr during 1998–2001 to ~1.4 cm/yr during 2004–2006. The other datasets show a similar pattern, i.e., surface uplift and extension rates decreased over time but deformation continued through August 2006. Our best-fit model to the deformation data is a vertical, prolate, spheroidal point-pressure source located 4.9–5.4 km below the surface. The source inflation rate decreased exponentially during 2001–2006 with a 1/e decay time of 5.3 ± 1.1 years. The net increase in source volume from September 1997 to August 2006 was 36.5–41.9 x 10⁶ m³. A swarm of ~300 small (M _max = 1.9) earthquakes occurred beneath the deforming area in March 2004; no other unusual seismicity has been noted. Similar deformation episodes in the past probably would have gone unnoticed if, as we suspect, most are small intrusions that do not culminate in eruptions.     

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.     

亚热带地区典型水库流域氮、磷湿沉降及入湖贡献率估算

为了探究汤浦水库流域氮、磷湿沉降对水库水体营养的贡献率,本研究对2014 2015年的汤浦水库流域4个采样点的雨水及3条溪流进行样品收集,测定其中磷和不同形态氮的质量浓度,分析汤浦水库流域大气湿沉降中氮、磷营养盐的分布特征,并估算氮、磷营养盐湿沉降对汤浦水库入库负荷的贡献率.结果表明:湿沉降中总氮(TN)平均浓度为1.02±0.58 mg/L,氨氮、硝态氮和有机氮浓度占TN浓度的比例分别为60.65%、34.07%和5.28%;总磷(TP)平均浓度为0.033±0.028 mg/L.4个采样点湿沉降中氮、磷浓度均表现为冬春季(少雨季)高、夏秋季(多雨季)低.空间上,王化点位的各形态氮和总磷浓度显著高于其他3个采样点.TN和TP年均湿沉降通量约为18.15和0.62 kg/(hm~2·a),年均沉降总量为834.94和28.39 t;库区TN和TP水面湿沉降量为24.14和0.82 t,直接贡献率占河流输入的1.77%和3.07%.湿沉降来源的氮、磷营养盐随河流输入的间接贡献率为8.3%和4.6%.综上所述,氮、磷湿沉降是水库外源营养的重要输入部分,深入掌握其时空分布特征及入库贡献率是进一步加强流域管理和减轻水库外源营养输入的重要前提.     

Degradation Pathway of the Photochemical Oxidation of Ethylenediaminetetraacetate (EDTA) in the UV/H2O2-process

The degradation pathway for the oxidation of EDTA in the UV/H₂O₂-process was investigated. In absence of iron ions, the mineralization of EDTA is dominated by the reaction of the HO-radicals generated by the photolysis of H₂O₂. The organic degradation products iminodiacetate (IMDA), glycinate, oxamate, glyoxylate, oxalate and formate, and the inorganic degradation products carbon dioxide, ammonia, nitrate, nitrite, and cyanate were found. In the presence of iron ions, photolytic decarboxylation processes inside the complex get an important role during degradation, and the organic degradation products ethylenediaminetriacetate (ED3A), ethylenediaminediacetate (EDDA), ethylenediaminemonoacetate (EDMA) were also found. By combining product studies with balances of carbon and nitrogen, the degradation pathway in the UV/H₂O₂-process could be elucidated. The degradation of EDTA was fast (k_deg = 0.012 s^–1), and no toxic degradation products were identified. Therefore, the process is well suited for the elimination of EDTA in water treatment.     

Compositions and constituents of freshwater dissolved organic matter isolated by reverse osmosis

Dissolved organic matter (DOM) from riverine and lacustrine water was isolated using a reverse osmosis (RO) system. Solid-state ¹³C nuclear magnetic resonance (¹³C NMR) was used to quantitatively evaluate the compositions and constituents of DOM, which are compared with previous investigations on marine DOM. Results indicated that concentration factor (CF) was a key metric controlling yield and sorption of DOM on the RO system. The sorption was likely non-selective, based on the ¹³C NMR and δ¹³C analyses. Carbohydrates and lipids accounted for 25.0–41.5% and 30.2–46.3% of the identifiable DOM, followed by proteins (18.2–19.8%) and lignin (7.17–12.8%). The freshwater DOM contained much higher alkyl and aromatic C but lower alkoxyl and carboxyl C than marine DOM. The structural difference was not completely accounted for by using structure of high molecular weight (HMW) DOM, suggesting a size change involved in transformations of DOM during the transport from rivers to oceans.