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1.
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.  相似文献   

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Absorbance at 360 nm was measured on 44 filtered streamwater samples of different dissolved organic matter (DOM) contents. A regression equation of DOM on absorbance predicted DOM with a standard error of estimate of 1.26 mgl?1, Use of a published equation relating dissolved organic carbon (DOC) to absorbance gave DOC values for the samples which were consistent with measured DOM. The method offers considerable potential for rapid quantification of dissolved organic matter concentrations in streamwater.  相似文献   

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The input and fate of dissolved organic matter (DOM) can have important consequences for coastal zone productivity in large lakes and oceans. Chromophoric DOM (CDOM) is often delivered to coastal zones from rivers and streams and affects light penetration in a water column. CDOM can protect biota from damaging ultraviolet (UV) light by acting as sunscreen, resulting in increased ecosystem productivity. Alternatively, CDOM can decrease ecosystem productivity by absorbing light needed for photosynthesis and forming photoreaction products that are harmful to coastal zone biota. Increased urbanization of watersheds and seasonal differences in weather patterns change the delivery pathways, reactivity, input, and energy flow of DOM (and its CDOM component) into aquatic systems. This study investigated the effects of watershed and season on the concentrations and potential photodegradation of stream-derived DOM in Lake Superior tributaries, chosen to be geographically and geologically similar but differing in land use. Organic carbon analysis, UV–Visible spectrophotometry, and terrestrial (land use) analysis were used to investigate differences among samples and sample treatments. The major differences in DOM concentration and photochemical response appeared seasonal rather than site specific, with snow-melt samples showing stronger and more consistent changes in UV–Visible parameters while base-flow samples showed stronger and more consistent losses in DOC.  相似文献   

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Two water samples from the Great Dismal Swamp National Wildlife Refuge with high dissolved organic matter (DOM) concentrations (51 and 121 mg C L?1) were subjected to ultraviolet (UV) light for up to 110 days. During the course of the irradiations, 74–88 % of the original dissolved organic carbon was lost along with 95–99 % of the absorption at 300 nm. Based on changes observed during light exposure, three pools of DOM were identified: photo-labile, photo-refractory, and photo-produced compounds. Solid-state 13C nuclear magnetic resonance (NMR) spectroscopy and Fourier transform infrared (FTIR) spectroscopy were used to determine structural moieties characteristic to each of these pools. These analyses showed aromatic carbons were preferentially removed while carbohydrate-like and amide/peptide-like carbons were preserved during UV exposure. An increase in carbon normalized 13C NMR signal in the 0–50 ppm region suggests that alkyl moieties were produced, while FTIR signal at 1,745 cm?1 and two-dimensional 1H–13C NMR results confirmed the photochemical production of acetate. Several properties typically used to trace terrigenous DOM in ocean margin and marine environments were significantly altered. Optical properties, including absorption spectral slopes and fluorescence indices, as well as carbon-normalized lignin yields shifted from terrestrial values towards those more typical of coastal or open ocean samples. The loss of terrestrial signatures during irradiation highlights the difficulty faced when quantifying the contribution of terrigenous DOM to aquatic carbon pools.  相似文献   

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Exploring the chemical characterization of dissolved organic matter (DOM) is important for understanding the fate of laterally transported organic matter in watersheds. We hypothesized that differences in water-extractable organic matter (WEOM) in soils of varying land uses and rainfall events may significantly affect the quality and the quantity of stream DOM. To test our hypotheses, characteristics of rainfall-runoff DOM and WEOM of source materials (topsoil from different land uses and gullies, as well as typical vegetation) were investigated at two adjacent catchments in the Loess Plateau of China, using ultraviolet–visible absorbance and excitation emission matrix fluorescence with parallel factor analysis (PARAFAC). Results indicated that land-use types may significantly affect the chemical composition of soil WEOM, including its aromaticity, molecular weight, and degree of humification. The PARAFAC analysis demonstrated that the soils and stream water were dominated by terrestrial/allochthonous humic-like substances and microbial transformable humic-like fluorophores. Shifts in the fluorescence properties of stream DOM suggested a pronounced change in the relative proportion of allochthonous versus autochthonous material under different rainfall patterns and land uses. For example, high proportions of forestland could provide more allochthonous DOM input. This study highlights the relevance of soils and hydrological dynamics on the composition and fluxes of DOM issuing from watersheds. The composition of DOM in soils was influenced by land-use type. Precipitation patterns influenced the proportion of terrestrial versus microbial origins of DOM in surface runoff. Contributions of allochthonous, terrestrially derived DOM inputs were highest from forested landscapes.  相似文献   

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Continuous monitoring of dissolved organic matter (DOM) character and concentration at hourly resolution is rare, despite the importance of analysing organic matter variability at high‐temporal resolution to evaluate river carbon budgeting, river water health by detecting episodic pollution and to determine short‐term variations in chemical and ecological function. The authors report a 2‐week experiment performed on DOM sampled from Bournbrook, Birmingham, UK, an urban river for which spectrophotometric (fluorescence, absorbance), physiochemical (dissolved organic carbon [DOC], electrical conductivity, pH) and isotopic (D/H) parameters have been measured at hourly frequency. Our results show that the river had sub‐daily variations in both organic matter concentration and characteristics. In particular, after relatively high‐magnitude precipitation events, organic carbon concentration increased, with an associated increase in intensity of both humic‐like and tryptophan‐like fluorescence. D/H isotopic ratio demonstrates different hydrological responses to different rainfall events, and organic matter character reflects this difference. Events with precipitation < 2 mm typically yielded isotopically heavy water with relatively hydrophilic DOM and relatively low specific absorbance. Events with precipitation > 2 mm had isotopically lighter water with higher specific absorbance and a decrease in the proportion of microbially derived to humic‐like fluorescence. In our heavily urbanized catchment, we interpret these signals as one where riverine DOM is dominated by storm sewer‐derived ‘old’ organic matter at low‐rainfall amounts and a mixed signal at high‐precipitation amounts where ‘event’ surface runoff‐derived organic matter dominate during storm sewer and combined sewer overflow routed DOM. Copyright © 2009 John Wiley & Sons, Ltd.  相似文献   

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The spatial and diurnal tidal variability of dissolved organic carbon (DOC) concentrations and the composition of dissolved organic matter (DOM), as evaluated by high-temperature catalytic oxidation and excitation–emission matrix combined with parallel factor analysis (EEM–PARAFAC), respectively, were determined in Liverpool Bay. EEM–PARAFAC modeling resulted in six fluorescent components characterized as terrestrial humic-like (two), microbial humic-like (two), and protein-like (two). The spatial distributions of DOC and the four humic-like components were negatively correlated with salinity in the high-salinity waters observed in this study (30.41–33.75), suggesting that terrestrial DOM was conservatively distributed. The spatial patterns of protein-like components were largely different from those of DOC, humic-like components, and chlorophyll a, suggesting that these distributions were the combined result of production and degradation in the bay in addition to river inputs. These findings suggest that the DOM dynamics in Liverpool Bay are strongly controlled by river-dominated allochthonous DOM inputs with some less significant contributions of autochthonous DOM within the bay. In addition, the temporal variations of DOM associated with the diurnal tidal cycles were determined at one inshore (31.34–32.24 salinity) and one offshore (33.64–33.75 salinity) station in the bay. Negative linear relationships between salinity and DOM characteristics, i.e., DOC, humic-like, and protein-like components, were observed at the inshore station. In contrast, no relationship was observed at the offshore station, suggesting that the export of DOM through rivers and possibly tidal flats have a noticeable influence on DOM concentration and composition up to a relatively elevated salinity of around 33 in Liverpool Bay.  相似文献   

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This study aimed to evaluate the importance of physical, chemical and biological factors (e.g., chlorophyll-a, and carbon) in the regulation of the summer epilimnion thickness (Zmix) of the tropical lakes focusing on trends of the current environmental variability. We sampled a set of tropical lakes from the middle Rio Doce lacustrine system (Minas Gerais, Brazil) for two consecutive summers. Besides Zmix, we analyzed the visible light attenuation (KdPAR), dissolved organic carbon (DOC), chlorophyll-a (Chl-a), total suspended solids (TSS), and fetch. We also analyze the quality of the dissolved organic matter (DOM) through colored dissolved organic matter (CDOM), spectral slope (S), DOC-specific absorbance (SUVA) and the ratio between the absorbance at 250 nm and 365 nm (E250:365). Our results showed quite different results during the two years studied. In the summer of 2012, when there was higher rainfall, variations in Zmix were correlated to the optical factors associated with DOM quality, while in the drier summer of 2013 Chl-a, TSS and fetch were the variables that more explained Zmix. It suggests that DOM regulates the Zmix in the rainy periods in the studied tropical lakes and that control is determined by the balance between the DOM input (runoff) and output (such as photodegradation) of the aquatic systems. In reduced rain conditions (summer 2013), the factors responsible by chemistry photodegradation of DOM were predominant, and the organic matter was no longer controlling Zmix, which was driven by internal mixing, productivity, and the wind (Chl-a, TSS and fetch). In this study we showed how changes in precipitation might cause shifts in the factors that regulate the epilimnion thickness in tropical lakes.  相似文献   

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Ultraviolet–visible absorption spectral slope ratios SR (slope in 275–295 nm divided by slope in 350–400 nm) and humification index (HIX, integrated fluorescence emission in 435–480 nm divided by that in 435–480 and 300–345 nm) were compared when characterizing chromophoric dissolved organic matter (CDOM) in three humic acids and 44 whole water samples. HIX increased with increasing pH for humic acids, while their SR showed much more complicated dependencies on pH. There was a negative correlation between SR and HIX. SR increased in the order terrestrial coal/peat < terrestrial soil/river < seawater, while HIX increased in the order seawater < terrestrial soil/river < terrestrial coal/peat. The comparative study in this work indicates that terrestrially derived CDOM has higher HIX and lower SR than marine CDOM. Investigators may potentially use these two indices to compare qualitatively the character of CDOM in different sources (e.g., terrestrial vs. marine).  相似文献   

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江苏省西部湖泊溶解性有机物光谱学特征和来源解析   总被引:11,自引:2,他引:9  
利用光谱学手段研究江苏省西部湖泊表层水体中溶解性有机物(DOM)组成与结构,并对其来源进行分析.单位浓度可溶性有机碳在254和280 nm波长下的吸光度值(SUVA)测定结果表明,各湖泊芳香性程度及分子量大小依次为邵伯湖>天岗湖>白马湖>石臼湖>洪泽湖>固城湖>骆马湖>高邮湖>宝应湖.特定波长下吸光度的比值(E2/E3、E3/E4)显示邵伯湖和白马湖中的DOM结构复杂、分子量大、苯环多,以腐殖酸为主要成分;其它湖泊的DOM腐殖化程度较低,以富里酸为主.指数函数曲线斜率(S275~295nm)拟合结果也同样表明邵伯湖DOM分子量最大,而宝应湖最低.各湖泊荧光指数和生物指数分别处于1.13~1.30和0.47~0.67范围内,体现出DOM强烈的陆源性.四个主要荧光峰的相对荧光强度之间均存在良好的相关性,表明这些湖泊的类腐殖酸及类蛋白物质可能有着相同的来源.结合这些湖泊的特征及流域经济发展水平,可以初步推断经入湖河流携带的由农业及其下游产业产生的有机质是江苏西部湖泊中DOM的主要来源.  相似文献   

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In this study, samples were taken from three contrasting freshwater sources and amended with salt in order to determine the influence of salinity and dissolved organic matter (DOM) composition on DOM recovery via ultrafiltration and solid phase extraction (SPE) with C18 disks. Salt addition caused variable recovery of DOM when using C18 SPE, and ultraviolet–visible spectroscopic characterization of the extracted material showed spectral responses that varied among sample sources. In contrast, increasing sample salinity from 0 to 30 ppt consistently caused a 15–25% reduction in the amount of high molecular weight DOM isolated by ultrafiltration for both dissolved organic carbon (DOC) and chromophoric DOM (CDOM), regardless of DOM composition. We hypothesize that a change in conformation (such as coiling or disaggregation) of DOM molecules occurs in the presence of salt, allowing them to pass through the ultrafiltration membrane and thereby decreasing the DOM retained by ultrafiltration. These results are important because they demonstrate that changes in salinity can influence DOM recovery in estuaries. Interpretation of DOM characteristics along estuarine gradients needs to account for potential artifacts introduced by sample isolation techniques.  相似文献   

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The characteristics of chromophoric dissolved organic matter (CDOM) were studied in Hudson Bay and Hudson Strait in the Canadian Arctic. Hudson Bay receives a disproportionately large influx of river runoff. With high dissolved organic matter (DOM) concentrations in Arctic rivers the influence of CDOM on coastal and ocean systems can be significant, yet the distribution, characteristics and potential consequences of CDOM in these waters remain unknown. We collected 470 discrete water samples in offshore, coastal, estuarine and river waters in the region during September and October 2005. Mixing of CDOM appeared conservative with salinity, although regional differences exist due to variable DOM composition in the rivers discharging to the Bay and the presence of sea-ice melt, which has low CDOM concentrations and low salinity. There were higher concentrations of CDOM in Hudson Bay, especially in coastal waters with salinities <28<28, due to river runoff. Using CDOM composition of water masses as a tracer for the freshwater components revealed that river runoff is largely constrained to nearshore waters in Hudson Bay, while sea-ice melt is distributed more evenly in the Bay. Strong inshore–offshore gradients in the bio-optical properties of the surface waters in the Hudson Bay cause large variation in penetration of ultraviolet radiation and the photic depth within the bay, potentially controlling the vertical distribution of biomass and occurrence of deep chlorophyll maxima which are prevalent only in the more transparent offshore waters of the bay. The CDOM distribution and associated photoprocesses may influence the thermodynamics and stratification of the coastal waters, through trapping of radiant heating within the top few meters of the water column. Photoproduction of biologically labile substrates from CDOM could potentially stimulate the growth of biomass in Hudson Bay coastal waters. Further studies are needed to investigate the importance of terrestrial DOM in the Hudson Bay region, and the impact of hydroelectric development and climate change on these processes.  相似文献   

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