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1.
Matthew P. Miller Bailey E. Simone Diane M. McKnight Rose M. Cory Mark W. Williams Elizabeth W. Boyer 《Aquatic Sciences - Research Across Boundaries》2010,72(3):269-275
In their article, “New light on a dark subject: On the use of fluorescence data to deduce redox states of natural organic
matter,” Macalady and Walton-Day (2009) subjected natural organic matter (NOM) samples to oxidation, reduction, and photochemical transformation. Fluorescence spectra
were obtained on samples, which were diluted “to bring maximum uvvisible absorbance values below 1.0.” The spectra were fit
to the Cory and McKnight (2005) parallel factor analysis (PARAFAC) model, and consistent variation in the redox state of quinone-like moieties was not detected.
Based on these results they concluded that fitting fluorescence spectra to the Cory and McKnight (2005) PARAFAC model to obtain information about the redox state of quinone-like moieties in NOM is problematic. Recognizing that
collection and correction of fluorescence spectra requires consideration of many factors, we investigated the potential for
inner-filter effects to obscure the ability of fluorescence spectroscopy to quantify the redox state of quinone-like moieties.
We collected fluorescence spectra on Pony Lake and Suwannee River fulvic acid standards that were diluted to cover a range
of absorbance wavelengths, and fit these spectra to the Cory and McKnight (2005) PARAFAC model. Our results suggest that, in order for the commonly used inner-filter correction to effectively remove inner-filter
effects, samples should be diluted such that the absorbance at 254 nm is less than 0.3 prior to the collection of fluorescence
spectra. This finding indicates that inner-filter effects may have obscured changes in the redox signature of fluorescence
spectra of the highly absorbing samples studied by Macalady and Walton-Day (2009). 相似文献
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峡谷分层型水源水库表层沉积物溶解性有机物光谱特征 总被引：7，自引：1，他引：6
结合三维荧光光谱技术（EEMs）与紫外吸收光谱（UV-vis），并利用平行因子分析（PARAFAC）的方法，对金盆水库表层沉积物中溶解性有机质（DOM）光谱的空间分布特征及来源进行分析，并探讨沉积物DOM的荧光组分与可溶性有机氮（SON）、可溶性无机氮（SIN）之间的相关性.结果表明，金盆水库表层沉积物DOM由3类荧光组分组成，分别是类富里酸C1（235 nm，315 nm/430 nm）、类色氨酸C2（220 nm，275 nm/330 nm）和类胡敏酸C3（265 nm/520 nm），各组分荧光强度占总荧光强度百分比的平均值分别为43.15%、31.54%和25.31%.表层沉积物DOM浓度在空间上呈现从上游到主库区先减少后增加的趋势.光谱斜率S275-295、S350-400和光谱斜率比SR反映出各采样点陆源与内源占比的差异性.荧光指数、自生源指标和腐殖化指标都表明金盆水库沉积物DOM的来源具有内源与陆源双重特征.相关性分析表明，表层沉积物DOM各组分与SON和SIN均呈显著正相关，说明DOM与氮元素的迁移转化密切相关. 相似文献
4.
周村水库汛期暴雨中溶解有机物(DOM)的光谱特征及来源解析 总被引：2，自引：2，他引：0
运用三维荧光光谱（EEMs）技术结合平行因子分析法（PARAFAC），对周村水库夏季两场暴雨不同降雨历时以及分子量的溶解有机物光谱特征和来源进行分析.结果表明：周村水库不同暴雨荧光光谱中出现了5种组分，分别为类腐殖质（C1、C2）、可见区富里酸（C3）和类蛋白（C4、C5）；相关性分析显示C1与C2、C3、C4以及C5具有显著的相关性，C2与C3具有显著的相关性，C3与C4以及C5具有显著的相关性；同一分子量下的雨水有机质总荧光强度以及各组分荧光强度随着降雨历时的增加均呈下降趋势，并且在各个历时和分子量间差异明显；同一降雨历时下，第一场暴雨总荧光强度随着分子量的减少而增加，第二场暴雨总荧光强度随着分子量的减少而减少；两场暴雨都呈现自生源的特征，其中第一场暴雨具有以陆源输入为主的特征；组分C1和C3与水质参数硝态氮、氨氮、总氮以及有机碳呈显著相关性.通过对暴雨在不同降雨历时以及分子量DOM光谱特征研究，可以进一步分析水库外源输入的天然有机质特征，为水库水质管理提供技术支持. 相似文献
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Zhongwu Li Hao Peng Binggeng Xie Chun Liu Xiaodong Nie Danyang Wang Mei Huang Haibing Xiao Lin Shi Xuqin Zhang Jieyu Jiang 《水文研究》2020,34(6):1446-1459
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
6.
蓝藻水华暴发和衰亡对太湖有色可溶性有机物的影响 总被引：1，自引：1，他引：0
利用平行因子分析(PARAFAC)技术对藻华暴发季节太湖梅梁湾和开敞区水样中有色可溶性有机物(CDOM)的三维荧光光谱进行分析,获得代表类酪氨酸、类色氨酸和类腐殖酸等3种荧光组分,这3个组分的荧光得分值均与叶绿素a浓度呈极显著正相关,其中类腐殖酸物质荧光得分值占总分值的比例也与叶绿素a浓度极显著正相关,由此可以推测,蓝藻水华可能是太湖CDOM的一个重要来源,并极大地影响了湖泊CDOM的组成结构.为进一步探索蓝藻水华对湖泊CDOM的影响,于太湖梅梁湾湖岸进行藻华暴发和衰亡模拟试验.PARAFAC结果显示,模拟试验水样CDOM的三维荧光图谱同样含有3个组分,其中类酪氨酸和类色氨酸荧光峰位置与湖泊水样基本相同,而类腐殖酸物质荧光峰则有一定程度的蓝移,表明培养试验中有新的内源类腐殖酸物质产生.利用PARAFAC模型中的得分值计算后发现,初始叶绿素a浓度越高,类腐殖酸物质所占比例越大,而实验结束时添加了高浓度和中等浓度藻的2个处理中类腐殖酸物质对荧光的贡献率也有显著提高.因此,藻华的长期暴发可以显著改变湖泊CDOM的组成,导致类腐殖酸物质比例提高. 相似文献
7.
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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《Limnologica》2021
The influence of dissolved organic matter (DOM) on mineral extraction from salt lake brines depend on DOM quality. This study contributes to our knowledge of DOM’s metal binding behavior in hypersaline environments by characterization of DOM from lakes in the Qaidam Basin, i.e., Qarhan Lake (LQDOM), Da Qaidam (DQDOM) and West Ginair Salt Lake (WGDOM). The DOM was fractionated based on solid phase extraction (SPE) and ultrafiltration (UF), and the spectral and metal binding behavior of these fractions were studied by absorption spectroscopy, Pb(II) titration techniques and fluorescence parallel factor (PARAFAC) analysis. The results showed that bulk DOM generally contained more dissolved organic carbon (DOC), lower specific UV absorbance (SUVA254), higher fluorescence and biological indices, comparable humification index, and lower condition stability constants compared to the other nature waters. Compared with UF, SPE-derived DOM exhibited higher DOC recovery and aromaticity and lower carbohydrate yield. It appeared that the SPE procedure used affects the spectral composition of bulk DOM to a larger extent than UF. Source and molecular weight (MW)-dependent differences in abundance and quality of brine DOM was indicated by higher SUVA254 in high MW DOM, for LQDOM and DQDOM, and humic-like fluorophores were mainly in high MW-DOM in each lake. Moreover, the high MW humic-like component exhibited higher metal binding potential than the bulk and low MW counterparts for LQDOM and DQDOM, while the inverse was observed for WGDOM. This study revealed the effects of isolation techniques on interpretation of DOM characteristics, and meanwhile highlighted the importance of origin- and MW-dependent DOM in manipulating the behavior, fate, and bioavailability of heavy metals in salt lake brine. 相似文献
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High-performance thin-layer chromatography with automated multiple development (AMD-HPTLC) was applied for the examination of pulp mill bleachery effluents from an alkali-oxygen-peroxide (EOP) bleaching stage of a sulfite pulp. A gradient based on methanol and dichloro-methane was developed for the separation of the effluent compounds over a wide range of migration distances. A series of reference substances such as lignin phenols and other aromatic acids, aldehydes, and alcohols as well as two resin acids were investigated in parallel using the AMD-HPTLC method. Characterization of the effluent compounds was possible using the migration distances and the recorded spectra. The composition of different samples of effluent were found to be very similar. The application of the AMD-HPTLC to effluent fractions from acidic liquid-liquid extraction using diethyl ether and from RP C18 solid-phase extraction allowed us to follow the behaviour of the effluent compounds in the extraction procedure. 相似文献
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以艾比湖流域主要入湖河流为研究对象，在5月（丰水期）和8月（枯水期）分别沿博尔塔拉河（博河）和精河进行采样，采用平行因子模型（PARAFAC）和三维荧光区域积分法对水体三维荧光特性进行研究并对其与水质的关系在枯、丰水期下的变化进行探讨.结果表明①河流DOM在枯水期与丰水期都含有C1（240、425 nm） UVC类腐殖质，C2（225、290 nm）紫外区内络氨酸类有机物，C3（230/280、330 nm）蛋白类有机物，C4（265、260 nm）腐殖质类共4种组分.通过对水体三维荧光进行区域积分可以看出DOM荧光成分的占比在不同时期的变化.博河在枯水期时EEM光谱中的区域Ⅲ富里酸含量低于丰水期，枯水期时区域Ⅱ芳香类蛋白质、区域Ⅳ可溶性微生物代谢物以及区域Ⅴ类腐殖质酸高于丰水期；对于精河来说，区域Ⅱ芳香类蛋白质和区域Ⅳ可溶性微生物代谢物在枯水期的含量高于丰水期，区域Ⅲ富里酸和区域Ⅴ类腐殖质酸的含量枯水期低于丰水期，这表明水体腐质化程度较高.②本研究选取了一些常规的荧光指数来描述枯、丰水期水体的荧光指数特性.经研究发现，精河的荧光指数、自生源指数和腐殖化指数在不同时期的变化幅度较小，而博河的变化幅度较大.③将荧光指数与水质参数进行相关性分析并建模，结果表明枯水期自生源指数（BIX）与化学需氧量呈显著正相关，相关系数R=0.688；丰水期时BIX与铵态氮浓度呈显著负相关，相关系数R=-0.493.通过对比分析艾比湖主要入湖河流的三维荧光光谱特性与水质在枯、丰水期时的关系进一步表明水体中DOM的特性以及在枯、丰水期下的差异，为艾比湖流域的治理改善提供一定的理论支持和参考依据. 相似文献
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《中国科学:地球科学(英文版)》2021,(7)
We applied stable carbon isotopes, ultraviolet-visible absorption(UV-Vis), fluorescence excitation-emission matrices spectroscopy(EEMs), and Fourier transform ion cyclotron resonance mass spectrometry(FT-ICR-MS) to investigate the chemical composition and sources of the dissolved organic matter(DOM) in both the water column and pore water in Xiangshan Bay, a representative semi-enclosed and eutrophic bay in Zhejiang Province, China. One protein-like fluorescent component(C1) and two humic-like fluorescent components(C2 and C3) were identified by PARAFAC modeling. The concentration of dissolved organic carbon(DOC), the relative intensities of C2, C3, and black carbon-like compounds are all negatively correlated with salinity, indicating that there is a dilution effect of terrestrial signals by seawater in Xiangshan Bay. The differences in light penetration ability of Xiangshan Bay cause different degrees of photo-degradation, which may play an important role in the transformation of organic matter in Xiangshan Bay. The weak correlation between the C1 fluorescent component and salinity indicates that autochthonous sources cannot dominate the protein-like FDOM in the Xiangshan Bay drainage area. Multiple sources(such as anthropogenic inputs and release of pore water) also affect the distribution of the protein-like fluorescent component under eutrophication conditions. The relative proportion of the protein-like fluorescent component in Xiangshan Bay is on a medium level in China and anthropogenic inputs may be a significant source of DOM in coastal bays. 相似文献
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以艾比湖主要入湖河流——精河与博尔塔拉河为研究对象,分别分析了精河与博尔塔拉河的水体溶解性有机质(DOM)的组成结构及水质参数与荧光指数的关系.利用平行因子分析法对三维荧光光谱(EEM)分析发现,精河与博尔塔拉河均含有C1(260/420 nm)腐殖酸等有机质、C2(240,240/490 nm)UVC类腐殖质、C3(220/280,300/450 nm)蛋白质类有机质和C4(260,270/530 nm)类腐殖质,且不同荧光组分结构具有一定差异性.为了进一步了解DOM组分特征,采用三维荧光区域积分法分析各区域标准体积百分比,结果表明精河与博尔塔拉河EEM的区域Ⅰ与区域Ⅱ蛋白质有机质含量最高,区域Ⅲ富里酸含量最低.相关性分析表明,主要入湖河流的水质参数与荧光指数中,自生源指数(BIX)与总氮(TN)浓度以及腐殖化指数(HIX)与铵态氮(NH_4~+-N)浓度的相关性较强,相关系数分别为0.831和0.684,且具有显著性;HIX与TN浓度的相关系数为0.604,达到显著性水平.进而对相关性较强的水质参数与荧光指数进行3次拟合,其中HIX与NH_4~+-N浓度的拟合效果最好,相关性系数为0.908,其次是BIX与TN浓度,相关性系数为0.844.总之,通过分析精河与博尔塔拉河三维荧光特征,以及探讨荧光指数与水质参数的关系,可为治理干旱区水环境问题提供理论依据和参考. 相似文献
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The mortality, growth and fecundity of transplanted adult mussel (Mytilus edulis) and barnacle (Balanus glandula) populations near a kraft pulp mill outfall at Port Mellon, British Columbia, were determined. The results indicated that adults of both species were tolerant of bleached kraft pulp mill effluent and survived near the pulp mill outfall. However, the growth rates of both species were retarded when compared with those at the control station. The reproductive activities of the transplanted barnacles were also impaired. 相似文献
16.
The fluorescent properties of dissolved organic matter (DOM) enable comparisons of humic‐like (H‐L) and fulvic‐like (F‐L) fluorescence intensities with dissolved organic carbon (DOC) in aquatic systems. The fluorescence‐DOC relationship differed in gradient, i.e. the fluorescence per gram of carbon, and in the strength of the correlation coefficient. We compare the fluorescence intensity of the F‐L and H‐L fractions and DOC of freshwater DOM in north Shropshire, England, featuring a river, wetland, spring, pond and sewage DOM sources. Correlations between fluorescence and DOC varied between sample sites. Wetland water samples for the F‐L peak gave the best correlation, r = 0·756; the lowest correlation was from final treated sewage effluent, r = 0·167. The relationship between fluorescence and DOC of commercially available International Humic Substances Society standards were also examined and they generally showed a lower fluorescence per gram of carbon for the F‐L peak than the natural samples, whereas peat wetland DOM gave a greater fluorescence per gram of carbon than river DOM. Here, we propose the strength of the fluorescence–DOC correlation to be a useful tool when discriminating sources of DOM in fresh water. Copyright © 2007 John Wiley & Sons, Ltd. 相似文献
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为探究引黄水源水库——门楼水库平水期和丰水期有色可溶性有机物(CDOM)的组成特征、来源及差异,运用紫外—可见光谱技术(UV-vis)和三维荧光光谱(EEMs)技术,结合平行因子分析法(PARAFAC)分析2022年5月(平水期)和2022年7月(丰水期)有色可溶性有机物含量及组分变化。研究结果表明:PARAFAC识别出2类荧光组分,分别是C1(Ex=355 nm,Em=476 nm,类腐殖质组分)和组分C2(Ex=225 nm,Em=320 nm,类蛋白组分);丰水期CDOM组分荧光强度显著高于平水期。CDOM光谱参数表明,门楼水库水体处于中营养状态,水体CDOM受新生内源和外源输入共同影响,以自生源为主;水库CDOM具有相对分子量小、腐殖化程度较弱的特点。丰水期水库富营养化水平和CDOM相对浓度低于平水期;丰水期CDOM疏水性组分比例和芳香化程度高于平水期。水质理化指标、CDOM组分和光谱参数相关性分析结果表明SUVA260和SUVA280与DOC呈显著负相关,说明紫外—可见光谱参数在一定程度上可以用来估算DOC的浓度;Chl.a浓度作为... 相似文献
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Frequent heavy rainfalls during the East Asian summer monsoon drastically increase water flow and chemical loadings to surface waters. A solid understanding of hydroclimatic controls on watershed biogeochemical processes is crucial for water quality control during the monsoon period. We investigated spatio‐temporal variations in the concentrations and spectroscopic properties of dissolved organic matter (DOM) and the concentrations of trace metals in Hwangryong River, Korea, during a summer period from the relatively dry month of June through the following months with heavy rainfall. DOM and its spectroscopic properties differed spatially along the river, and also depended on storm and flow characteristics around each sampling time. At a headwater stream draining a forested watershed, the concentrations (measured as dissolved organic carbon (DOC)), aromaticity (measured as specific UV absorbance at 254 nm), and fulvic acid‐ and protein‐like fluorescence of DOM were higher in stormflow than in baseflow waters. DOC concentrations and fluorescence intensities increased along the downstream rural and urban sites, in which DOC and fluorescence were not higher in stormflow waters, except for the ‘first flush’ at the urban site. The response of DOM in reservoir waters to monsoon rainfalls differed from that of stream and river waters, as illustrated by storm‐induced increases in DOM aromaticity and fulvic‐like fluorescence, and no significant changes in protein‐like fluorescence. The results suggest that surface water DOM and its spectroscopic properties differentially respond to changes in hydroclimatic conditions, depending on watershed characteristics and the influence of anthropogenic organic matter loadings. DOC concentrations and intensities of spectroscopic parameters were positively correlated with some of the measured trace metals (As, Co, and Fe). Further research will be needed to obtain a better understanding of climate effects on the interaction between DOM and trace metals. Copyright © 2006 John Wiley & Sons, Ltd. 相似文献
20.
The molecular characteristics of dissolved organic matter (DOM) reflect both its source material and its biogeochemical history. In glacial systems, DOM characteristics might be expected to change over the course of a melt season as changes in the glacier drainage system cause the mobilization of DOM from different OM pools. To test this hypothesis we used Principal Components Analysis (PCA) of synchronous fluorescence spectra to detect and describe changes in the DOM in meltwater from a glacier system in the Coast Mountains of northern British Columbia, Canada. For most of the melt season, the dominant component of subglacially routed meltwater DOM is characterized by a tyrosine‐like fluorophore. This DOM component is most likely derived from supraglacial snowmelt. During periods of high discharge, a second component of DOM is present which is humic in character and similar to DOM sampled from a nearby non‐glacial stream. This DOM component is inferred to be derived from a moss‐covered soil environment that has been glacially overrun. It is probably entrained into glacial melt waters when the supraglacial meltwater flux exceeds the capacity of the principal subglacial drainage channels and water floods areas of the glacier bed that are normally isolated from the subglacial drainage system. Another source of DOM also appears to be mobilized during periods of high air temperatures. It is characterized by both humic and proteinaceous fluorophores and may be derived from the drainage of supraglacial cryoconite holes. Copyright © 2009 John Wiley & Sons, Ltd. 相似文献