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1.
The determination of optical properties of organic matter using spectroscopic techniques is a powerful tool for the characterization of humic substances (HS) in soils and sediments because of sensitivity, specificity and sample throughput. However, basic spectroscopic techniques have practical limitations because of the similarity in the optical properties of many HS. To improve resolution, the combination of excitation-emission matrix (EEM) fluorescence and parallel factor analysis (PARAFAC) was applied for characterizing fulvic acid (FA) and humic acid (HA) fractions from soils and sediments of two estuarine environments in Spain. Five fluorescent components were identified by EEM-PARAFAC and were found in both FA and HA fractions, consistent with the new paradigm of HS as supramolecular associations as well as the ubiquity of the HS components in the environment. Their contribution was, however, different between the FA and HA fractions. Two different, humic-like, fluorescent components were representative of FA and HA fractions, respectively. The spectral characteristics of these components were similar to previously reported PARAFAC components in dissolved organic matter (DOM) in a wide range of environments, suggesting their applicability in assessing OM quality and environmental dynamics. A microbial humic-like component was much more abundant in FA than in HA fractions. Furthermore, principal component analysis clarified that the two identified protein-like components, were enriched in sediment HA compared to soil HA, suggesting a larger contribution of refractory algaenan in sediment HA. The results of the present study demonstrate that EEM-PARAFAC is a useful technique for the biogeochemical characterization of soil and sedimentary HS.  相似文献   

2.
In this study, the variations in the fluorescent components of dissolved organic matter (DOM) were tracked for an aerobic submerged membrane bioreactor (MBR) at three different operation stages (cake layer formation, condensation, and after cleaning). The fluorescent DOM was characterized using excitation–emission matrix (EEM) spectroscopy combined with parallel factor analysis (PARAFAC). Non-aromatic carbon structures appear to be actively involved in the membrane fouling for the cake layer formation stage as revealed by much higher UV-absorbing DOM per organic carbon found in the effluent versus those inside the reactor. Four fluorescent components were successfully identified from the reactor and the effluent DOMs by EEM-PARAFAC modeling. Among those in the reactor, microbial humic-like fluorescence was the most abundant component at the cake layer formation stage and tryptophan-like fluorescence at the condensation stage. In contrast to the reactor, relatively similar composition of the PARAFAC components was exhibited for the effluent at all three stages. Tryptophan-like fluorescence displayed the largest difference between the reactor and the effluent, suggesting that this component could be a good tracer for membrane fouling. It appears that the fluorescent DOM was involved in membrane fouling by cake layer formation rather than by internal pore adsorption because its difference between the reactor and the effluent was the highest among all the four components, even after the membrane cleaning. Our study provided an insight into the fate and the behavior fluorescent DOM components for an MBR system, which could be an indicator of the membrane fouling.  相似文献   

3.
In this study, biodegradation of natural organic matter (NOM) in a biological aerated filter (BAF) as pretreatment of UF treating river water was investigated. Photometric measurement, three-dimensional excitation–emission matrix (EEM) fluorescence spectroscopy and liquid chromatography with online organic carbon detector (LC-OCD) were used to investigate the fate of NOM fractions in the BAF + UF process. Results showed that the BAF process could effectively remove particles and parts of dissolved organic matter, which led to a lower NOM loading in the UF system, but different NOM fractions showed different biodegradation potentials. Further biodegradation batch experiments confirmed this observation and identified that polysaccharides and proteins (quantified using photometric methods) contained a large proportion of readily biodegradable matter while humic substances were mainly composed of inert organic substances. According to EEM measurements, it is evident that protein-like substances were more readily eliminated by microorganisms than humic-like substances. LC-OCD data also supported the phenomena that the polysaccharides and large-size proteins were more degradable than humic substances.  相似文献   

4.
Yang XL  Song HL  Chen M  Cheng B 《Bioresource technology》2011,102(20):9490-9496
The effect of polymeric ferric chloride (PFC) addition on phosphorus removal and membrane fouling were investigated in an anoxic/oxic submerged membrane bioreactor. The total phosphorus concentration in effluent averaged at 0.26 mg/L with PFC addition of 10-15 mg/L, while the rate of membrane fouling increased 1.6 times over the control MBR (without PFC addition). Three-dimensional excitation-emission matrix fluorescence spectroscopy and Gel Filtration Chromatography analysis indicated that soluble microbial byproduct-like materials and large molecules (M(W)>100 kDa) were one of the main contributors of biofouling. Fourier transform infrared spectrum confirmed that the major components of the cake layer were proteins and polysaccharides materials. Scanning electron microscopy demonstrated that membrane surfaces were covered with compact gel layer formed by organic substances and Energy Dispersive X-ray analysis indicated that ferric metals were the most important inorganic pollutants. Consequently, soluble organic substances and dose of PFC should be controlled to minimize membrane fouling.  相似文献   

5.
To investigate the seasonal and interannual dynamics of dissolved organic matter (DOM) in the Yangtze Estuary, surface and bottom water samples in the Yangtze Estuary and its adjacent sea were collected and characterized using fluorescence excitation-emission matrices (EEMs) and parallel factor analysis (PARAFAC) in both dry and wet seasons in 2012 and 2013. Two protein-like components and three humic-like components were identified. Three humic-like components decreased linearly with increasing salinity (r>0.90, p<0.001), suggesting their distribution could primarily be controlled by physical mixing. By contrast, two protein-like components fell below the theoretical mixing line, largely due to microbial degradation and removal during mixing. Higher concentrations of humic-like components found in 2012 could be attributed to higher freshwater discharge relative to 2013. There was a lack of systematic patterns for three humic-like components between seasons and years, probably due to variations of other factors such as sources and characteristics. Highest concentrations of fluorescent components, observed in estuarine turbidity maximum (ETM) region, could be attributed to sediment resuspension and subsequent release of DOM, supported by higher concentrations of fluorescent components in bottom water than in surface water at two stations where sediments probably resuspended. Meanwhile, photobleaching could be reflected from the changes in the ratios between fluorescence intensity (Fmax) of humic-like components and chromophoric DOM (CDOM) absorption coefficient (a355) along the salinity gradient. This study demonstrates the abundance and composition of DOM in estuaries are controlled not only by hydrological conditions, but also by its sources, characteristics and related estuarine biogeochemical processes.  相似文献   

6.
Dissolved organic matter (DOM) in the waters from Lake Biwa, Japan was fractionated using tangential flow ultrafiltration, and subsequently characterized by fluorescence properties and amino acids. While major dissolved organic carbon (DOC), UV absorbance (Abs), humic-like fluorescence (Flu) and total hydrolyzed amino acids (THAA) occurred in the less than 5 kDa molecular size fraction, they were not evenly distributed among various molecular size fractions. Flu/Abs ratios increased, and THAA/DOC ratios decreased with decreasing molecular size. Humic-like fluorescence occurred in all molecular size fractions, but protein-like fluorescence only occurred in the 0.1 m-GF/F fraction. Subtle differences in amino acid compositions (both individuals and functional groups) were observed between various molecular size fractions, this may indicate the occurrence of DOM degradation from higher to lower molecular weight. The results reported here have significance for further understanding the sources and nature of DOM in aquatic environments.  相似文献   

7.
Abstract

Root exudates are considered to have an important role in mobility and bioavailability of heavy metals. High molecular weight (HMW) substances are the main components of root exudates, however, knowledge about their interactions with heavy metals is lacking. In the present study, Pb(II) complexation of the HMW fluorescent fractions in root exudates from Salicornia europaea L. was investigated using excitation emission matrix (EEM) fluorescence spectroscopy. Two protein-like fluorescence peaks were identified in the EEM spectrum of root exudates. The fluorescence of both peaks was clearly quenched by Pb(II). The values of conditional stability constants, log Ka, for these two protein-like fluorescence peaks were 4.14 and 3.79. This indicates that the fluorescent substances are strong Pb(II) complexing organic ligands.  相似文献   

8.
Solid surface fluorescence excitation-emission matrix (EEM) is developed a potential method to characterize soil organic matter (SOM). Solid surface EEM spectroscopy with parallel factor analysis (PARAFAC) and hierarchical cluster analysis (HCA) is used to extract fluorescent components, to seek latent factors, and to investigate spatial distribution of SOM. Soil samples were collected from four native halophyte and two furrow-irrigated soil profiles, i.e. Comm. Salicornia europaea (CSE), Comm. Suaeda glauca (CSG), Comm. Kalidium cuspidatum (CKC), Comm. Sophora alopecuroides (CSA), corn fields (CFD), and wheat fields (WFD). SOM contained six fluorescent components: microbial/terrestrial fulvic-like fluorescent components (C1), tryptophan-like/lignin-derived phenol fluorescent components (C2), terrestrial humic-like fluorescent component (C3), lignin oxidative degradation by-products (C4 and C5), and amino acids (C6). The C 4 and C5 were the representative components of SOM within the CSE, CSG, CKC, CSA and CFD soil profiles, while the C2 and C6 were dominated within the WFD soil profile. The C4, C5, C1 and C2 were latent factors, and they could roughly distinguish SOM within the whole saline soil profiles except the CFD. A humification index (H/L) deduced from the fluorescent components, was very suitable to indicate humification levels of SOM. Humification levels of SOM within the halophyte soil profiles decreased with soil depth, but the opposite trends within the furrow-irrigated soil profiles. The H/L was closely correlated with exchangeable sodium percentage (ESP), and humification levels increased with the decreasing ESP. Soil surface EEM may not only indicate organic matter fractions of saline soils, but may be transferred to other types of landscape.  相似文献   

9.
Surface-flow wetlands constructed with Acorus and Typha plants, connected to a wastewater treatment plant, were investigated with respect to organics (dissolved organic matter), anions (nitrate, sulfate, and phosphate), metals (Cu, Ni, Zn, Fe, and Mn), and metalloids (As). The results of the research indicated: (1) effluent organic matter (EfOM), based on dissolved organic carbon (DOC), was not efficiently removed by the wetlands. However, the hydrophobic, transphilic, and hydrophilic EfOM fractions varied throughout the wetlands, as identified by XAD-8/4 resins. (2) Nitrate, as compared to sulfate and phosphate, was efficiently removed, especially in the Typha wetland pond that had long retention time, under anoxic condition. (3) Most of the heavy metals were ineffectively removed via the wetland ponds. However, the iron concentration increased in the Typha wetland pond, which was probably due to its reduction under anoxic condition.  相似文献   

10.
《Process Biochemistry》2010,45(10):1699-1706
Four flat-sheet membrane modules, which were operated under four different filtration modes but with the same treatment capacity, were used to treat synthetic wastewater in a submerged membrane bioreactor (MBR). Particle size distribution (PSD), gel filtration chromatography (GFC), capillary suction time (CST), and three-dimensional excitation–emission matrix (EEM) fluorescence spectroscopy were used to characterize membrane fouling properties. The high instantaneous flux induced faster fouling rate and continuous filtration mode was the most applicable filtration mode in this study. The average particle size of all foulants was smaller than that of bulk sludge; and the higher the instantaneous flux was adopted, the larger the average particle size of foulants would be. Only macromolecule substances were detected in all the foulants. The macromolecule substances in the influent were degraded by microorganism and retained by membrane, and small molecular substances could pass through membrane pores to enter the effluent. The membrane foulants had poorer dewaterability compared to the mixed liquor confirmed by CST measurement. Although there were several peaks associated with protein-like fluorophores, fulvic acid-like substances and humic acid-like organics in soluble microbial products (SMP) and extracellular polymeric substances (EPS) sample, it was found that the dominant fluorescence substances in membrane foulants were protein-like substances.  相似文献   

11.
Binary aqueous solutions of bovine serum albumin (BSA) and beta-lactoglobulin (bLG) were subject to flux-stepping and constant flux ultrafiltration to identify the apparent critical flux and to study the mechanisms and factors affecting fouling when the membrane is permeable to one protein component. Membranes from these filtration experiments were analyzed using matrix-assisted laser desorption ionization mass spectrometry (MALDI-MS) to locate and quantify levels of fouling below and above the apparent critical flux. Hydrophilic (PLTK) regenerated cellulose and hydrophobic (PBTK) polysulfone asymmetric membranes were used, both of 30 kDa nominal molecular weight cut-off. For the hydrophilic PLTK membrane, protein deposition was shown to depend on electrostatic forces, exhibiting little or no fouling when the proteins had the same charge sign as that of the membrane. This was found to apply for both dilute equal mass-per-unit-volume and equimolar binary mixtures. For the PBTK membrane, hydrophobic protein-membrane attractive forces were sufficiently strong to cause deposition of bLG even in the presence of repulsive electrostatic forces. For the PBTK membrane deposition exceeded monolayer coverage below and above apparent critical flux conditions but for the PLTK membrane this generally occurred when the apparent critical flux was exceeded. MALDI-MS was shown to be a facile direct analytical technique for individually quantifying adsorbed proteins on membrane surfaces at levels as low as 50 fmol/mm(2). The high levels of compound specificity inherent to mass spectrometry make this approach especially suited to the quantification of individual components in mixed deposits. In this study, MALDI-MS was found to be successful in identifying and quantifying the protein species responsible for fouling.  相似文献   

12.
Minimization and management of membrane fouling is a formidable challenge in diverse industrial processes and other practices that utilize membrane technology. Understanding the fouling process could lead to optimization and higher efficiency of membrane based filtration. Here we show the design and fabrication of an automated three-dimensionally (3-D) printed microfluidic cross-flow filtration system that can test up to 4 membranes in parallel. The microfluidic cells were printed using multi-material photopolymer 3-D printing technology, which used a transparent hard polymer for the microfluidic cell body and incorporated a thin rubber-like polymer layer, which prevents leakages during operation. The performance of ultrafiltration (UF), and nanofiltration (NF) membranes were tested and membrane fouling could be observed with a model foulant bovine serum albumin (BSA). Feed solutions containing BSA showed flux decline of the membrane. This protocol may be extended to measure fouling or biofouling with many other organic, inorganic or microbial containing solutions. The microfluidic design is especially advantageous for testing materials that are costly or only available in small quantities, for example polysaccharides, proteins, or lipids due to the small surface area of the membrane being tested. This modular system may also be easily expanded for high throughput testing of membranes.   相似文献   

13.
白洋淀沉水植物腐解释放溶解性有机物光谱特性   总被引:9,自引:2,他引:7  
利用水生植物修复受污染水体中,水生植物在秋冬季节腐烂分解会释放大量溶解性有机物(DOM),DOM可影响水环境中污染物的迁移转化,对水体中的化学和生物过程产生一定影响。因此利用紫外可见光光谱(UV-vis)结合平行因子分析法(PARAFAC)和主成分分析法(PCA)来表征和分析水生植物腐解产物中DOM的组分及其特点。UV-vis的研究表明随着腐解时间的增加,样品中DOM的腐殖化程度逐渐升高,当腐殖化程度达到最高值时,腐解进入矿化阶段,此时腐殖化程度逐渐降低。通过PARAFAC分析可以分离出3种类蛋白组分(C1、C2和C5)和2种类腐殖酸组分(C3和C4)。由PCA可以得出在腐解初期,类蛋白组分占据主导地位;随着腐解时间的增加,类蛋白组分含量逐渐降低,而类腐殖酸组分含量逐渐升高。  相似文献   

14.
In this study changes in the properties of natural organic matter (NOM) were studied during composting of sewage sludge in a laboratory experiment using the pile method. Typical physicochemical parameters were measured during 53 days of composting including humic fractions. The effects of humification on the molecular properties of humic acids (HA) were investigated by 13C CP/MAS NMR spectroscopy. On the basis of chemical analyses, 53 days of composting sewage sludge with structural material can be divided into three phases: (i) domination of rapid decomposition of non-humic, easily biodegradable organic matter (two to three weeks), (ii) domination of organic matter humification and formation of polycondensed, humic-like substances (the next two weeks), (iii) stabilization of transformed organic material and weak microbial activity. Spectroscopic characterization (13C NMR) of compost humic acids reveals changes in their structures during maturation. The changes are highly correlated with the processes taking place in bulk compost.  相似文献   

15.
Biofouling is a major reason for flux decline in the performance of membrane-based water and wastewater treatment plants. Initial biochemical characterization of biofilm formation potential and biofouling on two commercially available membrane surfaces from FilmTec Corporation were investigated without filtration in laboratory rotating disc reactor systems. These surfaces were polyamide aromatic thin-film reverse osmosis (RO) (BW30) and semi-aromatic nanofiltration (NF270) membranes. Membrane swatches were fixed on removable coupons and exposed to water with indigenous microorganisms supplemented with 1.5 mg l(-1) organic carbon under continuous flow. After biofilms formed, the membrane swatches were removed for analyses. Staining and epifluorescence microscopy revealed more cells on the RO than on the NF surface. Based on image analyses of 5-μm thick cryo-sections, the accumulation of hydrated biofoulants on the RO and NF surfaces exceeded 0.74 and 0.64 μm day(-1), respectively. As determined by contact angle the biofoulants increased the hydrophobicity up to 30° for RO and 4° for NF surfaces. The initial difference between virgin RO and NO hydrophobicities was ~5°, which increased up to 25° after biofoulant formation. The initial roughness of RO and NF virgin surfaces (75.3 nm and 8.2 nm, respectively) increased to 48 nm and 39 nm after fouling. A wide range of changes of the chemical element mass percentages on membrane surfaces was observed with X-ray photoelectron spectroscopy. The initial chemical signature on the NF surface was better restored after cleaning than the RO membrane. All the data suggest that the semi-aromatic NF surface was more biofilm resistant than the aromatic RO surface. The morphology of the biofilm and the location of active and dead cell zones could be related to the membrane surface properties and general biofouling accumulation was associated with changes in the surface chemistry of the membranes, suggesting the validity of the combination of these novel approaches for initial assessment of membrane performance.  相似文献   

16.
Dissolved organic matter (DOM) in sediment pore waters from Yangtze estuary of China based on abundance, UV absorbance, molecular weight distribution and fluorescence were investigated using a combination of various parameters of DOM as well as 3D fluorescence excitation emission matrix spectra (F-EEMS) with the parallel factor and principal component analysis (PARAFAC-PCA). The results indicated that DOM in pore water of Yangtze estuary was very variable which mainly composed of low aromaticity and molecular weight materials. Three humic-like substances (C1, C2, C4) and one protein-like substance (C3) were identified by PARAFAC model. C1, C2 and C4 exhibited same trends and were very similar. The separation of samples on both axes of the PCA showed the difference in DOM properties. C1, C2 and C4 concurrently showed higher positive factor 1 loadings, while C3 showed highly positive factor 2 loadings. The PCA analysis showed a combination contribution of microbial DOM signal and terrestrial DOM signal in the Yangtze estuary. Higher and more variable DOM abundance, aromaticity and molecular weight of surface sediment pore water DOM can be found in the southern nearshore than the other regions primarily due to the influence of frequent and intensive human activities and tributaries inflow in this area. The DOM abundance, aromaticity, molecular weight and fluorescence intensity in core of different depth were relative constant and increased gradually with depth. DOM in core was mainly composed of humic-like material, which was due to higher release of the sedimentary organic material into the porewater during early diagenesis.  相似文献   

17.
Chromophoric dissolved organic matter (CDOM) can play an important role in regulating biological production in coastal environments. Fluorescent dissolved organic matter (FDOM) is a subset of the larger CDOM pool that can be used to look at sources of CDOM. Experiments were conducted with copepods and the pelagic larvacean, Oikopleura dioica to determine if these two types of zooplankton excrete FDOM. Shipboard bottle experiments were conducted with copepods in the Gulf of Mexico, in the Mississippi River Plume in April 2001 and laboratory experiments with the pelagic larvacean, O. dioica were conducted in Oviedo, Spain in June 2001. Both copepods and O. dioica were found to excrete FDOM. Excitation/emission matrices revealed that both animals contributed to fluorescent protein pools (ex/em 275/315-350 nm) and to humic-like material (maximum ex/em 300/420 nm). The humic-like material excreted by the copepods and larvaceans was shifted toward shorter wavelengths, providing a possible unique fluorescent signature for zooplankton. Using a ratio of the humic-like fluorescence excreted by the animals (ex/em 300/420) to the humic-like fluorescence maximum in controls (ex/em 320/420 nm) showed the zooplankton could contribute nearly 50% of the Peak M fluorescence. Molecular weight analysis of the CDOM in an O. dioica excretion study showed that O. dioica excreted CDOM was primarily < 30 kDa. Both copepods and larvaceans are sources of marine FDOM and CDOM and can potentially influence the amount and type of CDOM present in coastal waters.  相似文献   

18.
One of the primary problems in membrane‐based protein separation is membrane fouling. In this study we explored the feasibility of employing Rayleigh light scattering data from fluorescence studies combined with chemometric techniques to determine whether a correlation could be established with membrane fouling phenomena. Membrane flux was measured in a dead‐end UF filtration system and the effect of protein solution properties on the flux decline was systematically investigated. A variety of proteins were used as a test case in this study. In parallel, the colloidal behavior of the protein solutions was assessed by employing multiwavelength Rayleigh scattering measurements. To assess the usefulness of Rayleigh scattering measurements for probing the colloidal behavior of proteins, a protein solution of β‐lactoglobulin was used as a base‐case scenario. The colloidal behavior of different β‐lactoglobulin solutions was inferred based on published data for this protein, under identical solution conditions, where techniques other than Rayleigh scattering had been used. Using this approach, good agreement was observed between scattering data and the colloidal behavior of this protein. To test the hypothesis that a high degree of aggregation will lead to increased membrane fouling, filtration data was used to find whether the Rayleigh scattering intensity correlated with permeate flux changes. It was found that for protein solutions which were stable and did not aggregate, fouling was reduced and these solutions exhibited reduced Rayleigh scattering. When the aggregation behavior of the solution was favored, significant flux declines occurred and were highly correlated with increased Rayleigh scattering. © 2010 American Institute of Chemical Engineers Biotechnol. Prog., 2010  相似文献   

19.
Understanding the quantity and quality of dissolved organic matter (DOM) in potential watershed sources is critical for explaining and quantifying the exports of DOM in stream runoff. Here, we examined the concentration and quality of DOM for ten watershed sources in a 12?ha forested catchment over a two-year period. DOM composition was evaluated for: throughfall, litter leachate, soil water (zero and tension), shallow and deep groundwater, stream water, hyporheic zone, and groundwater seeps. DOM quality was measured using a suite of optical indices including UV–visible absorbance and PARAFAC modeling of fluorescence excitation-emission matrices (EEMs). DOM concentrations and quality displayed a pronounced trend across watershed sources. Surficial watershed sources had higher DOM concentrations and more humic-like DOM with higher molecular weight whereas deeper groundwater sources were rich in % protein-like fluorescence. The greater % contribution of protein-like fluorescence in groundwater suggested that a larger fraction of groundwater DOM may be bioavailable. DOM for wetland groundwater was more aromatic and humic-like than that at the well-drained riparian location. Principal component analyses (PCA) revealed that the differences in surficial watershed compartments were dictated by humic-like components while groundwater sources separated out by % protein-like fluorescence. Observations from optical indices did not provide any conclusive evidence for preferential association of dissolved organic carbon (DOC) or dissolved organic nitrogen (DON) with any particular DOM quality pools.  相似文献   

20.
The fluorescence properties of dissolved organic matter (DOM) in the water of Lake Fuxian and its adjacent rivers on the Yunnan Plateau, southwestern China, were studied to specify the characterization of DOM in the lake and river waters. The fluorescence properties with the excitation–emission matrix in the water of Lake Fuxian are different from those in the river water. The differences in these properties between the lake and river water could arise not only from their sources but also from the reactivity of the photobleaching of DOM. In the lake, the supplying of allochthonous fluorescent materials from inflowing rivers to the fluorescent DOM is less significant than the photobleaching of fluorescent substances.  相似文献   

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