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1.
Four highly contaminated sediment samples obtained from three sampling locations of the Teltow Canal, Berlin, were investigated by quantitation of extractable and nonextractable organic contaminants. The selection of the anthropogenic contaminants (including chlorinated and brominated naphthalenes, 2, 4, 6‐tribromoaniline, phthalates, tri‐n‐butylphosphate, 2, 2, 4‐trimethyl‐1, 3‐pentanediol diisobutyrate, bisphenol A, butylated nitrophenols, 4‐nitrobenzoic acid, galaxolide, and tonalide) based on the results of extended GC‐MS screening analyses applied to the extracts of the sediment samples as well as to the extracts derived from selective chemical degradation procedures. In detail, alkaline hydrolyses, BBr3‐treatment and RuO4‐oxidation were applied to the pre‐extracted sediment samples in both a separate and a sequential mode.  相似文献   

2.
Organic matter of nine surface sediments from the Daya Bay was Soxhlet-extracted with a mixture of 2:1 (v/v) dichloromethane-methanol and separated into five fractions: non-aromatic hydrocarbons, aromatic hydrocarbons, ketones, alcohols, and fatty acids and asphaltenes, and analyzed to determine their bulk and biomarker composition. Marine autogenic input appears to be a major source of organic matter. Generally, non-aromatic hydrocarbons are the most dominant fraction of solvent-extractable organic matter (EOM) followed by the other four fractions in decreasing amounts: fatty acids and asphaltenes, ketones, alcohols and aromatic hydrocarbons. On average, both non-aromatic hydrocarbon fraction and fatty acid and asphaltene fraction account for approximately 40% of EOM. The sources of acyclic methyl ketones, alkanols and fatty acids were examined. For n-alkan-2-ones, allochthonous input is a more important source than marine autogenetic input; the reverse is true for n-fatty acids; for n-alkanols, allochthonous and autogenetic inputs seem comparable. Both n-alkan-2-ones and n-fatty acids in the surface sediments of different areas appear to be derived from common sources.  相似文献   

3.
Selected samples of dissolved organic matter (DOM) isolated by ultrafiltration (UDOM) have been analyzed by thermochemolysis in the presence of tetramethylammonium hydroxide (TMAH). This technique cleaves ester and ether bonds of bio‐ and geological macromolecules and releases monomer subunits and methylates them in situ as their methyl ethers and methyl esters. Compared with conventional pyrolysis, TMAH thermochemolysis avoids decarboxylation of preexisting carboxylic moieties and produces aromatic acids as their methyl esters. Various phenolic derivatives, which might originate from incorporated lignin‐derived structures, from the highly aliphatic and resistant biopolymer cutan and also from proteinaceous materials, were identified among the products produced from UDOM upon thermochemolysis. The presence of lignin derivatives in UDOM indicates input of organic matter derived from terrestrial sources. Various aromatic acids, perhaps representing the final steps in the oxidation of the side‐chain during microbial oxidation of lignin, were released upon TMAH thermochemolysis, suggesting they are structural constituents of the UDOM. Different ratios of lignin‐derived materials, commonly determined using the CuO oxidation method, such as the Δ value, indicative of the amount of lignin present, the acid/aldehyde ratio (Ad/Al)G, indicative of the extent of oxidative degradation of the lignin component, and the syringyl/guaiacyl (S/G) and p‐hydroxyphenyl/guaiacyl (P/G) ratios, indicative of the contribution for the different types of lignin, were determined.  相似文献   

4.
The degradation of dissolved organic matter (DOM) was studied in alkaline solution. The products were characterised using UV/vis spectroscopy, size‐exclusion chromatography (SEC), and by the analysis of low‐molecular‐weight organic acids (LMWOA). The degradation experiments were performed with water from a brown water lake or its isolated fulvic acid fraction and sodium hydroxide at different reaction times and temperatures. Depending on the wavelength and the reaction time, the UV/vis absorbance between 230 nm and 600 nm increased or decreased. The behaviour of model compounds during reactions in alkaline media was compared to the UV/vis spectroscopic behaviour of DOM. The release of LMWOA was described by kinetic data and compared to the data of model reactions. Evidence was given for the carboxylic esters playing a significant role in the release of LMWOA only during the beginning of the alkaline degradation. The results gained by SEC with on‐line UV and DOC detection showed that the average size of DOM was decreasing, and that a major part of the degradation products consisted of low‐molecular‐weight mono‐ and dicarboxylic acids.  相似文献   

5.
Molecular evidence for life in the 3.5 billion year old Warrawoona chert   总被引:1,自引:1,他引:0  
The biological origin of organic matter in the oldest siliceous sediments (cherts) is still debated. To address this issue, the insoluble organic matter (kerogen) was isolated from a chert of the Warrawoona group. The chemical structure of the kerogen was investigated through a combination of analytical techniques including solid-state 13C nuclear magnetic resonance and pyrolysis. Although dominated by aromatic hydrocarbons, the pyrolysate comprises a homologous series of long chain aliphatic hydrocarbons characterized by odd-over-even carbon number predominance. This distribution is only consistent with a biological origin. As kerogen must be contemporaneous of the solidification of the chert, this observation should be regarded as an evidence for the presence of life on Earth, 3.5 By ago.  相似文献   

6.
Akiko  Omura  Koichi  Hoyanagi  Satoko  Ishikawa 《Island Arc》2006,15(3):355-365
Abstract   Both marine and terrigenous organic matter are deposited in shelf and continental slope environments. In the present study, the relationship between environmental changes in the Choshi area and the sedimentation of organic matter was examined. The sediments of the Choshi core were deposited on a shelf environment and their lithology and ichnofacies, as well as the composition of the contained kerogen (insoluble organic matter) indicate a shallowing upward succession. The organic matter preserved in the sediments is of both marine and terrigenous origin, on the basis of C/N ratios (5.90–9.45), δ13C values (−21.6‰−24.6‰) and kerogen microscopy. The total organic carbon (TOC) content (0.39–1.08%) of the sediments shows a positive correlation with the increase of terrigenous organic matter before 500 ka, but decreases (0.26–0.61%) after 500 ka as the shelf environment becomes shallower because of dilution, caused by the input of terrigenous inorganic clasts, and oxidation. The variation in TOC contents was thus influenced by the increasing sedimentation rate of terrigenous materials, including both organic and inorganic particles as the basin filled.  相似文献   

7.
《Continental Shelf Research》2008,28(18):2535-2549
Extensive physical and biological measurements were made of the surface sediments within the shallow, semi-urbanised Coombabah Lake in southern Moreton Bay, Australia. Sediment bulk parameters (C/N ratios, δ13C and δ15N) and fatty acid biomarkers were used to determine distributions and sources of organic matter in the intertidal sediments. The determination of organic matter sources within coastal and estuarine settings is important in understanding the roles of organic matter as energy and nutrient sources. Spatial variability of biomarker values within the sediments were interpreted by thematic maps employing the Krigging algorithm. Grain size analysis indicated the lake was dominated by mud (<63 μm) in the southern (landward) and sand (>63 μm) in the northern (seaward) lake regions, respectively. Surface sediment organic C and N values ranged from 0.12% to 1.76% and 0.01% to 0.12% dry weight, respectively, and C/N ratios averaged 16.3±3.19%. Sedimentary δ13C values ranged from −26.1‰ to −20.9‰, with an average value of −23.9±1.0‰. Sedimentary δ15N values ranged from +1.7‰ to +4.8‰, with an average value of +2.8±0.8‰. Bulk sediment parameters suggested that sedimentary organic matter is provided predominantly by allochthonous sources in the form of fringing mangroves. Thirty-nine individual fatty acids were identified using gas chromatography–mass spectrometry. The mean contributions of long chain fatty acids (LCFAs), polyunsaturated fatty acids (PUFAs), saturated fatty acids (SAFAs) and bacterial fatty acids (BAFAs) were, respectively, 13.9±11.4%, 7.6±4.1%, 53.6±8.6% and 18.2±4.6% of the identified fatty acid methyl esters (FAMEs), with BAFAs occurring in all sampled sediments. Fatty acid compositions varied throughout lake sediments, which indicated spatial differences in autochthonous and allochthonous organic matter sources, including terrestrial and planktonic (i.e. zooplankton, diatoms and other algal species) sources. The contribution of organic matter from shoreline mangroves was confirmed by the presence of LCFAs and 18:2ω6 and 18:3ω3, which are markers for mangroves in this ecosystem. BAFAs were identified in increased proportions in sediments adjacent to urban developments and dominated by mud. Grain size was identified as a dominant factor in the fatty acid compositions and contributing values to FAME pool. Spatial patterns of C/N ratios, δ13C and δ15N values, and fatty acid biomarker contributions illustrated that there is a greater contribution of autochthonous and labile organic matter to the sedimentary organic matter pool in the northern (marine entrance) sediments compared to the more allochthonous sourced organic matter of the southern region of the lake. This study details the distribution and sources of organic matter within Coombabah Lake and illustrates the usefulness of a multiple biomarker approach in discriminating organic matter sources within estuarine environments.  相似文献   

8.
Bacteria that degrade natural organic matter in groundwater contain oxygenase enzymes that can co‐oxidize trichloroethene (TCE). This degradation pathway is promising for large dilute plumes, but its evaluation is limited because the density of the bacteria with oxygenase enzymes has not been correlated to field scale rates of degradation. A 14C–TCE assay was developed to determine pseudo first‐order rate constants for the aerobic co‐oxidation of TCE in groundwater. The assay involved incubating 14C–TCE in samples of groundwater contained in 160 mL serum bottles, and monitoring the accumulation of radiolabel in degradation products. A first‐order rate constant for co‐oxidation was extracted from the rate of accumulation of 14C in products, accounting for volumetric changes in the serum bottles due to sampling and subsequent changes to the distribution of TCE between the aqueous and gaseous phases. Of the groundwater samples evaluated from 19 wells at five sites, eight samples at three sites had 14C product accumulation rates that exceeded the accumulation rate in filter‐sterilized groundwater controls. First‐order rate constants ranged from 2.65 to 0.0066 year?1, which is equivalent to half‐lives of 0.26 to 105 years. Groundwater samples from a few of the wells in which co‐oxidation occurred had volatile organic contaminants in addition to TCE; their presence may have induced the oxygenase enzymes that are needed for TCE co‐oxidation. 14CO2 represented ~37% to 97% of the 14C products that accumulated; the balance of the products was soluble and non‐volatile.  相似文献   

9.
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 (kdeg = 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.  相似文献   

10.
11.
Study of Late Cretaceous lacustrine sedimentary strata in the eastern Songliao Basin, China revealed that the paleoclimate was relatively arid and hot during sedimentation of the upper Santonian of the Yaojia Formation, but became relatively humid and warm during deposition of the lower Campanian Nenjiang Formation. The upper Yaojia Formation was deposited in a freshwater lake environment, while the lower Nenjiang Formation was deposited in a slightly brackish to brackish environment. The average total organic carbon content in the upper Yaojia Formation is 0.15%, while the hydrogen index is 36 mgHC/gTOC, implying poor source rock for oil generation and the organic matter comprised of a mixture of woody and herbaceous organic matter. In contrast, the hydrogen index of oil shale and black shale of the lower Nenjiang Formation is 619 mgHC/gTOC, and total organic carbon content on average is 3.37%, indicating a mixed algae and herbaceous source of kerogen and an increase in aquatic bioproductivity. The black shale and oil shale have low Pristane/Phytane and C29 5α,14α,17α(H) ? stigmastane 20R/(20R + 20S) ratios, with maximum concentration of n‐alkanes at n‐C23, implying an anoxic depositional environment with algae, bacteria and higher plants providing most of the organic matter. Relatively abundant gammacerane and a higher Sr/Ba ratio in the oil shales suggest the presence of brackish water and development of salinity stratification in the lake. During sedimentation of the upper Yaojia through the lower Nenjiang Formations, the level of Songliao lake increased and a deep‐lake environment was formed with bottom waters being oxygen depleted. Concomitantly, as the lake deepened bottom conditions were changing from oxic to anoxic, and the input of organic matter changed from predominantly higher plants to a mixture of bacteria, algae and higher plants providing favorable conditions for oil source rock accumulation.  相似文献   

12.
The oxidation of organic matter from wastewater using ozone, ultraviolet radiation and ozone/UV oxidation was evaluated in a pilot plant, applying a continuous effluent arising from the Autonomous Metropolitan University wastewater treatment plant. The oxidation was measured as the efficiency to remove organic load, measured as chemical oxygen demand. The use of ozone and UV was evaluated separately and in combination through a continuous process. Three different ozone doses (0.6–1.2 mg O3/L) and three different UV radiation fluencies (6.7–20.12 mJ/cm2) were assessed. A synergistic effect of the combined process ozone/UV was demonstrated, and a maximal chemical oxygen demand reduction was achieved both processes. Due to residence times used (less than 1 min), 36% of chemical oxygen demand reduction was obtained when ozone treatment was evaluate separately and only 9% using ultraviolet radiation.  相似文献   

13.
Organic and inorganic occurrence of selenium in Laerma Se-Au deposit   总被引:9,自引:0,他引:9  
Se and other trace elements in kerogen are determined. Based on biochemical evidence, theoretical calculations and infrared spectra, it is indicated that Se may occur as organic minerals by combining with organic legends. The inorganic occurrence of selenium is also discussed. Project supported by the National Natural Science Foundation of China (Grant No. 60633110).  相似文献   

14.
To quantify changes in organic carbon inputs and preservation, sediments from the Northern Chukchi Sea spanning the last 9000 years of the Holocene period were collected during the HOTRAX expedition and analyzed. The multi-proxy approach included molecular organic markers, bulk carbon and isotope measurements plus more recent approaches to terrestrial carbon estimation (the BIT index of Branched and Isoprenoid Tetraethers). The upper 1100 cm of the core, corresponding to the last 7.4 ka, showed a relatively stable total organic carbon content of 1.13-1.38% which decreased below 1100 cm to 0.6%. C:N ratios ranged from 8.4 to 10.83 over the Holocene time period examined. The distribution of n-alcohols and n-alkanes revealed major contributions from long-chain n-alcohols and n-alkanes while minimal contributions were seen from short-chain n-alkanes. The majority of the total fatty acids was comprised of saturated and monounsaturated fatty acids with short-chain and long-chain saturated fatty acids present in similar concentrations throughout most of the core and monounsaturated fatty acids decreasing down-core. Total sterol concentrations showed considerable inputs from marine sterols, C28Δ5,22, C28Δ5,24(28) and dinosterol, as well as C29Δ5, typically considered a terrestrial marker. The BIT indices for core sediments ranged from 0.021 to 0.216 with minor changes seen in older sequences. Overall, organic biomarkers indicate marine sources as the more dominant input of organic matter with lower but continual contributions from terrestrial sources at this location during the Holocene. The remarkable consistency among multiple molecular organic markers of both marine and terrestrial origin over the Holocene period encompassed by the core suggests that sinking material or surface sediments were heavily influenced by bottom currents or other mixing processes prior to their deposition.  相似文献   

15.
Photooxidation degradation of Reactive Brilliant Red K‐2BP (K‐2BP) aqueous solution by ultraviolet irradiation/sodium hypochlorite (UV/NaClO) was investigated. The effects of NaClO dosage, pH, temperature and initial dye concentrations were studied. A possible degradation pathway of K‐2BP was investigated. Acidic or neutral conditions were beneficial to the decolorization of K‐2BP aqueous solution. However, alkaline conditions facilitated chemical oxygen demand (COD) removal. Increasing the solution temperature from 20 to 50°C increased the removal of color and COD. However, at 60°C, the final percentage color and COD removal decreased by approximately 17 and 10%, respectively. Based on the products indentified and theoretical analysis, N=N cleavage and C‐N cleavage were possible initial steps in the degradation of K‐2BP. From the results of this work, we conclude that treatment of UV/NaClO is an efficient method to degrade K‐2BP in aqueous solution.  相似文献   

16.
古小治  姜维华 《湖泊科学》2018,30(6):1518-1524
借助微氧电极测试技术对太湖贡湖湾试验区疏浚后的新生界面溶解氧动态进行一年的跟踪调研,分析溶解氧在新生微米级界面的分布特征、扩散通量以及界面附近有机质矿化速率.结果表明疏浚后半年内,溶解氧在表层沉积物的侵蚀深度增大,氧化层明显加厚.氧气在新生界面表层沉积物中呈指数下降,但衰减相对较缓.在连续一年的跟踪调查中发现,仅秋季新生界面附近溶解氧浓度明显高于对照,而在其他月份无差异.污染底泥疏浚后一个月内氧扩散通量及有机碳矿化速率下降最为明显,仅为疏浚前的13%,其他月份沉积物-水界面氧的扩散通量、氧气的消耗速率、有机碳的降解速率均有不同程度下降,疏浚后新生界面氧气交换速率下降以及由此导致的有机碳矿化过程变缓可能深刻影响界面生源要素的迁移过程.  相似文献   

17.
Ken  Sawada 《Island Arc》2006,15(4):517-536
Abstract Organic petrological observations of kerogen macerals and organic geochemical analyses of carbon isotopes of kerogen macerals and biomarkers were conducted on Neogene neritic sediments of the Takafu syncline area of central Japan. The Senmi, Sakainomiya and Lower Shigarami Formations in that area were deposited at the neritic provinces on the southern edge of the paleo‐Japan Sea during the Late Miocene to Early Pliocene. Sedimentary organic matter in these formations was almost terrigenous in origin. Changes in kerogen maceral compositions reflect sedimentological and tectonic histories evaluated in previous studies from sedimentary facies and paleontology. It was found that carbon isotope ratios (δ13C) of kerogen macerals increased from ?28‰ to ?25‰ from the Sakainomiya to the lower part of the Lower Shigarami Formations. The cause of that increase was presumably the expansion of C4 plants into southwest Japan. The timing was concordant with that of the expansion of C4 plant grasslands in East Asia. The oxicity (oxic to anoxic) conditions of sea bottoms evaluated from pristane/phytane ratios varied. Particularly, in the lower part of the Senmi Formation, layers in which no steroid biomarkers could be detected were found, and had presumably formed under oxic conditions when strong biodegradation had occurred. Concentrations of regular (C27–C29) steranes and dinosteranes were higher in the Sakainomiya and Lower Shigarami Formations. This indicates that dinoflagellates‐dominant primary productions were higher at those stages. In addition, concentrations of diatomaceous biomarkers such as C26 norsterane increased from the Lower Shigarami Formation, thus adding diatoms to the major producers. Furthermore, similar associations between the increases of δ13C values of kerogen macerals and concentrations of diatomaceous biomarkers were observed in the Takafu syncline area. Thus, the expansion of C4 plants was possibly associated with the high production of diatom in the shallow‐marine areas of the paleo‐Japan Sea during the Neogene Period.  相似文献   

18.

Devonian strata in the Guizhong region, Guangxi, China consist mainly of marine deposition carbonates (limestones and dolomites) as well as restricted clastic rocks. The strata thickness is measured as 2041m and classified into 14 formations. An integrated field geological, petrographic, sedimentological, palaeobiological, and geochemical study of these strata reveals that the depositional paleoenvironments were carbonate tidal flat, restricted platform, open platform, shelf, platform margin slop, and algal herm. The total organic carbon (TOC) of sedimentary organic matter ranges between 0.07% and 1.96% with average of 0.21%. The organic matter types are Type I and Type III. The vitrinite reflectance (R 0) of kerogen ranges between 0.99% and 2.03%, indicating the maturated and highly maturated stages. The analytical results of the representative samples collected from shelf and subtidal facies show that the differences of organic matter type and biological diagnostic compounds are related to the types of source rocks deposited in different paleoenvironments.

  相似文献   

19.
The diagenetic mechanism and process of carbonate rocks, which is different to that of clastic rocks, decides the existence of different existing state organic matters in carbonate rocks. This has been verified by both the microscopic observation of organic petrology and the analysis of organic geochemistry of many samples. Based on the hydrous pyrolysis simulation experiment of the low-mature carbonate rocks, the contrasting study on the yield and their geochemistry characteristics of different existing state soluble organic matters of a series of various maturity samples shows that the different existing state organic matters make different contributions to hydrocarbon generation during every evolution state. So that, the hydrocarbon generation process of carbonate rocks can be summarized as the following three stages: the first is the direct degradation of biogenic bitumen macromolecules during the immature stage, the second is the thermal degradation of a large amount of kerogen at the mature stage, the last stage is the expulsion or release of inclusion organic matter owing to the increased thermal expansion pressure during the high evolution stage. Part of achievements of the Eighth Five-Year National Science-Technology Key-Task Project “85-102-02-07”.  相似文献   

20.
By measuring carbon and hydrogen isotope compositions for C1, C2 and C3 of 74 gas samples, natural gases from the Tarim Basin can be divided into six groups on the basis of their origins: (1) coal-type gas derived from coal measures; (2) coal-type gas generated from the T-J lacustrine mudstones; (3) oil-type gas derived from the Cambrian and low Ordovician marine source rocks; (4) oil-type gas from the source rocks deposited in the marine-transitional facies; (5) mixing gas between gas derived from the Carboniferous transitional source rocks and the Mesozoic humic gas, and (6) mixing gases of thermal genetic gas and little deep gas in the Southwest depression of the Tarim Basin. The δ D values of methane in natural gases originating from different type kerogens are affected by both palaeo-environments of the source rock formation (kerogen types) and thermal maturity, with sedimentary environment (kerogen type) as the main controlling factor. Under the similar thermal maturity, the hydrogen isotope composition of methane is more enriched in deuterium in marine environments than lacustrine one. With the increase of thermal maturity and the increase of carbon atomic numbers of gaseous alkanes, the hydrogen isotopes become enriched in deuterium. The δ D values of ethane and propane (δ D2, δ D3) are controlled mainly by thermal maturity and to a lesser degree by sedimentary environment of the source rock formation. The partial reversal of hydrogen isotopes for gaseous alkanes would be related to the microbial oxidation, mixing of sapropelic and humic gases and / or mixing of gases from similar kerogen sources with various thermal maturities. In the oil-type gas, the sulfate reduction reaction would result in the reversed order of δ D1 and δ D2 (e.g. δ D1>δ D2).  相似文献   

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