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1.
This work reports the historical trends and sources of aliphatic hydrocarbons (AHs) and polycyclic aromatic hydrocarbons (PAHs) in two 210Pb dated sediment cores extracted from the central mud areas of Bohai Sea (Bohai). The TOC/TN ratio of the bulk organic matter (OM) and the composition of the n-alkanes suggest that the sedimentary organic matter was of mixed marine and terrigenous sources. The coarser sediment grain size and decreasing C/N ratios since ∼1976 could be attributed to the relocation of the Yellow River mouth causing a decreased influence of Yellow River derived sediments and associated OM into the central Bohai. The concentration of total 16 PAHs in the two cores ranged from 34.2-202 ng/g (mean, 91.5) for BC1, and from 53.3-186 ng/g (mean, 103) for BC2, with a high abundance of 2-3 ring PAHs. Perylene in the two cores mainly originated from terrigenous sources via riverine discharge and thus could be potentially related to changes in the sediment load from the Yellow River into the Bohai over time. Petroleum inputs could be revealed by ratios of methylphenanthrenes to phenanthrene (MP/P) and the patterns of more stable geochemical biomarkers (hopanes and steranes) along the two cores, in addition to the presence of unresolved complex mixtures (UCM) in the surface layers. Source diagnostic ratios of PAHs indicated a pyrogenic origin from biomass and coal combustion with a minor petroleum contribution. Downcore trends of compositional PAHs profiles were in agreement with the socio-economic development in China in the past decades. This temporal variation of sedimentary PAHs can also reflect a different evolution stage of energy structure in China as compared with those of the western developed countries.  相似文献   

2.
The presence of PAHs, n-alkanes, pristane, and phytanes in core sediment from the Vossoroca reservoir (Parana, southern Brazil) was investigated. The total concentration of the 16 PAHs varied from 15.5 to 1646 μg kg−1. Naphthalene was present in all layers (3.34–74.0 μg kg−1). The most abundant and dominant n-alkanes were n-C15 and n-C36, with average concentrations of 198.1 ± 46.8 and 522.9 ± 167.7 μg kg−1, respectively. Lighter n-alkanes were distributed more evenly through the layers and showed less variation, specially n-C9, n-C12, and n-C18, with average concentrations of 14.6 ± 3.0, 31.6 ± 1.9, and 95.0 ± 5.2 μg kg−1, respectively; heavier n-alkanes were more unevenly distributed.  相似文献   

3.
The burial characteristics and toxicity risks associated with n-alkanes and polycyclic aromatic hydrocarbons (PAHs) in the riverine and estuarine sediments of the Daliao River watershed were investigated based on three sediment cores. The sum of the n-alkane and PAH concentrations, normalized to organic carbon (OC), ranged from 0.27 to 63.09 μg g?1OC?1 and 6.60 to 366.20 μg g?1OC?1, respectively. The features and the history of industrial activities, such as the oil and chemical industries and port activities near the river and estuary, resulted in different distributions and sources of hydrocarbons. The sources of pollution were identified based on n-alkane indexes and on diagnostic ratios of PAHs. The diagnostic ratios indicated that the n-alkanes were derived from both biogenic and petrogenic sources in different proportions and that the PAHs were derived primarily from petrogenic combustion sources. A hierarchical cluster analysis grouped the core samples into two clusters. The first cluster, river sediments, corresponded to industrial activities; the second cluster, estuarine sediments, corresponded to port shipping activities. The toxic potency of the PAHs in the cores was assessed in terms of toxic equivalents (TEQs) of dibenzo[a,h]anthracene and benzo[a]pyrene. The top layer of the sediment in the cores had a relatively high toxicity. The TEQ values for benzo(a)pyrene (TEQBaP) and dioxins (TEQTCDD) furnished a consistent assessment of the PAHs in the sediment cores.  相似文献   

4.
Transfer of organic carbon (OC) from the terrestrial to the oceanic carbon pool is largely driven by riverine and aeolian transport. Before transport, however, terrigenous organic matter can be retained in intermediate terrestrial reservoirs such as soils. Using compound-specific radiocarbon analysis of terrigenous biomarkers their average terrestrial residence time can be evaluated.Here we show compound-specific radiocarbon (14C) ages of terrigenous biomarkers and bulk 14C ages accompanied by geochemical proxy data from core top samples collected along transects in front of several river mouths in the Black Sea. 14C ages of long chain n-alkanes, long chain n-fatty acids and total organic carbon (TOC) are highest in front of the river mouths, correlating well with BIT (branched and isoprenoid tetraether) indices, which indicates contribution of pre-aged, soil-derived terrigenous organic matter. The radiocarbon ages decrease further offshore towards locations where organic matter is dominated by marine production and aeolian input potentially contributes terrigenous organic matter. Average terrestrial residence times of vascular plant biomarkers deduced from n-C29+31 alkanes and n-C28+30 fatty acids ages from stations directly in front of the river mouths range from 900 ± 70 years to 4400 ± 170 years. These average residence times correlate with size and topography in climatically similar catchments, whereas the climatic regime appears to control continental carbon turnover times in morphologically similar drainage areas of the Black Sea catchment. Along-transect data imply petrogenic contribution of n-C29+31 alkanes and input via different terrigenous biomarker transport modes, i.e., riverine and aeolian, resulting in aged biomarkers at offshore core locations. Because n-C29+31 alkanes show contributions from petrogenic sources, n-C28+30 fatty acids likely provide better estimates of average terrestrial residence times of vascular plant biomarkers. Moreover, sedimentary n-C28 and n-C30 fatty acids appear clearly much less influenced by autochthonous sources than n-C24 and n-C26 fatty acids as indicated by increasing radiocarbon ages with increasing chain-length and are, thus, more representative as vascular plant biomarkers.  相似文献   

5.
Surface sediments from the subtropical Pearl River estuary and adjacent South China Sea were investigated by molecular organic geochemical methods to determine the composition, distribution and origin of extractable lipids (n-alkanes, n-alkanols and sterols). The absolute and organic C normalized concentrations of total alkane, n-alkanol, and sterol ranged from 0.16 to 2.67 μg g−1 and 0.9 to 12.3 μg g−1 OC, 24.4 to 427.3 ng g−1 and 63.2 to 1966.7 ng g−1 OC, and 9.0 to 493.5 ng g−1 and 58.4 to 1042.4 ng g−1 OC, respectively. The spatial distributions of these biomarkers indicated that terrestrial-derived molecular biomarkers such as long-chain n-alkanes, n-alkanols and plant-derived sterols were higher at the river mouth and along the coastline, suggesting that a higher proportion of terrestrial particulate organic matter was deposited there. Relatively lower amounts of marine-derived biomarkers such as short-chain n-alkanes, algal sterols at the river mouth reflected the lower primary productivity due to high turbidity. The spatial patterns of these biomarkers were partially related to the estuarine processes and conditions, evidencing an increased terrestrial signal from the Pearl River mouth to the inner estuary, and enhanced marine conditions further offshore.  相似文献   

6.
The surface reactivity of biogenic, nanoparticulate UO2 with respect to sorption of aqueous Zn(II) and particle annealing is different from that of bulk uraninite because of the presence of surface-associated organic matter on the biogenic UO2. Synthesis of biogenic UO2 was accomplished by reduction of aqueous uranyl ions, by Shewanella putrefaciens CN32, and the resulting nanoparticles were washed using one of two protocols: (1) to remove surface-associated organic matter and soluble uranyl species (NAUO2), or (2) to remove only soluble uranyl species (BIUO2). A suite of bulk and surface characterization techniques was used to examine bulk and biogenic, nanoparticulate UO2 as a function of particle size and surface-associated organic matter. The N2-BET surface areas of the two biogenic UO2 samples following the washing procedures are 128.63 m2 g−1 (NAUO2) and 92.56 m2 g−1 (BIUO2), and the average particle sizes range from 5-10 nm based on TEM imaging. Electrophoretic mobility measurements indicate that the surface charge behavior of biogenic, nanoparticulate UO2 (both NAUO2 and BIUO2) over the pH range 3-9 is the same as that of bulk. The U LIII-edge EXAFS spectra for biogenic UO2 (both NAUO2 and BIUO2) were best fit with half the number of second-shell uranium neighbors compared to bulk uraninite, and no oxygen neighbors were detected beyond the first shell around U(IV) in the biogenic UO2. At pH 7, sorption of Zn(II) onto both bulk uraninite and biogenic, nanoparticulate UO2 is independent of electrolyte concentration, suggesting that Zn(II) sorption complexes are dominantly inner-sphere. The maximum surface area-normalized Zn(II) sorption loadings for the three substrates were 3.00 ± 0.20 μmol m−2 UO2 (bulk uraninite), 2.34 ± 0.12 μmol m−2 UO2 (NAUO2), and 2.57 ± 0.10 μmol m−2 UO2 (BIUO2). Fits of Zn K-edge EXAFS spectra for biogenic, nanoparticulate UO2 indicate that Zn(II) sorption is dependent on the washing protocol. Zn-U pair correlations were observed at 2.8 ± 0.1 Å for NAUO2 and bulk uraninite; however, they were not observed for sample BIUO2. The derived Zn-U distance, coupled with an average Zn-O distance of 2.09 ± 0.02 Å, indicates that Zn(O,OH)6 sorbs as bidentate, edge-sharing complexes to UO8 polyhedra at the surface of NAUO2 nanoparticles and bulk uraninite, which is consistent with a Pauling bond-valence analysis. The absence of Zn-U pair correlations in sample BIUO2 suggests that Zn(II) binds preferentially to the organic matter coating rather than the UO2 surface. Surface-associated organic matter on the biogenic UO2 particles also inhibited particle annealing at 90 °C under anaerobic conditions. These results suggest that surface-associated organic matter decreases the reactivity of biogenic, nanoparticulate UO2 surfaces relative to aqueous Zn(II) and possibly other environmental contaminants.  相似文献   

7.
Bulk geochemical characterization (total organic carbon, grain size distribution, carbon isotope composition) and molecular biomarkers (lignin phenols, straight chain aliphatic hydrocarbons, glycerol dialkyl glycerol tetraethers) were analyzed for a 21 m core from the Bohai Sea (North China), spanning ca 21 ka BP. These paleo-proxies presented remarkable differences between the late glacial period and the Holocene, reflecting continental and coastal environments, respectively. Two peat layers were deposited during the period of ca 9000-8460 yr BP. Thereafter the core site has been consistently covered by seawater until recent reclamation of land from the sea. The occurrence of a total organic carbon maximum from ca 6000-3800 yr BP was attributed to delivery of organic carbon enriched sediments via the Yellow River, consistent with increased vegetation density and higher development of soil under warm and humid mid-Holocene climate conditions. The distributions of lignin phenol compositions and C31/C29n-alkane ratio suggested the largest expansion of woody plants between ca 5300 and 4000 yr BP, corresponding to the extremely favorable climatic conditions. Since ca 3800 yr BP, an abrupt increase in the C31/C29n-alkane ratio suggested higher abundance of grasses, consistent with a drying climate trend after the mid-Holocene. Since our coastal sediments close to the Yellow River outflow contain catchment-integrated environmental signals of the river basin, molecular proxies demonstrate that the variability of vegetation distributions in the Holocene is a widespread phenomenon in those areas adjacent to Yellow River Basin.  相似文献   

8.
Two piston cores, one located far from the continents (The North Pacific Ocean: ES core), and another located comparatively closer to the continents (The Bering Sea: BOW-8a core) were investigated to reconstruct environmental changes on source land areas. The results show significant contribution of terrestrial organic matter to sediments in both cores. The δ13C values of n-C27, n-C29, and n-C31 alkanes in sediments from the North Pacific ES core show significant glacial to interglacial variation whereas those from the Bering Sea core do not. Variations of δ13C values of land plant n-alkanes are related to the environmental or vegetational changes in the source land areas. Environmental changes, especially, aridity, rainfall, and pCO2 during glacial/interglacial transitional periods can affect vegetation, and therefore C3 / C4 plant ratios, resulting in δ13C changes in the preserved land plant biomarkers. Maximum values of δ13C as well as maximum average chain length values of long chain n-alkanes in the ES core occur mostly at the interglacial to glacial transition zones reflecting a time lag related to incorporation of living organic matter into soil and transportation into ocean basins via wind and/or ability of C4 plants to adapt for a longer period before being replaced by C3 plants when subjected to gradual climatic changes. Irregular variations with no clear glacial to interglacial trends in the BOW-8a core may result from complex mixture of aerosols from westerly winds and riverine organic matter from the Bering Sea catchments. In addition, terrestrial organic matter entering the Bering Sea could originate from multiple pathways including eolian, riverine, and ice rafted debris, and possibly be disturbed by turbidity and other local currents which can induce re-suspension and re-sedimentation causing an obliterated time relation in the Bering Sea biomarker records.  相似文献   

9.
Attention has been paid for the levels, sources and health risks of atmospheric aliphatic and polycyclic aromatic hydrocarbons (n-alkanes and PAHs) in remote areas, however, few studies have focused on those in the Tibetan Plateau. In this study, 18 pairs of atmospheric samples were obtained during the period from August 2006 to July 2007 in Lhasa, the capital city of Tibet. Both gas-phase and particulate-phase n-alkanes and PAHs were measured. Concentrations of n-alkanes (gas + particulate phase, 99.1–480.9 ng/m3) and PAHs (gas + particulate phase, 11.4–72.5 ng/m3) in Lhasa are lower than those in many cities. The sources of n-alkanes related to biological and petroleum sources were 67 and 33%, respectively. According to the results of diagnostic ratios and principal component analysis, emission of traffic vehicles was one of the important PAH sources, and sources of benzo(a)pyrene was likely attributed to incense burning. Good simulations were obtained by traffic soot-based model for fluoranthene, pyrene and benzo(a)anthracene, while, wood soot-based model fitted the experimental results of benzo(a)pyrene better. This meant atmospheric fate of PAHs was mainly influenced by the adsorptive partitioning that occurred during traffic and incense burning procedures. In addition, the benzo[a]pyrene-equivalent carcinogenic power (BaPE) in the present study (0.1–1.6 ng/m3) is lower than those in other cities and also the air quality standard of China, suggesting that atmospheric PAHs caused low health risks.  相似文献   

10.
《Applied Geochemistry》2002,17(11):1467-1494
Samples from the Ocean Drilling Program Leg 169 in Escanaba Trough, Gorda Ridge, NE Pacific Ocean, were analyzed to study maturation by accelerated diagenesis and/or by catagenesis of the sedimentary organic matter to hydrothermal petroleum. At Site 1038 the hydrothermal petroleums have migrated after generation to shallower horizons. The n-alkane maturation was indicated by the strong even C number preference (i.e., CPI <1.0) as in the case of Middle Valley. All samples contained admixed organic matter of terrigenous and marine components as indicated by the distributions of the biomarkers. The biological precursors were catagenetically altered to their equivalent mature compounds. The presence of high molecular weight PAHs in some sediment sections at Site 1038 reflected the high temperature alteration and reworking of organic matter into mature hydrothermal petroleum. At Site 1037, the reference hole in the Escanaba Trough, the n-alkanes with a strong predominance of odd C number homologs reflected immature non-marine lipid components essentially throughout the hole. Maturation of organic matter was only observed below 450 mbsf with n-alkanes showing a CPI <1.0. The strong even C number predominance in those intervals was attributed to initial maturation by high heat flow during the early rifting process.  相似文献   

11.
Dissolved and particulate hydrocarbons of biogenic origin were investigated for the first time in surface waters along the Seine River and its estuary. They comprise n-alkanes (n-ALKs) and diagenetic polycyclic aromatic hydrocarbons (PAHs). Samples were collected in three different sections of the estuary: the riverine zone, the mixing zone, and the marine zone. At the river mouth, two mooring stations were used for the collection of samples over tidal cycles. Total particulate n-ALK concentrations ranged from 31 ng 1?1 to 2,918 ng 1?1, or 5 μg g?1 dry ng 1?1, or 2 μg g?1 of SM. Concentrations varied with the SM load and could be related to sedimentation and estuarine mixing. The sources of the n-ALKs were different in each zone of the estuary. The dissolved n-ALKs displayed lower concentrations than the particulate phase, varying from 136 ng 1?1 to 344 ng 1?1, while biogenic dissolved PAHs were almost absent.  相似文献   

12.
This paper reports on the spatial distribution patterns and investigates the controlling mechanisms of phytoplankton biomarkers (brassicasterol for diatoms, alkenones for haptophytes, dinosterol for dinoflagellates) and terrestrial biomarkers (odd C number long-chain (C27 + C29 + C31) n-alkanes) in surface sediments from the southern Yellow Sea (SYS). The contents of the phytoplankton biomarkers in the SYS surface sediments reveals a clear spatial pattern, with low values near the coasts and increased values seaward, caused by higher phytoplankton primary productivity and low sedimentation rates in the basin. The contents of terrestrial biomarkers show high values in the northern part of the study areas off the Shandong Peninsula and Jiangsu coast, caused by inputs of materials from the modern Huanghe River and the old Huanghe delta, respectively. The results also indicate that biomarker ratios offer the best approach for reconstructing marginal sea C cycles, as these proxies can be used to estimate the contributions of both terrestrial and marine organic matter and to reconstruct paleoproductivity and paleoecological changes in the SYS.  相似文献   

13.
We measured molecular distributions and compound-specific hydrogen (δD) and stable carbon isotopic ratios (δ13C) of mid- and long-chain n-alkanes in forest soils, wetland peats and lake sediments within the Dorokawa watershed, Hokkaido, Japan, to better understand sources and processes associate with delivery of terrestrial organic matter into the lake sediments. δ13C values of odd carbon numbered C23-C33n-alkanes ranged from −37.2‰ to −31.5‰, while δD values of these alkanes showed a large degree of variability that ranged from −244‰ to −180‰. Molecular distributions in combination with stable carbon isotopic compositions indicate a large contribution of C3 trees as the main source of n-alkanes in forested soils whereas n-alkanes in wetland soil are exclusively derived from marsh grass and/or moss. We found that the n-alkane δD values are much higher in forest soils than wetland peat. The higher δD values in forest samples could be explained by the enrichment of deuterium in leaf and soil waters due to increased evapotranspiration in the forest or differences in physiology of source plants between wetland and forest. A δ13C vs. δD diagram of n-alkanes among forest, wetland and lake samples showed that C25-C31n-alkanes deposited in lake sediments are mainly derived from tree leaves due to the preferential transport of the forest soil organic matter over the wetland or an increased contribution of atmospheric input of tree leaf wax in the offshore sites. This study demonstrates that compound-specific δD analysis provides a useful approach for better understanding source and transport of terrestrial biomarkers in a C3 plant-dominated catchment.  相似文献   

14.
Due to the widespread contamination of groundwater resources with arsenic (As), controls on As mobility have to be identified. In this study we focused on the distribution of As in the dissolved, colloidal and particulate size fraction of experimental solutions rich in ferric iron, dissolved organic matter (DOM) and As(V). Size fractions between <5 kDa and >0.2 μm were separated by filtration and their elemental composition was analyzed. A steady-state particle size distribution with stable element concentration in the different size classes was attained within 24 h. The presence of DOM partly inhibited the formation of large Fe-(oxy)hydroxide aggregates, thus stabilized Fe in complexed and colloidal form, when initially adjusted molar Fe/C ratios in solution were <0.1. Dissolved As concentrations and the quantity of As bound to colloids (<0.2 μm) increased in the presence of DOM as well. At intermediate Fe/C ratios of 0.02-0.1, a strong correlation between As and Fe concentration occurred in all size fractions (R2 = 0.989). At Fe/C ratios <0.02, As was mainly present in the dissolved size fraction. These observations indicate that As mobility increased in the presence of DOM due to (I) competition between As and organic molecules for sorption sites on Fe particles; and (II) due to a higher amount of As bound to more abundant Fe colloids or complexes <0.2 μm in size. The amount of As contained in the colloidal size fractions also depended strongly on the initial size of the humic substance, which was larger for purified humic acids than for natural river or soil porewater samples. Arsenic in the particle size fraction >0.2 μm additionally decreased in the order of pH 4 ? 6 > 8. The presence of DOM likely increases the mobility of As in iron rich waters undergoing oxidation, a finding that has to be considered in the investigation of organic-rich terrestrial and aquatic environments.  相似文献   

15.
Lake Kivu is a gas-charged East African rift lake with currently anoxic bottom water. The extractable compounds and residual organic matter of a short sediment core have δ13C values typical of lacustrine microbial detritus. The total extracts consist primarily of polar compounds such as n-alkanoic acids, hydroxyalkanoic acids, triterpenoids, steroids and monosaccharides, with minor amounts of n-alkanes and n-alkanols. These tracer compounds and δ13C values indicate that the organic matter in the surficial and deeper sedimentary record was dominated by bacterial sources. The sapropelic sediment between these horizons contains organic matter from primarily algal with lesser bacterial input. Terrestrial organic markers are minor in all samples. The major fractions of the compounds in the total extracts were oxidized in the upper water column prior to transit through the anoxic bottom water to sedimentary deposition. The sapropelic horizon may reflect lake water turnover with ventilation or hydrothermal activity and consequently increased algal blooms.  相似文献   

16.
This work was carried out in order to study the impact of car body repair activities in Bouzaréah City (suburban area located at the plateau of Algiers) on the air quality. Atmospheric particulate matter was targeted using high-volume sampler. Precisely, the particulate organic matter such as organophosphate esters, especially triphenyl phosphate and tributyl phosphate, was evaluated by the implementation of accelerated solvent extraction. The results of the major extractable organic components revealed that tributyl phosphate and triphenyl phosphate were found at 5.46 and 1.78 ng m?3, respectively. On the other hand, the classical pollutants such as n-alkanes, n-alkanoic monocarboxylic acids and polycyclic aromatic hydrocarbons were also measured, respectively, at average total concentrations of 35.8, 107.4 and 9.8 ng m?3. This work confirms that sanding and painting car bodies may contribute to air pollution, especially after detection of diethylnitrosamine which remains the most surprising compound in the particulate matter due to its volatility and can be considered as emerging contaminant.  相似文献   

17.
Biofilm-embedded Mn oxides exert important controls on trace metal cycling in aquatic and soil environments. The speciation and mobility of Zn in particular has been linked to Mn oxides found in streams, wetlands, soils, and aquifers. We investigated the mechanisms of Zn sorption to a biogenic Mn oxide within a biofilm produced by model soil and freshwater MnII-oxidizing bacteria Pseudomonas putida. The biogenic Mn oxide is a c-disordered birnessite with hexagonal layer symmetry. Zinc adsorption isotherm and Zn and Mn K-edge extended X-ray absorption fine structure (EXAFS) spectroscopy experiments were conducted at pH 6.9 to characterize Zn sorption to this biogenic Mn oxide, and to determine whether the bioorganic components of the biofilm affect metal sorption properties. The EXAFS data were analyzed by spectral fitting, principal component analysis, and linear least-squares fitting with reference spectra. Zinc speciation was found to change as Zn loading to the biosorbent [bacterial cells, extracellular polymeric substances (EPS), and biogenic Mn oxide] increased. At low Zn loading (0.13 ± 0.04 mol Zn kg−1 biosorbent), Zn was sorbed to crystallographically well-defined sites on the biogenic oxide layers in tetrahedral coordination to structural O atoms. The fit to the EXAFS spectrum was consistent with Zn sorption above and below the MnIV vacancy sites of the oxide layers. As Zn loading increased to 0.72 ± 0.04 mol Zn kg−1 biosorbent, Zn was also detected in octahedral coordination to these sites. Overall, our results indicate that the biofilm did not intervene in Zn sorption by the Mn-oxide because sorption to the organic material was observed only after all Mn vacancy sites were capped by Zn. The organic functional groups present in the biofilm contributed significantly to Zn removal from solution when Zn concentrations exceeded the sorption capacity of the biooxide. At the highest Zn loading studied, 1.50 ± 0.36 mol Zn kg−1 biosorbent, the proportion of total Zn sorption attributed to bioorganic material was 38 mol%. The maximum Zn loading to the biogenic oxide that we observed was 4.1 mol Zn kg−1 biogenic Mn oxide, corresponding to 0.37 ± 0.02 mol Zn mol−1 Mn. This loading is in excellent agreement with previous estimates of the content of cation vacancies in the biogenic oxide. The results of this study improve our knowledge of Zn speciation in natural systems and are consistent with those of Zn speciation in mineral soil fractions and ferromanganese nodules where the Mn oxides present are possibly biogenic.  相似文献   

18.
Stable carbon (δ13C) and hydrogen (δD) isotopic compositions of n-alkanes, anteiso-alkanes, n-alkanoic acids, n-alkanols, phytol and sterols in raw leaves of Acer argutum and Acer carpinifolium, their fallen leaves, mold and soils from a natural Acer forest were measured in order to: (1) understand isotopic variation of the plant biomarkers in a plant-soil system and (2) evaluate which biomarker is the most effective recorder of soil vegetation. Long-chain (> C24) n-alkanes, n-alkanoic acids and n-alkanols are gradually enriched in 13C up to 12.9‰ (average of 4.3‰) and depleted in D up to 94‰ (average of 55‰) from raw leaves to soils. However, anteiso-alkanes, phytol and sterols show little variation in both δ13C (< ± 1‰) and δD (< ± 2‰) from raw leaves to soils. These isotope signatures in a plant-soil system indicate that isoprenoid plant biomarkers such as sterols in soils faithfully preserve the isotopic compositions of dominant higher plants growing on the soils without a diagenetic effect upon the isotopic compositions. In contrast, long-chain n-alkyl molecules in soils undergo specific isotopic modification during biodegradation associated with early diagenesis and/or a significant contribution from heterotrophic reworking.  相似文献   

19.
The molecular sources, dynamics and analytical characterizations of the phosphorus (P) containing components of marine dissolved and particulate organic matter (OM) are reviewed. Using a combination of 13C and 31P nuclear magnetic resonance spectroscopy on samples collected from a depth profile (20-4000 m) at Station Aloha in the North Pacific subtropical gyre, the biomolecular associations of P functional groups in marine OM are identified. Compositional differences between ultrafiltered dissolved organic matter (UDOM; 1-100 nm size fraction) and ultrafiltered particulate organic matter (UPOM; 0.1-60 μm size fraction) as reflected by NMR and elemental analyses indicate that UDOM does not originate from simple solubilization of UPOM, and the aggregation of UDOM is not the primary source of UPOM. Regression analyses indicated a large fraction of the P in UDOM is associated with carbohydrates and amino acids, but not with lipids. Similar analyses for UPOM indicated that P is associated with carbohydrates, amino acids and lipids. The P functional groups also appear to be balanced in their distribution among molecular classes, because they remain in relatively constant proportion throughout the ocean.  相似文献   

20.
《Applied Geochemistry》2006,21(6):919-940
Smoke particulate matter from grasses (Gramineae, temperate, tropical and arctic) subjected to controlled burning, both under smoldering and flaming conditions, was sampled by high volume air filtration on pre-cleaned quartz fiber filters. The filtered particles were extracted with dichloromethane/methanol and the crude extracts were methylated for separation by thin layer chromatography into hydrocarbon, carbonyl, carboxylic acid ester and polar fractions. Then, the total extract and individual fractions were analyzed by GC–MS. The major organic components directly emitted in grass smoke particles were the homologous series of n-alkanoic acids from plant lipids, n-alkanes from epicuticular wax, and sterols and triterpenols. The major natural products altered by combustion included pyrolysis products from cellulose and lignin biopolymers, and oxidation products from triterpenoids and sterols. Polycyclic aromatic hydrocarbons (PAH) were also present; however, only as minor components. Although the concentrations of organic compounds in smoke aerosols are highly variable and dependent on combustion temperature, the biomarkers and their combustion alteration products are in these cases source specific. The major components are adsorbed on or trapped in smoke particulate matter and thus may be utilized as molecular tracers in the atmosphere for determining fuel type and source contributions from grass burning.  相似文献   

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