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1.
Lipid biomarkers from a peat plateau profile from the Northeast European Russian Arctic were analyzed. The peat originated as a wet fen ca. 9 ka BP and developed into a peat bog after the onset of permafrost ca. 2.5 ka BP. The distributions and abundances of n-alkanols, n-alkanoic acids, n-alkanes, n-alkan-2-ones and sterols were determined to study the effect of degradation on their paleoclimate proxy information. Plant macrofossil analysis was also used in combination with the lipid distributions. The n-alkanol and n-alkanoic acid distributions in the upper part of the sequence generally correspond to compositions expected from plant macrofossil assemblages. Their carbon preference index (CPI) values increase with depth and age, whereas those of the n-alkanes decrease. The different CPI patterns suggest that n-alkanoic acids and n-alkanols deeper in the sequence may be produced during humification through alteration of other lipids. Excursions in the n-alkanoic acid content also suggest an important contribution of invasive roots to the lipid biomarker composition. The CPIs associated with these compounds show that under permafrost conditions organic material from Sphagnum is better preserved than material from vascular plants. Increasing stanol/stenol ratio values and decreasing n-alkane CPI values indicate progressive degradation of organic matter (OM) with depth. The n-alkan-2-one/n-alkane and n-alkan-2-one/n-alkanoic acid ratios were shown to be useful proxies that can reflect the degree of OM preservation and suggest that both microbial oxidation of n-alkanes and decarboxylation of n-alkanoic acids produce n-alkan-2-ones in this peat sequence. 相似文献
2.
Hydrogen isotopic composition of n-alkanes was measured in sediments from an excavated profile of the Early Cretaceous Yixian Formation in Liaoning Province, NE China, aiming to assess the significance of the δD value of n-alkanes in ancient lacustrine sediments as the indicator for determining the source inputs of organic matters and paleoclimatic conditions. The δD values of n-alkanes are in the range of − 250‰ to − 85‰ and display an obvious three-stage variation pattern through the profile, which is consistent with the distribution of the dominated n-alkanes and the profile of their δ13C values. The δD and δ13C values of n-alkanes suggest that short-chain n-alkanes are primarily derived from photosynthetic bacteria and algae; n-C29 and n-C31 are mainly originated from terrestrial higher plants; n-C28 and n-C30 may be derived from the same precursor but via the different biological mechanism of hydrogen isotopic fractionation; while the source inputs of medium-chain n-alkanes are more complicated, with n-C23 being derived from some specific algae or biosynthesized by various aquatic organisms. The paleoclimatic conditions are reconstructed via two approaches. The reconstructed hydrogen isotopic values of lake water and meteoric water (expressed as δDLW and δDMW, respectively) were at the intervals of − 51.8‰ to 17.0‰ and − 118.1‰ to − 43.5‰, respectively, indicating a general climate transition from semi-arid to arid. The calculated ΔδDLW-MW values vary from 37.0‰ to 89.1‰ and display a similar but a significant large-scale variation trend with the ΔδDC23 ‐ long (− 28.8‰ to 85.0‰; long represents long-chain n-alkanes) and ΔδDmid-long (− 15.4‰ to 43.4‰; mid represents medium-chain n-alkanes) values. The discrepancy may be attributed to the source input overlap for n-alkanes and the uncertainties of εwater/lipid values. The coupling of ΔδDC23 ‐ long, ΔδDmid-long and ΔδDLW-MW values with the paleoclimatic evidence indicates that the δD values of n-alkanes could be more sensitive to the change of paleoclimatic conditions. 相似文献
3.
We investigated the effect of ionizing radiation on organic matter (OM) in the carbonaceous uranium (U) mineralization at the Mulga Rock deposit, Western Australia. Samples were collected from mineralized layers between 53 and 58.5 m depths in the Ambassador prospect, containing <5300 ppm U. Uranium bears a close spatial relationship with OM, mostly finely interspersed in the attrinite matrix and via enrichments within liptinitic phytoclasts (mainly sporinite and liptodetrinite). Geochemical analyses were conducted to: (i) identify the natural sources of molecular markers, (ii) recognize relationships between molecular markers and U concentrations and (iii) detect radiolysis effects on molecular marker distributions. Carbon to nitrogen ratios between 82 and 153, and Rock–Eval pyrolysis yields of 316–577 mg hydrocarbon/g TOC (HI) and 70–102 mg CO2/g TOC (OI) indicate a predominantly lipid-rich terrigenous plant OM source deposited in a complex shallow swampy wetland or lacustrine environment. Saturated hydrocarbon and ketone fractions reveal molecular distributions co-varying with U concentration. In samples with <1700 ppm U concentrations, long-chain n-alkanes and alkanones (C27–C31) reveal an odd/even carbon preference indicative of extant lipids. Samples with ⩾1700 ppm concentrations contain intermediate-length n-alkanes and alkanones, bearing a keto-group in position 2–10, with no carbon number preference. Such changes in molecular distributions are inconsistent with diagenetic degradation of terrigenous OM in oxic depositional environments and cannot be associated with thermal breakdown due to the relatively low thermal maturity of the deposits (Rr = 0.26%). It is assumed that the intimate spatial association of high U concentrations resulted in breakdown via radiolytic cracking of recalcitrant polyaliphatic macromolecules (spores, pollen, cuticles, or algal cysts) yielding medium chain length n-alkanes (C13–C24). Reactions of n-alkenes with OH− radicals from water hydrolysis produced alcohols that dehydrogenated to alkanones or through carbonylation formed alkanones. Rapid reactions with hydroxyl radicals likely decreased the isomerization of n-alkenes and decreased alkanone diversity, such that the alkan-2-one isomer is predominant. This specific distribution of components generated by natural radiolysis enables their application as “radiolytic molecular markers”. Breaking of C–C bonds through radiolytic cracking at temperatures much lower than the oil window (<50 °C) can have profound implications on initiation of petroleum formation, paleoenvironmental reconstructions, mineral exploration and in tracking radiolysis of OM. 相似文献
4.
Lake sediments generally contain a mixture of terrestrial and aquatic source inputs, and determining the major inputs is important for understanding geological records in paleoenvironment and paleoclimate research. In this study we describe the distribution of n-alkanes and n-fatty acids (FAs) in representative modern plants from around Lake Qinghai. We found a significant difference in the average length of n-FA carbon chains (ACL Fa16–32) in terrestrial (23.3) and aquatic plants (18.6). The results reveal that ACL Fa16–32 may essentially serve as a proxy for evaluating the major source inputs to lake sediments. Assessment of surface sediments from the lake showed that the FAs originated from a mixture of inputs, with the aquatic source input predominant at most sites. Additionally, the δD values of sediment mid-chain n-acids (C22) showed a relationship with the ACL Fa16–32 proxy: an increased Fa ACL corresponded to more negative hydrogen isotope ratio values. We suggest that different sources should be considered and ACL Fa16–32 could be a potential calibration proxy before using δD values to extract reliable isotopic information from lake water. More attention should be paid to source inputs and their relationship to other geochemical proxies in future studies of lake sediments. 相似文献
5.
The Mundaú–Manguaba estuarine–lagoon system (MMELS) constitutes one of the most representative ecosystems in the state of Alagoas, NE Brazil. Approximately 30% or 60,000 ha of the lower surrounding drainage basin of the MMELS are covered by sugar cane and a total of 250,000 inhabitants contribute untreated effluent to the system. Short sediment cores from MMELS were collected in 2007 at three sites: Manguaba Lagoon (C03), Mundaú Lagoon (C07) and Mundaú River (C08) in order to characterize the delivery and deposition of n-alkanes over the past 40 yr. The n-alkanes ranged from C15 to C35, with total aliphatic hydrocarbon (TAH) concentration in the range 27.8–139.5 μg g−1. An unresolved complex mixture (UCM) was observed in all sediments. The terrigenous/aquatic ratio (TAR), carbon preference index (CPI) and average chain length (ACL) showed that the terrigenous input dominated. The (δ13C) values of individual n-alkanes (C16–C33) varied between −22.6‰ and −34.2‰, suggesting a dominance of 12C-enriched n-alkanes that originated from C3 plants and lacustrine algae. The data reflect how anthropogenic input (via sewage, industrial pollution and agriculture) has influenced the organic content of the system through time. 相似文献
6.
Novel ecosystem development is occurring within the western boreal forest of Canada due to land reclamation following oil sand surface mining. Sphagnum peat is the primary organic amendment used to reconstruct soil in these novel ecosystems. We hypothesised that ecosystem recovery would be indicated by an increasing similarity in the biomolecular characteristics of novel soil organic matter (SOM) derived from peat to those of natural boreal ecosystems. We evaluated the use of the homologous series of long chain (⩾ C21) n-alkanes with odd/even predominance to monitor the re-establishment of boreal forest on these anthropogenic soils. The lipids were extracted from dominant vegetation inputs and SOM from a series of natural and novel ecosystem reference plots. Twice the concentration of n-alkanes was extracted from natural than from novel ecosystem SOM (p < 0.01). We observed unique n-alkane signatures for the source vegetation, e.g. peat material was dominated by C31, and aspen (Populus tremuloides Michx.) leaves by C25. The n-alkane distribution differed between the two systems (p < 0.001) and reflected the dominant vegetation input, i.e. peat or tree species. Our results indicate that further research is required to clarify the influence of vegetation or disturbance on the signature of n-alkanes in SOM; however, the use of n-alkanes as biomarkers of novel ecosystem development is a promising application. 相似文献
7.
Future climatic conditions may coincide with an increased potential for wildfires in grassland and forest ecosystems, whereby charred biomass would be incorporated into soils. Molecular changes in biomass upon charring have been frequently analysed with a focus on black carbon. Aliphatic and aromatic hydrocarbons, known to be liberated during incomplete combustion of biomass have been preferentially analysed in soot particles, whereas determinations of these compounds in charred biomass residues are scarce. We discuss the influence of increasing charring temperature on the aliphatic and aromatic hydrocarbon composition of crop grass combustion residues. Straw from rye, representing C3 grasses and maize, representing C4 grasses, was charred in the presence of limited oxygen at 300, 400 and 500 °C. Typical n-alkane distribution patterns with a strong predominance of long chain odd-numbered n-alkanes maximising at C31 were observed in raw straw. Upon combustion at 300 °C aliphatic hydrocarbons in char were dominated by sterenes, whereas at 400 °C sterenes disappeared and medium chain length n-alkanes, maximising around n-C20, with a balanced odd/even distribution were present. At a charring temperature of 500 °C n-alkane chain length shifted to short chain homologues, maximising at C18 with a pronounced predominance of even homologues. Even numbered, short chain n-alkanes in soils may thus serve as a marker for residues of charred biomass. Aromatic hydrocarbons indicate an onset of aromatization of biomass already at 300 °C, followed by severe aromatization upon incomplete combustion at 400–500 °C. The diagnostic composition of aliphatic and aromatic hydrocarbons from charred biomass affords potential for identifying residues from burned vegetation in recent and fossil soils and sediments. 相似文献
8.
Graham A. Logan Michael A. Abrams Nicola F. Dahdah Emmanuelle Grosjean 《Organic Geochemistry》2009,40(3):365-375
A laboratory study has been conducted to determine the best methods for the detection of C10–C40 hydrocarbons at naturally occurring oil seeps in marine sediments. The results indicate that a commercially available method using n-C6 to extract sediments and gas chromatography–flame ionization detection (GC–FID) to screen the resulting extract is effective at recognizing the presence of migrated hydrocarbons at concentrations from 50 to 5000 ppm. When non-biodegraded, the amount of oil charge is effectively tracked by the sum of n-alkanes in the gas chromatogram. However, once the charge oil becomes biodegraded, with the loss of n-alkanes and isoprenoids, the amount of oil is tracked by the quantification of the unresolved complex mixture (UCM). Gas chromatography–mass spectrometry (GC–MS) was also found to be very effective for the recognition of petroleum related hydrocarbons and results indicate that GC–MS would be a very effective tool for screening samples at concentrations below 50 ppm oil charge. 相似文献
9.
Precise indices based on n-alkane signatures were developed in order to determine the sources and composition of sedimentary organic matter (SOM) in coastal systems. The Arcachon Bay (France), a well-studied temperate lagoon, was used as an example of a complex coastal system sheltering a wide diversity of OM sources. Three main groups of sources were well discriminated from their n-alkane signatures: seagrass (Zostera sp.) produced mainly n-C17, n-C19, n-C21, n-C23 and n-C25 alkanes, algae (Rhodophyta, Chlorophyta) produced n-C15 and n-C17 and the terrigenous input [Quercus sp., Spartina sp. and river suspended particulate OM (SPOM)] was characterized by n-C25, n-C27, n-C29, n-C31 and n-C33. From the above and literature n-alkane fingerprints, we developed a set of indices (n-alkane ratios) to quantify the contribution of these three major sources of the SOM. At the Arcachon Bay scale, they indicated that SOM was composed mainly of seagrass (ca. 53 ± 19%) and terrestrial (ca. 41 ± 17%) material, followed by algae (ca. 6 ± 9%). Moreover, the new n-alkane indices exhibited more relevant spatial patterns than classical ones – the TAR (C27 + C29 + C31/C15 + C17 + C19; terrestrial to aquatic ratio) and the Paq (C23 + C25/C23 + C25 + C29 + C31; aquatic plant %) – with a greater contribution from marine sources in the central part of the lagoon where a high density of Zostera seagrass was observed. Therefore, the development of precise indices adapted to the local diversity of OM sources is needed when using n-alkanes for quantifying the source composition of SOM in complex coastal systems. 相似文献
10.
Noorhazlina Abu BakarKheng Soo Tay Nasr Yousef M.J. OmarM. Radzi Bin Abas Bernd R.T. Simoneit 《Applied Geochemistry》2011,26(8):1433-1445
The molecular distributions of homologous aliphatic lipid compounds (n-alkanes, n-alkanoic acids, n-alkanols, n-alkanals and n-alkan-2-ones) were investigated in sediments of Lake Bera, Malaysia as well as in plant waxes from the vicinity using gas chromatography-mass spectrometry. In addition, triterpenoids of the oleanane, ursane, lupane and friedelane series, and their diagenetic products were also identified. Using the aquatic proxy Paq, it was found that the n-alkanes present in surface sediments S1, S5 and S6 correspond to an input from emergent macrophytes, whereas in sediments collected from open water (S2, S3 and S4) they correspond to input from submerged/floating macrophytes. The presence of n-alkan-2-ols, a commonly found homologous series in the sediments as well as in the plant wax, is novel here. In addition, the presence of 24-methylcycloart-22-enol and 24-ethylcycloart-22-enol in sediments as well as the plant wax of Pandanus helicopus, a dominant reed around the lake, also supports the input of plant biomarkers to the sediments. The occurrence of 5-membered ring triterpenoid derivatives as major diagenetic products of the triterpenoids identified (e.g. friedelan-2,3-dione) shows that the degradation of the organic matter in the sediments occurs mainly under oxic conditions. Also, the presence of ring-A degraded triterpenoids (dihydroputranjivic acid, 3-nor-2,4-seco-friedelane, 4α- and 4β-3-norfriedelanes, A-norfriedel-10-one, and A-norfriedel-8-en-10-one) and the aromatized triterpenoid hydrocarbons (mono- and triaromatic derivatives) as minor diagenetic products indicates photochemical and microorganism-mediated alteration reactions of natural products in the sediments. Additional novel polyfunctional friedelane derivatives, namely friedelane-2,3-dione, friedelane-1,3-diol-2-one and friedel-1(10)-ene-1,3-diol-2-one were identified for the first time in this study. These novel polyfunctional triterpenoids were inferred to derive from the oxidation of the triterpenoids from higher plants in this oxic tropical environment. For future reference purposes, the mass spectra of the identified polar triterpenoids are also presented here. This study provides important data on the biogeochemistry of organic matter in a tropical lake of SE Asia. 相似文献
11.
Ryoshi Ishiwatari Koichi Negishi Hiroyasu Yoshikawa Shuichi Yamamoto 《Organic Geochemistry》2009,40(4):520-530
Temporal changes in paleoproductivity of Lake Biwa (Japan) over the past 32 kyr have been studied by analyzing bulk organic carbon and photosynthetic pigments (chlorins) in the BIW95-5 core. Primary productivity was estimated on the assumption of C/Norg values of 8 for autochthonous organic matter (OM) and 25 for allochthonous OM and using an equation developed for the marine environment. The estimate indicates that primary productivity ranges from 50 to 90 g C m?2 yr?1 in the Holocene, while it is ～60 g C m?2 yr?1 on average in the last glacial. Pheophytin a and pheophorbide a are the major chlorins. A downcore profile of chlorin concentration normalized to autochthonous organic carbon (OC) shows a decreasing trend. Chlorin productivity was corrected by removal of the effect of post-burial chlorin degradation. The temporal profile of chlorin productivity thereby obtained resembles that from autochthonous OC.The difference in primary productivity between the Holocene and the glacial for the lake is markedly smaller than that for Lake Baikal situated in the boreal zone. This difference between the two lakes is probably caused by the difference in their climatic conditions, such as temperature and precipitation. Precipitation at Lake Biwa is relatively large during the glacial and the Holocene because of the continuous influence of the East Asian monsoon. Lake Baikal precipitation is generally small as a result of control by the continental (Siberia) climate regime. In addition, a significant difference in productivity between the glacial and the Holocene for Lake Baikal may be essentially controlled by the hydrodynamic systems in the lake.Lake Biwa terrigenous OM input events occurred at least five times over the period 11–32 kyr BP, suggesting enhanced monsoon activity. Molecular examination of the layer with a large input of terrigenous OM during the Younger Dryas indicates that concentrations of terrigenous biomarkers such as n-C27–C31 alkanes, lignin phenols, cutin acids, ω-hydroxy acids and C29 sterols are high, suggesting that soil OM with peat-like material entered the lake as a result of flooding. An enhanced sedimentation rate in the last 3000 years might have been partially caused by agricultural activity around the lake. 相似文献
12.
Moss covered, high latitude wetlands hold large amounts of terrestrial organic matter (OM), which may be vulnerable to expected climate warming. Molecular analysis of fluvially transported material from these regions can distinguish between different sources of terrestrial OM. Sphagnum moss may represent one of the major sources. This study aimed to quantitatively establish a molecular proxy for identifying Sphagnum-derived OM from high latitude peatlands in the sub-Arctic coastal ocean. We collected and analyzed Sphagnum species throughout northern Sweden and Finland. Results show that the C25/(C25 + C29) n-alkane ratio is most suitable for terrestrial OM source apportionment in these coastal regions since, compared to other n-alkane Sphagnum proxies, it shows (i) the least variation between species, (ii) the most constant values for different latitudinal regimes and (iii) the largest dynamic range to the higher plant end member in two-source mixing models. Application of the proxy to surface sediments and suspended particulate matter in the sub-Arctic northern Baltic Sea shows that 68–103% of the terrestrial OM fraction is derived from Sphagnum-rich peatland. We recommend that future studies on terrestrial OM fluxes into (sub-)Arctic regions should apply the C25/(C25 + C29) proxy to improve insight into the contribution of Sphagnum-derived terrestrial OM from climate-vulnerable, high latitude wetlands. 相似文献
13.
We determined biomarker concentrations and distributions for surface sediments from 54 sites in the Pearl River Estuary, China. We focus on a suite of four biomarker-based indicators for relative terrestrial to marine organic matter (OM) source: the branched-isoprenoid tetraether (BIT) index, the ratio of high/low molecular weight n-alcohols [(ΣC26–34/(ΣC16+18 + ΣC26–34)], an analogous ratio for n-fatty acids and the ΣC29-steroids/(ΣC29-steroids + brassicasterol) ratio. All four exhibit the same terrestrial to marine transition seen in previous bulk δ13C studies, but with an abrupt decrease in the relative terrestrial contribution across the delta front to pro-delta transition. Concentrations of terrestrially-derived biomarkers show no systematic decrease across the transition. Instead, the decrease in the proportion of terrestrial OM is due to a decrease in the sedimentation rate and associated terrestrial OM burial across the delta toe. This suggests that diagenetic controls on the fate of terrestrial OM, such as increased biodegradation where sedimentation rate is low, are subordinate to sedimentological processes. Biomarker-derived temperature values are cooler than expected for the lower Pearl River catchment, suggesting that the dominant component of the terrestrial OM is derived from the cooler upland regions of the catchment. The dominance of input from more distal terrain with greater topographic relief is evidence for the importance of geomorphological control on terrigenous OM transport. Collectively, the results demonstrate the importance of sedimentological processes in the supply, deposition and transport of terrestrial OM. 相似文献
14.
Plant-derived terpenoids, long recognized as biomarkers, can help reveal the major taxonomic groups of land plants present in ancient environments, even if rocks and sediments do not preserve plant macro- or microfossils. Previous studies have used simple di- to triterpenoid ratios to reconstruct floral changes in the geologic past, but few have compared terpenoid ratios with estimates of floral composition from fossils. Further, reconstructions have not taken into account differences in biomarker production (i.e. concentration relative to leaf biomass) between different types of plants. Here, we have examined terpenoids from early Cenozoic fluvial rocks from the Bighorn Basin (Wyoming, USA), where fossil flora has been studied in detail. We analyzed the distributions of diterpenoids, triterpenoids and n-alkanes from leaf wax in a total of 43 samples from 15 stratigraphic horizons of late Paleocene (63 Ma) to early Eocene (53 Ma) in age. In nearly all samples, triterpenoids, derived from angiosperms, were significantly lower in abundance than conifer-specific diterpenoids, a finding that contrasted with plant fossil evidence for the same rocks. This suggests that di- to triterpenoid ratios severely underestimate the abundance of angiosperms in paleovegetation. Angiosperms dominated n-alkane production among modern plants, and we propose a new paleovegetation proxy based on the ratio of diterpenoids (conifers) to n-alkanes (angiosperms), corrected for lipid production estimated from extant vegetation. Using diterpenoids and alkanes, we infer the composition of paleovegetation to be similar to that inferred from plant fossils. Although the approach works well for the Bighorn Basin, we stress the new paleovegetation proxy will need to be evaluated for other time periods, communities, paleogeography and depositional environments with pollen or megafossil data available. 相似文献
15.
Ahmed I. Rushdi Khalid F. Al-Mutlaq Bernd R. T. Simoneit Adnan Al-Azri Ali A. Z. DouAbul Sheikha Al-Zarban Faiza Al-Yamani 《Arabian Journal of Geosciences》2010,3(2):113-131
River runoff and atmospheric fallout (dust and air particulate matter) are major input sources of natural and anthropogenic
terrestrial organic and inorganic components to the Arabian seas. In this study, we report on the various lipid tracer compounds
that might be transported to the Arabian Gulf by rivers, dust, and air particulate matter. These are based on geochemical
analysis of sediment, dust, and particulate samples collected from Iraq, Kuwait, and Saudi Arabia. The samples were extracted
with a dichloromethane/methanol mixture and analyzed by gas chromatography-mass spectrometry. The extractable organic compounds
(lipids) in the samples include n-alkanes, n-alkanoic acids, n-alkanols, methyl n-alkanoates, steroids, triterpenoids, carbohydrates, and petroleum hydrocarbons. The steroids and triterpenoids were major
components in river and wetland samples. The major sources of these lipids were from natural vegetation, microbial (plankton
and bacteria) residues in the sediments, sand, and soils, with some contribution from anthropogenic sources. Accordingly,
these sources could be major inputs to the Arabian seas besides the autochthonous marine products. Future studies of the organic
and inorganic biogeochemistry on river, dust, and coastal areas are needed to characterize the various regional sources, transformation,
and diagenetic processes of the organic matter en route to the marine environment. 相似文献
16.
Laura Sánchez-García J. Ramón de Andrés J. Antonio Martín-Rubí Patrick Louchouarn 《Organic Geochemistry》2009,40(2):184-194
Surface sediments from the Gulf of Cádiz (GoC) were analyzed by alkaline CuO oxidation, in order to estimate the contribution of terrigenous organic matter (TOM) to the inner continental shelf of the southwest Iberian Peninsula. The parallel analysis of sediment samples from the two most important rivers draining to this coastal area (i.e. Guadiana River and Tinto–Odiel fluvial system) provided fundamental information regarding local terrestrial sources. Relatively constant intensive lignin parameters (S:V = 1.0 ± 0.1 and C:V = 0.22 ± 0.04) and high values of the lignin phenol vegetation index (LPVI = 155 ± 43) indicated that non-woody angiosperm tissues constitute the dominant component of vascular plant material reaching the shelf sediments. The NW to SE decreasing isotopic (13C) and molecular (Λ8) signatures found among the sediments, coinciding with the Guadiana delivery plume, suggest that this river is the main terrestrial source in the inner GoC shelf. Slightly elevated values of degradation indicative ratios ([Ad:Al]V = 0.41 ± 0.10; [Ad:Al])S = 0.34 ± 0.07; [3,5-Bd:V] = 0.14 ± 0.05; P:[V + S] = 0.24 ± 0.09) suggested the alteration state of the shelf sediments. The two fold higher ratios of the river sediments (Guadiana: [Ad:Al]V = 0.82 ± 0.08; [Ad:Al]S = 0.84 ± 0.03; Tinto–Odiel: [Ad:Al]V = 0.86 ± 0.12; [Ad:Al]S = 0.83 ± 0.013) and the increasing degradation trend observed outward in the shelf, lead us to consider preferential sorption processes, instead of in situ diagenesis, to affect the degradation signature of the shelf sediments. Preferentially solubilized degraded OM is more likely to be sorbed and stabilized prior to transport to the marine system, showing an apparently more advanced degradation state. The use of the 3,5-Bd:V ratio in conjunction with (Ad:Al)V revealed a composition continuum of the sedimentary OM ranging from fresh plant materials to highly altered soil humic constituents. Elemental and molecular analyses show a land to sea gradient by a NW to SE decrease of the terrestrial influence, accounting for larger terrestrial inputs (TOM: 71–98%) in those sediments near the Guadiana mouth, and predominantly autochthonous composition (TOM: 42–50%) in those located offshore. This work utilizes lignin derived biomarkers to determine the contribution of terrigenous OM delivered to this poorly described coastal area from regional rivers. Within a context of increasing international efforts to better understand the global C cycling, this study illustrates the relevance of using the alkaline CuO oxidation approach to evaluate C budgets and continental influence in river dominated ocean margins. 相似文献
17.
《Applied Geochemistry》2006,21(6):1006-1015
We investigated the ability of accelerated solvent extraction (ASE) to extract selected lipid biomarkers (C19–C34 n-alkanes, n-alcohols and n-fatty acids as well as dehydroabietic acid and β-sitosterol) from a sandy soil profile under Corsican pine. Two organic layers (moss and F1) as well as two mineral soil horizons (EA and C1) were sampled and extracted with DCM/MeOH (93:7 v/v) by ASE at 75 °C and a pressure of 6.9 × 106 Pa or 17 × 106 Pa. Soxhlet extractions were used as the established reference method. After clean-up and derivatization with BSTFA, the extracts were analyzed on GC/MS.Using Soxhlet as a reference, we found ASE to extract all compounds adequately. The n-alkanes, especially, were found to be extracted very efficiently from all horizons studied. Only the n-fatty acids and β-sitosterol from the organic layers seemed to be extracted at a slightly lower efficiency by ASE. In all but two instances the relative abundance of extracted lipids within a component class was the same regardless of the extraction method used.Using a higher pressure in the ASE extractions significantly increased the extraction efficiency for all component classes in the moss layer, except β-sitosterol. The effect was most pronounced for the n-alkanes. In the EA horizon, a higher pressure slightly reduced the extraction efficiency for dehydroabietic acid. The observed differences between ASE and Soxhlet extractions as well as the pressure effect can be explained by a decrease in polarity of the extractant due to the elevated pressure and temperature applied during ASE extractions as compared to Soxhlet extractions. This would mainly increase the extraction efficiency of the least polar biomarkers: the n-alkanes as was observed. In addition, a better penetration of still partially water-filled micro pores under elevated pressure and temperature may have played a role. 相似文献
18.
We present a systematic study of chain-length distributions and D/H ratios of n-alkyl lipids (both n-alkanes and n-alkanoic acids) in a wide range of terrestrial and aquatic plants around and in Blood Pond, Massachusetts, USA. The primary goal is to establish a model to quantitatively assess the aquatic plant inputs of the mid-chain length n-alkyl lipids to lake sediments and to determine the average hydrogen isotopic ratios of these lipids in different plants. Our results show that middle-chain n-alkyl lipids (C21-C23n-alkanes and C20-C24n-alkanoic acids) are exceptionally abundant in floating and submerged aquatic plants, in contrast to the dominance of long-chain n-alkyl lipids (C27-C31n-alkanes and C26-C32n-alkanoic acids) in other plant types, which are consistent with previously published data from Mountain Kenya and the Tibetan Plateau. Combining available data in different environmental settings allows us to establish statistically robust model distributions of n-alkyl lipids in floating/submerged macrophytes relative to other plant types. Based on the model distributions, we established a multi-source mixing model using a linear algebra approach, in order to quantify the aquatic inputs of mid-chain n-alkyl lipids in lake sediments. The results show that ∼97% of the mid-chain n-alkyl lipids (C23n-alkane and C22n-acid (behenic acid)) in Blood Pond sediments are derived from floating and submerged macrophytes. In addition, D/H ratios of C22n-acid and C23n-alkane in the floating and submerged plants from Blood Pond display relatively narrow ranges of variation (−161 ± 16‰ and −183 ± 18‰, respectively). Our study demonstrates that mid-chain n-alkyl lipids such as C23n-alkane and C22n-acid could be excellent recorders of past lake water isotopic ratios in lakes with abundant floating and submerged macrophyte inputs. 相似文献
19.
Ryoshi Ishiwatari Naoki Fujino David Brincat Shuichi Yamamoto Hikaru Takahara Koji Shichi Sergey K. Krivonogov 《Organic Geochemistry》2009,40(1):51-60
We characterized the compositions of organic compounds in a Cheremushka bog sediment core (deposited over the last 35 kyr), located at the eastern coast of Lake Baikal, to obtain basic information about the terrestrial organic matter (OM) which contributed to Lake Baikal sediments. The bog sediment was analyzed for the molecular composition of n-alkanes, lignin phenols and n-C24 to C30 alkanoic acids, as well as the carbon isotopic composition of plant wax derived n-C27 to C33 alkanes.Concentrations of lignin phenols [vanillyl (V) plus syringyl (S) phenols] normalized to total organic carbon (TOC) in the Holocene are twice those for the last glacial maximum (LGM), while concentrations of TOC-normalized n-C24 to C30 alkanoic acids do not change markedly in this period. Thus, the ratio of lignin phenols to n-C24 to C30 alkanoic acids increases from the LGM to the Holocene. This result is essentially consistent with pollen analysis indicating an expansion of woody plants in the Holocene and a prevailing herb-abundant environment for the LGM. The δ13C values of n-C27 to C33 alkanes (e.g. ?29‰ to ?33‰ for C31) indicate the presence of C3-dominant plants throughout the core.The contribution of terrestrial OM to Lake Baikal sediments was estimated using the biomarkers, on the assumption that the OM in the bog sediments is a representative of the terrestrial OM around the lake. Hence, the estimation using lignin phenol or n-C24 to C30 alkanoic acid parameters indicates that 11–24% of the TOC in the Academician Ridge sediments is land-derived for both the Holocene and the LGM, which is similar to the estimates from C/N values of bulk OM. However, the estimates for terrestrial OM using the n-C27 to C33 alkane parameter are generally higher than those using lignin phenol or n-C24 to C30 alkanoic acid parameters. The difference is thought to be associated with the difference in source and behavior of these biomarkers. 相似文献
20.
Joseph H. Street R. Scott Anderson Robert J. Rosenbauer Adina Paytan 《Quaternary Research》2013,79(1):14-23
n-Alkane biomarker distributions in sediments from Swamp Lake (SL), in the central Sierra Nevada of California (USA), provide evidence for an increase in mean lake level ~ 3000 yr ago, in conjunction with widespread climatic change inferred from marine and continental records in the eastern North Pacific region. Length distributions of n-alkane chains in modern plants growing at SL were determined and compared to sedimentary distributions in a core spanning the last 13 ka. As a group, submerged and floating aquatic plants contained high proportions of short chain lengths (< nC25) compared to emergent, riparian and upland terrestrial species, for which chain lengths > nC27 were dominant. Changes in the sedimentary n-alkane distribution over time were driven by variable inputs from plant sources in response to changing lake level, sedimentation and plant community composition. A shift toward shorter chain lengths (nC21, nC23) occurred between 3.1 and 2.9 ka and is best explained by an increase in the abundance of aquatic plants and the availability of shallow-water habitat in response to rising lake level. The late Holocene expansion of SL following a dry mid-Holocene is consistent with previous evidence for increased effective moisture and the onset of wetter conditions in the Sierra Nevada between 4.0 and 3.0 ka. 相似文献