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1.
Guido L. B. Wiesenberg Jan Schwarzbauer Michael W. I. Schmidt Lorenz Schwark 《Organic Geochemistry》2004,35(11-12):1371
Agricultural soils are regarded as one potential sink for atmospheric CO2 via photosynthetic fixation in plant biomass and subsequent transformation into soil organic matter upon soil diagenesis. The difference in C-isotope signatures of C3- vs. C4-plants allows for a natural isotopic labelling of soil organic matter after changes from C3- to C4-cropping. In this study, we demonstrate that isotopic shifts are paralleled by molecular signatures of C3- vs. C4-crop alkyl lipids. Turnover times vary significantly, based on cropping techniques. For grain-maize cropped soils at steady state average turnover times of 40 years for bulk SOC, 35 years for n-alkanes and 21 years for n-carboxylic acids were determined. Turnover times for silage-maize cropped soil at steady state were on average 250 years for bulk SOC, 60 years for n-alkanes and 49 years for n-carboxylic acids. Turnover times reported here for silage-maize cropped soils may be taken as maximum values only, because they derive from a single trial, which was affected by addition of anthropogenic refractory carbon. Discrimination of input from various plant parts (roots, stems and leaves) based on bulk C-isotopes is not feasible but can easily be achieved using compositions of carboxylic acids, especially the ratio of n-C24 vs. n-C22+26 and their respective C-isotope values. This enables delineation of the influence of different cropping techniques, e.g., silage- or grain-maize, on carbon storage in soils. Admixture of external sources of organic matter to the soil organic carbon pool of an urban site in Halle, Germany was identified based on alkyl lipid distributions. Nearby lignite mining was identified as a source for non-crop-derived alkyl lipids, primarily based on the elevated n-C26-carboxylic acid content and heavier carbon isotopic signatures. 相似文献
2.
Simon C George Christopher J Boreham Sandra A Minifie Stan C Teerman 《Organic Geochemistry》2002,33(12)
A suite of 18 oils from the Barrow Island oilfield, Australia, and a non-biodegraded reference oil have been analysed compositionally in order to detail the effect of minor to moderate biodegradation on C5 to C9 hydrocarbons. Carbon isotopic data for individual low molecular weight hydrocarbons were also obtained for six of the oils. The Barrow Island oils came from different production wells, reservoir horizons, and compartments, but have a common source (the Upper Jurassic Dingo Claystone Formation), with some organo-facies differences. Hydrocarbon ratios based on hopanes, steranes, alkylnaphthalenes and alkylphenanthrenes indicate thermal maturities of about 0.8% Rc for most of the oils. The co-occurrence in all the oils of relatively high amounts of 25-norhopanes with C5 to C9 hydrocarbons, aromatic hydrocarbons and cyclic alkanes implies that the oils are the result of multiple charging, with a heavily biodegraded charge being overprinted by fresher and more pristine oil. The later oil charge was itself variably biodegraded, leading to significant compositional variations across the oilfield, which help delineate compartmentalisation. Biodegradation resulted in strong depletion of n-alkanes (>95%) from most of the oils. Benzene and toluene were partially or completely removed from the Barrow Island oils by water washing. However, hydrocarbons with lower water solubility were either not affected by water washing, or water washing had only a minor effect. There are three main controls on the susceptibility to biodegradation of cyclic, branched and aromatic low molecular weight hydrocarbons: carbon skeleton, degree of alkylation, and position of alkylation. Firstly, ring preference ratios at C6 and C7 show that isoalkanes are retained preferentially relative to alkylcyclohexanes, and to some extent alkylcyclopentanes. Dimethylpentanes are substantially more resistant to biodegradation than most dimethylcyclopentanes, but methylhexanes are depleted faster than methylpentanes and dimethylcyclopentanes. For C8 and C9 hydrocarbons, alkylcyclohexanes are more resistant to biodegradation than linear alkanes. Secondly, there is a trend of lower susceptibility to biodegradation with greater alkyl substitution for isoalkanes, alkylcyclohexanes, alkylcyclopentanes and alkylbenzenes. Thirdly, the position of alkylation has a strong control, with adjacent methyl groups reducing the susceptibility of an isomer to biodegradation. 1,2,3-Trimethylbenzene is the most resistant of the C3 alkylbenzene isomers during moderate biodegradation. 2-Methylalkanes are the most susceptible branched alkanes to biodegradation, 3-methylalkanes are the most resistant and 4-methylalkanes have intermediate resistance. Therefore, terminal methyl groups are more prone to bacterial attack compared to mid-chain isomers, and C3 carbon chains are more readily utilised than C2 carbon chains. 1,1-Dimethylcyclopentane and 1,1-dimethylcyclohexane are the most resistant of the alkylcyclohexanes and alkylcyclopentanes to biodegradation. The straight-chained and branched C5–C9 alkanes are isotopically light (depleted in 13C) relative to cycloalkanes and aromatic hydrocarbons. The effects of biodegradation consistently lead to enrichment in 13C for each remaining hydrocarbon, due to preferential removal of 12C. Differences in the rates of biodegradation of low molecular weight hydrocarbons shown by compositional data are also reflected in the level of enrichment in 13C. The carbon isotopic effects of biodegradation show a decreasing level of isotopic enrichments in 13C with increasing molecular weight. This suggests that the kinetic isotope effect associated with biodegradation is site-specific and often related to a terminal carbon, where its impact on the isotopic composition becomes progressively ‘diluted’ with increasing carbon number. 相似文献
3.
We measured hydrogen isotope compositions (δD) of high-molecular-weight n-alkanes (C27-C33) from grasses grown in greenhouses and collected from the US Great Plains. In both cases, n-alkanes from C4 grasses are enriched in D by more than 20‰ relative to those from C3 grasses. The apparent enrichment factor (εC29-GW) between C29n-alkane and greenhouse water is −165 ± 12‰ for C3 grasses and −140 ± 15‰ for C4 grasses. For samples from the Great Plains, δD values of C29n-alkanes range from −280 to −136‰, with values for C4 grasses ca. 21‰ more positive than those for C3 grasses from the same site. Differences in C3 and C4 grass n-alkane δD values are consistent with the shorter interveinal distance in C4 grass leaves, and greater back-diffusion of enriched water from stomata to veins, than in C3 grass leaves. Great Plains’ grass n-alkane isotopic ratios largely reflect precipitation δD values. However, the offset or apparent fractionation between n-alkanes and precipitation is not uniform and varies with annual precipitation and relative humidity, suggesting climatic controls on lipid δD values. The dryer sites exhibit smaller absolute apparent fractionation indicative of D-enrichment of source waters through transpiration and/or soil evaporation. To explore the relationship between climate and n-alkane δD values, we develop three models. (1) The ‘direct analog’ model estimates δDC29 values simply by applying the apparent enrichment factors, εC29-GW, observed in greenhouse grasses to precipitation δD values from the Great Plains. (2) The ‘leaf-water’ model uses a Craig-Gordon model to estimate transpirational D-enrichment for both greenhouse and field sites. The transpiration-corrected enrichment factors between C29 and bulk leaf-water, εC29-GW, calculated from the greenhouse samples (−181‰ for C3 and −157‰ for C4) are applied to estimate δDC29 values relative to modeled bulk leaf-water δD values. (3) The ‘soil- and leaf-water’ model estimates the combined effects of soil evaporation, modeled by analogy with a flow-through lake, and transpiration on δDC29 values. Predictions improve with the addition of the explicit consideration of transpiration and soil evaporation, indicating that they are both important processes in determining plant lipid δD values. D-enrichment caused by these evaporative processes is controlled by relative humidity, suggesting that important climatic information is recorded in leaf wax n-alkane δD values. Calibration studies such as this one provide a baseline for future studies of plant-water-deuterium systematics and form the foundation for interpretation of plant wax hydrogen isotope ratios as a paleo-aridity proxy. 相似文献
4.
5.
文章利用黄土高原西缘代表性的塬堡剖面有机碳同位素数据,估算了末次冰期以来地表植被中C3/C4植 物的相对丰度,指示出研究区域末次冰期几乎为纯粹的C3植物,而全新世为C3植物占优势的C3和C4混合植被类 型。温度是控制中国黄土高原C4植物是否发生的关键性气候因素,末次冰期向全新世转化过程中存在的某“阈值 温度”控制了两种植被类型的存在。全新世土壤有机碳同位素偏正于末次冰期,符合前人研究得到的认识。末次 冰期间冰段(MIS3)至盛冰期,土壤有机碳同位素为偏正变化趋势,符合现代C3植物本身随气候条件改变的碳同位 素组成变化。研究表明,利用黄土-古土壤有机碳同位素进行古气候变化研究,不能只将有机碳同位素简单的解 释为C3/C4植物相对丰度的变化,在单一植被类型下,还需要考虑植物本身碳同位素组成随气候条件的变化;另外, 研究还说明,我国黄土高原不同地区同时段土壤有机碳同位素值可以不同,其变化可以不具有相同的趋势,因此, 简单将有机碳同位素偏正归因于夏季风增强是值得商榷的。 相似文献
6.
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
7.
Simultaneous mass spectral detection and stable carbon isotope analysis was performed on individual indigenous n-alkanes isolated from single C4 and C3 plant species and on a series of aliphatic and polycyclic aromatic hydrocarbons (PAH) produced from the combustion of these same biomass materials. The analysis technique used a combined gas chromatograph-mass spectrometer/combustion/isotope ratio mass spectrometer (GC-MS/C/IRMS). Precision (2σ) for replicate measurements of individual compounds in standard solutions using this novel configuration ranged between 0.2 and 0.5‰ for n-alkanes and 0.3 and 0.8‰ for PAH. Accuracy of the n-alkane measurements ranged between 0.1 and 0.4‰ and that of the PAH measurements ranged between 0.2 and 0.9‰. Replicate GC-MS/C/IRMS measurements on the combustion-derived n-alkene/alkane pairs were performed to within a precision of between 0.1 and 1.1‰ and the precision for the combustion PAH was similar to the standard PAH solution. No notable isotopic effects were observed when altering the temperature of the combustion process from 900 to 700°C, or as a result of the individual n-alkenes/alkanes partitioning between the gaseous and condensate fractions. Combustion-derived n-alkenes/alkanes ranged from C11 to C31, and the C4-derived n-alkenes/alkanes were approx. 8‰ more enriched in 13C than the C3-derived compounds. Both the C4 and C3-derived n-alkenes/alkanes (C20-C30) were isotopically similar to the indigenous n-alkanes and were 2-3‰ more depleted in 13C than the lower mol. wt (C1111-C19) n-alkenes/alkanes, suggesting an independent origin for the lower mol. wt compounds. Combustion-generated C4 and C3-derived 2-, 3-, and 4-ring PAH were also isotopically distinct (Δδ = 10‰). Unlike the n-alkenes/alkanes, no compound-to-compound variations were observed between the low and high mol. wt PAH. This study demonstrates that the isotopic composition of original plant biomass material is mainly preserved in the aliphatic hydrocarbons and PAH generated by its combustion. Consequently, analyses of these compounds in sediments impacted by fire occurrences may provide useful information about paleo-fire activity that may help elucidate the impact biomass burning may have had and could have on climate-biosphere interactions. 相似文献
8.
Will Meredith Chen-Gong Sun Colin E. Snape Mark. A. Sephton Gordon D. Love 《Organic Geochemistry》2006,37(12):1705
This study describes the reduction of functionalised model compounds to their corresponding hydrocarbons by catalytic hydropyrolysis to provide information on the release of biomarkers from kerogens and asphaltenes covalently bound through the functional groups investigated. Five model compounds were investigated, the n-C18 carboxylic acids, stearic and oleic acids; the C24 steroidal acid, 5β-cholanic acid; and the saturated and unsaturated C27 sterols, 5α-cholestanol and cholesterol. The yield and distribution of the hydrocarbons generated were assessed for the model compounds adsorbed to silica and carbon substrates, and unsupported on a bed of catalyst. The n-C18 acids are shown to be reduced to the n-C18 alkane, with a selectivity of >95% for stearic acid, although due to its unsaturated structure, oleic acid is prone to cracking, with shorter chained n-alkanes also being formed. The conversion of these compounds, adsorbed to either silica or carbon is relatively low, even at hydropyrolysis temperatures significantly above their boiling point, suggesting that interactions between the acids and substrate leading to the formation of stable entities (Si–O–C linkages in the case of silica) significantly retard volatilisation. The yield can be increased by placing the compounds directly onto a bed of catalyst, but for low boiling compounds such as stearic acid this can result in volatilisation and cracking at temperatures below that of the activation point of the catalyst. This method produced improved yields of >95% pure product for higher boiling compounds such as 5β-cholanic acid. The presence of the functional group attached to the ring system of compounds such as 5α-cholestanol does not diminish the selectivity of the technique. The double bond in cholesterol resulted in more incomplete hydrogenation with sterenes being generated, and in addition to 5α and 5β-cholestane, diasteranes were also generated via migration of the double bond. 相似文献
9.
Unusual short chain lanostanes (C24 and C25) and C30 lanostane were identified in sulfur rich crude oils from the Jinxian Sag, Bohai Bay Basin, northern China. Besides the regular steranes (C27-30), a series of 4-methyl steranes (C22−23, C27−30), 4,4-dimethyl steranes (C22−24, C28−30), short chain steranes (C23−26), abundant pregnanes (C21−22) and androstanes (C19−20), together with sulfur containing steroids (20-thienylpregnanes and thienylandrostanes) were detected in the aliphatic and branched-cyclic hydrocarbon fraction of these crude oils. A literature survey of some long chain sterane analogues (e.g., A-nor-steranes, norcholestanes, C30 steranes, lanostanes) and pregnanes seems to point to a sponge and/or dinoflagellate source. 4-Methyl, 4,4-dimethyl steroids and lanosterols (4,4,14-trimethyl steroids as the basic skeleton of lanostanes) can be derived from methanotrophic bacteria. Thus, a biological origin from a prokaryotic methylotroph can be used to explain the common source of abundant short chain steranes (C23-26), 4-methyl (C22-23) and 4,4-dimethyl steranes (C22-24), as well as lanostanes (C24-25 and C30 analogues) in our oil samples. Generally, the steroids appear to have been extensively sulfurized with sulfur substitution at the C-22 position in the side chain during the early stage of diagenesis, which was readily subject to attack by bacterial degradation (enzymatic cleavage) and/or abiotic oxidation. As a consequence, short chain sterane analogues (e.g., abundant pregnanes and androstanes in this study) and short chain lanostanes (C24−C25) might later be released through cleavage of weak C-S bonds at the C-22 carbon in the sulfurized steroids and lanostane sulfides. Finally, the formation of the short chain C24−C25 lanostanes and distinctive occurrence of short chain steranes in this study can be well explained by microbial biodegradation of sulfurized lanostanoids and steroids in the reservoir. 相似文献
10.
Yang Pu Hucai Zhang Guoliang Lei Fengqin Chang Mingsheng Yang Xianyu Huang 《Frontiers of Earth Science》2009,3(3):327-335
Lipids extracted from lacustrine deposits in the paleolake Qarhan of the Qaidam basin in the northeastern Tibetan Plateau
were determined by conventional gas chromatography-mass spectrometry. Several series of biomarkers were identified, mainly
including n-alkanes, n-alkan-2-ones, n-alkanoic acids, branched alkanes, triterpenoids and steroids, indicative of various biogenic contributions. On the basis
of cluster analysis, the n-C15, n-C17, n-C19 alkanes were proposed to be derived from algae and/or photosynthetic bacteria, the n-C21, n-C23, n-C25 homologues from aquatic plants, and the n-C29, n-C31 homologues from vascular plants. In contrast, the n-C27 alkane is not categorized in the n-C29 and n-C31 group of alkanes, probably due to more complex origins including both aquatic and vascular plants, and/or differential biodegradation.
Stratigraphically, layers-2, 4 and 5 were found to show a close relationship in n-alkane distribution, associated with a positive shift in carbon isotope composition of bulk organic matter (δ13Corg), inferring a cold/dry period. Layers-1 and 6 were clustered together in association with a negative δ13Corg, excursion, probably indicating a relatively warm/humid climate. The potential coupling between the n-alkane distributions and δ13Corg, suggests a consequence of vegetation change in response to climate change, with the late MIS3 being shown to be unstable,
thought to be the climatic optimum in the Tibetan Plateau. Our results suggest that the cluster analysis used in this study
probably provides an effective and authentic method to investigate the n-alkane distribution in paleolake sediments. 相似文献
11.
Imogen Poole Pim F. van Bergen Johan Kool Stefan Schouten David J. Cantrill 《Organic Geochemistry》2004,35(11-12):1261
The degree of isotopic variation in fossil organic matter renders bulk δ13C signatures strongly influenced by molecular isotopic heterogeneity. For example, in fossil wood the relative abundance of less depleted 13C moieties, i.e. preserved 13C enriched polysaccharides versus the relatively 13C depleted lignin moieties, can be seen to significantly bias δ13Cfossil wood values. Moreover the variation in δ13C values of specific compounds within fossil material are themselves highly variable and reflect the heterogeneity in isotopic values of different carbon atoms within individual compounds. For studies using δ13C values of fossil plant material as proxies (e.g., for δ13Cpalaeoatmosphere, δ13Cbiomass) it is recommended that the biases introduced through molecular heterogeneity, preservation type and taxonomic status of the fossil material are determined initially. Biases inherent in the bulk signature can then be reduced, rendering this value more robust. Alternatively, compound specific stable carbon isotope measurements of individual moieties preserved through geological time might prove to be an alternative proxy for monitoring changes in the bulk δ13C value of the plant and might reveal atmospherically induced trends. 相似文献
12.
Stable carbon isotopes have been frequently used to indicate carbon pools and processes in soils, plants, and the atmosphere. Carbon isotope compositions are particularly useful in partitioning soil carbon sources between C3 and C4 vegetation because of the distinct δ13C distributions for C3 and C4 vegetation. Remote sensing is a powerful tool used to identify ecosystem patterns and processes at larger scales. A union of these two approaches would hold promise for spatially continuous estimates of carbon isotope compositions. In the current study, a framework is presented for using high spatial resolution remote sensing to predict soil δ13C distributions across a southern Africa savanna ecosystem. The results suggest that if the vegetation–soil δ13C relationship can be established, soil δ13C distributions can be estimated by high-resolution satellite images (e.g., IKONOS, Quickbird). Despite limitations remote sensing is a promising tool to expand estimates of terrestrial δ13C spatial patterns and dynamics. 相似文献
13.
Mathematical models of hydrocarbon formation can be used to simulate the natural evolution of different types of organic matter and to make an overall calculation of the amounts of oil and/or gas produced during this evolution. However, such models do not provide any information on the composition of the hydrocarbons formed or on how they evolve during catagenesis.From the kinetic standpoint, the composition of the hydrocarbons formed can be considered to result from the effect of “primary cracking” reactions having a direct effect on kerogen during its evolution as well as from the effect of “secondary cracking” acting on the hydrocarbons formed.This report gives experimental results concerning the “primary cracking” of Types II and III kerogens and their modelling. For this, the hydrocarbons produced have been grouped into four classes (C1, C2–C5, C6–C15 and C15+). Experimental data corresponding to these different classes were obtained by the pyrolysis of kerogens with temperature programming of 4°C/min with continuous analysis, during heating, of the amount of hydrocarbons corresponding to each of these classes.The kinetic parameters of the model were optimized on the basis of the results obtained. This model represents the first step in the creation of a more sophisticated mathematical model to be capable of simulating the formation of different hydrocarbon classes during the thermal history of sediments. The second step being the adjustment of the kinetic parameters of “secondary cracking”. 相似文献
14.
Angela Vogts Heiko Moossen Florian Rommerskirchen Jürgen Rullkötter 《Organic Geochemistry》2009,40(10):1037-1054
Leaf wax components of terrestrial plants are an important source of biomass in the geological records of soils, lakes and marine sediments. Relevant to the emerging use of plant wax derived biomarkers as proxies for past vegetation composition this study provides key data for C3 plants of tropical and subtropical Africa. We present analytical results for 45 savanna species and 24 rain forest plants sampled in their natural habitats. Contents and distribution patterns of long chain n-alkanes (n-C25 to n-C35) and n-alkan-1-ols (n-C24 to n-C34) as well as bulk and molecular carbon isotopic data are presented. The variations of the analysed parameters among different growth forms (herb, shrub, liana and tree) are small within the vegetation zones, whereas characteristic differences occur between the signatures of rain forest and savanna plants. Therefore, we provide averaged histogram representations for rain forest and savanna C3 plants.The findings were compared to previously published data of typical C4 grass waxes of tropical and subtropical Africa. Generally, trends to longer n-alkane chains and less negative carbon isotopic values are evident from rain forest over C3 savanna to C4 vegetation. For n-alkanols of rain forest plants the maximum of the averaged distribution pattern is between those of C3 savanna plants and C4 grasses. The averaged presentations for tropical and subtropical vegetation and their characteristics may constitute useful biomarker proxies for studies analysing the expansion and contraction of African vegetation zones. 相似文献
15.
Even-carbon number C22-C28n-alkanes, are present in higher concentrations than their C21-C29 odd-carbon number homologs in an organic-rich rock of Mississippian (ca. 310 × 106-yr-old) age, which contains algae-like remnants. Environmental indicators associated with this organic-rich rock permitted environmental comparison with ancient and modern environments that contain n-alkanes which exhibit similar distributions. The results of these comparisons suggest that even-carbon number n-alkanes are preferentially produced in highly saline, carbonate environments where aerobic and anaerobic bacteria have subsisted on the remains of blue-green algae. 相似文献
16.
David M. Nelson Feng Sheng Hu Jill A. Mikucki Ann Pearson 《Geochimica et cosmochimica acta》2007,71(16):4005-4014
Pollen grains from grasses using the C3 and C4 photosynthetic pathways have distinct ranges of δ13C values that may be used to estimate their relative abundance in paleorecords. We evaluated a spooling-wire microcombustion device interfaced with an isotope-ratio mass spectrometer (SWiM-IRMS) for δ13C analysis of individual grass-pollen grains. Pollen from four C3 and four C4 grass species was isolated through micromanipulation and analyzed as single grains suspended in water. A carbon yield greater than the 2σ range of the carbon content of blanks containing only water was used to distinguish samples containing pollen (“pollen present”) from those not containing pollen. This criterion resulted in the exclusion of ∼45% of the 946 samples applied to the wire. The average δ13C values (±1σ) of the remaining samples were −26.9‰ (±6.3‰) and −11.5‰ (±9.6‰) for C3 grasses and C4 grasses, respectively, after blank-correcting the δ13C data. These results suggest that the SWiM-IRMS system can be used to distinguish C3 from C4 grass pollen. The high variability in measured δ13C values is likely caused by a combination of factors. These include natural isotopic variability among individual pollen grains; the relatively poor precision that can be obtained when determining δ13C values of such small samples; and the uncertainty in the magnitude, isotopic composition, and stability of the analytical blank. Nonetheless, high percentages of individual pollen grains were correctly classified as being of either C3 or C4 origin. On average, 90% (range = 78-100%) of pollen grains from C3 grasses had δ13C values more negative than the cutoff threshold of −19.2‰; while 84% (range = 77-90%) of pollen grains from C4 grasses had δ13C values more positive than −19.2‰. Compared with analysis using an elemental analyzer interfaced with an IRMS (EA-IRMS), the number of pollen grains required for δ13C-based evaluation of C3/C4 grass composition is many times lower with the SWiM-IRMS. Additionally, δ13C data from the SWiM-IRMS does not need to be incorporated into a mixing model to derive estimates of the abundance of C3 and C4 grass pollen. Carbon-isotopic analysis of individual grass-pollen grains using the SWiM-IRMS system may help improve our understanding of the evolutionary and ecological significance of grass taxa in the paleorecord. 相似文献
17.
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
18.
Stephanie Kusch Janet Rethemeyer Enno Schefuß 《Geochimica et cosmochimica acta》2010,74(24):7031-7047
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
19.
Lipid geochemistry in a sediment core from Ruoergai Marsh deposit (Eastern Qinghai-Tibet plateau, China) 总被引：3，自引：0，他引：3
Peats in a sediment core from Ruoergai bog, which has a cold and moist plateau climate with major source input from herbaceous plants, have been studied by GC–MS in order to understand the composition and diagenetic processes of lipids in this depositional environment. Long chain components (C21–C35) predominate in the n-alkanes, n-alk-1-enes, n-fatty acids, n-alkan-2-ones and n-alkanols with a maximum of C31, C27, C22 or C24, C23 or C25 and C22, respectively. A herbaceous origin for these long chain compounds is suggested, and this is supported by their stable carbon isotopic compositions. Diterpenoid hydrocarbons with abietane, pimarane and kaurane skeletons, some of which have not been reported often in modern sediments, are prominent and are derived from higher plants. Several triterpenoid ketones and alcohols with oleanane or lupane skeletons, and a series of des-A-triterpenoid hydrocarbons which have not been reported often in modern sediments are also present, and are assigned to a higher plant source. Hopanoids, including their alkanes, alkenes, ketones, alcohols and esters, are abundant and of bacterial origin. Steroid ketones and alkanols are dominated by C29 homologues. C28 and C29 steroids are derived mainly from higher plants, whereas the C27 component is assigned to a microbial source. The presence of short-chain n-alkanes with no odd-even carbon predominance, bacterially derived fatty acids (C14, C15, iso- and unsaturated acids), n-alkan-2-ones, des-A-triterpenoid hydrocarbons, hopanoids and some steroid ketones indicate that intense microbial reworking of the organic matter has taken place in this depositional environment. The chemical and biochemical conversions of some cyclic alkenes to alkanes, such as tricyclic diterpenoids, tetracyclic terpenoids and steroid ketones, are also evident with depth. The dominance of C20 components in the diterpenoid hydrocarbons may reflect an oxidizing or reducing depositional condition. 相似文献
20.
Lignin and fatty acid records in Lake Baikal sediments over the last 130 kyr: A comparison with pollen records 总被引：1，自引：0，他引：1
A 10 m sediment core from Academician Ridge in Lake Baikal was analyzed for its molecular composition using on-line TMAH (tetramethylammomium hydroxide) thermochemolysis. Major products are lignin phenols, n-C14 to C30 fatty acids (alkanoic acids), cutin acids, hydroxy acids and aliphatic dicarboxylic acids. Lignin phenols are abundant in warmer periods (the interglacial: marine isotope stage (MIS) 5e and MIS 1), but extremely low in the other (colder) periods. This result coincides well with pollen records reported for a core near the present site, where an expansion of coniferous forests in sub-stage 5e and MIS 1 was implied. Normal C24–C30 alkanoic acids, important components of plant wax esters, are abundant in 5e and MIS 1 and are present in significant amounts in the other (colder) periods, unlike the lignin phenols. A high abundance of n-C24 to C30 alkanoic acids relative to lignin phenols in the Bølling–Allerød warm period suggests an enhanced development of herbs.It is implied from comparison of the sedimentary lignin phenol record with fossil pollen records and lignin phenol analysis of modern pollen that the ratio of cinnamyl phenols to vanillyl phenols may serve as an indicator of pollen contribution to sedimentary organic matter. 相似文献