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1.
The distribution of glycerol dialkyl glycerol tetraethers (GDGTs) can reflect continental environmental changes. Recently, the distribution of branched GDGTs (bGDGTs) has been proposed as a novel tool for paleoelevation reconstructions. Here we report the variation in TEX86 (tetraether index of 86 carbon atoms) of isoprenoidal GDGTs (iGDGTs) and MBT (methylation of branched tetraether index) of bGDGTs along an altitudinal transect on Mt. Xiangpi, NE Qinghai-Tibetan Plateau. Both TEX86 and MBT values of surface soils showed significant linear decreases with altitude (TEX86: R2 = 0.65; n = 50; MBT: R2 = 0.69; n = 24). We suggest that the apparent relationships between the two indices and altitude may be related to temperature. Our preliminary investigation suggests that the TEX86 index can potentially be applied as a paleoelevation indicator in addition to the MBT index on the Qinghai-Tibetan Plateau.  相似文献   

2.
This study of five small (<3.0 ha) lakes in southwestern Greenland examines the veracity of branched glycerol dialkyl glycerol tetraethers (br GDGTs) as a temperature proxy in lacustrine systems. The proximity (<5 km) of the lakes suggests that their temperature history, and thus their br GDGT records, should be similar. Distributions of br GDGTs in (i) surface sediments from all five lakes, (ii) 14C-dated sediment cores from two lakes (Upper and Lower EVV Lakes) and (iii) soil samples from the area surrounding the lakes were examined. The temporal records of br GDGT-based temperature for the two cores exhibited both similarities and major discrepancies. The differences between the paleotemperature records for the two lakes suggest that br GDGTs are not solely soil-derived, reflecting air temperature, but also indicate an additional br GDGT contribution from another source. Among the broader suite of lake sediments, there was a strong correlation (R2 0.987) between br GDGT-based surface sediment temperatures and measured summer bottom water temperatures for the four lakes with hypoxic/anoxic bottom waters, including Upper EVV Lake. The correlation suggests production of br GDGTs by anaerobic bacteria within the bottom water and/or sediment–water interface, reflecting environmental temperature for the individual lakes and augmenting the uniform, soil-derived signal. Hence, assessment of br GDGTs in Greenland lake sediments provides evidence for their origin from anaerobic autochthonous bacteria and indicates that interpretation of lacustrine br GDGT-based paleotemperature records requires contextual knowledge of individual lake systems and potential source(s) of sedimentary br GDGTs.  相似文献   

3.
We studied the distribution of glycerol dialkyl glycerol tetraethers (GDGTs) in suspended particulate matter from the water column of Lake Tanganyika (East Africa), where sediment studies had shown the applicability of the TEX86 proxy for reconstructing surface lake water temperature. GDGTs, in particular crenarchaeol, showed maximum abundance within the suboxic zone (100–180 m), suggesting that this is the preferred niche of ammonia-oxidizing Thaumarchaeota. Despite evidence for anaerobic methane oxidation in deep anoxic water (300–1200 m) no unambiguous evidence for an imprint of methanotrophic archaea on GDGT distribution was found. Comparison of TEX86 and BIT indices with those of surface sediments suggests that the sedimentary GDGTs are derived predominantly from the oxic zone and suboxic zone of the lake.  相似文献   

4.
Archaeal and bacterial glycerol dialkyl glycerol tetraether lipids (GDGTs) are used in various proxies, such as TEX86 and the BIT index. In living organism, they contain polar head groups (intact polar lipids – IPLs). IPL GDGTs have also been detected in ancient marine sediments and it is unclear whether or not they are fossil entities or are part of living cells. In order to determine the extent of degradation of IPL GDGTs over geological timescales, we analyzed turbidite deposits, which had been partly reoxidized for several kyr after deposition on the Madeira Abyssal Plain. Analysis of core lipid (CL) and IPL-derived GDGTs showed a reduction in concentration by two orders of magnitude upon post-depositional oxidation, while IPL GDGTs with a mono- or dihexose head group decreased by 2–3 orders of magnitude. The BIT index for CL- and IPL-derived GDGTs increased substantially upon oxidation from 0.1 to up to 0.5. Together with changing MBT/CBT values, this indicates preferential preservation of soil-derived branched GDGTs over marine isoprenoid GDGTs, combined with in situ production of branched GDGTs in the sediment. The TEX86 value for IPL-derived GDGTs decreased by 0.07 upon oxidation, while that of CL GDGTs showed no significant change. Isolation of IPLs revealed that the TEX86 value for monohexose GDGTs was 0.55, while the that for dihexose GDGTs was substantially higher, 0.70. Thus, the decrease in TEX86 for IPL-derived GDGTs was in agreement with the dominance of monohexose GDGTs in the oxidized turbidite, probably caused by a combination of in situ production as well as selective preservation of terrestrial isoprenoid GDGTs. Due to the low amount of IPL GDGTs vs. CL GDGTs, the impact of IPL degradation on CL-based TEX86 paleotemperature estimates was negligible.  相似文献   

5.
Glycerol dialkyl glycerol tetraethers (GDGTs) and bulk organic geochemical parameters were examined for a short core from the Bohai Sea, a Yellow River-dominated continental margin. A three end member mixing model using branched/isoprenoid tetraethers (BIT) index, δ13C and C/N shows that the average fractions of soil, marine and plant organic matter (OM) during the period of 1933–2011 are 67.7% (38–92%), 26.1% (0–58%) and 6.2% (0–23%), respectively. Abrupt changes of sedimentary OM compositions around 1953, 1976 and 1996 are synchronous with the Yellow River mouth relocations. The BIT index values (0.33–0.80) present a stronger correlation with crenarchaeol abundance (R2 = 0.88) than branched GDGTs abundance (R2 = 0.27), suggesting that variations of marine Thaumarchaeota abundance rather than soil OM inputs is the first order factor controlling the BIT index values, although this proxy has been widely used for soil OM. The comparison between the BIT index, nutrient status and historical Yellow River sediment load indicates that the high sensitivity of the BIT index to the Yellow River channel shifts cannot be explained by a nutrient stimulation mechanism, but instead is likely caused by the restriction of Thaumarchaeota growth in highly turbid water due to the enormous sediment inputs from Yellow River. Our study demonstrates that local conditions should be considered when applying the BIT index as an environmental proxy.  相似文献   

6.
Branched glycerol dialkyl glycerol tetraethers (GDGTs) are bacterial membrane lipids, ubiquitously present in soils and peat bogs, as well as in rivers, lakes and lake sediments. Their distribution in soil is controlled mainly by pH and mean annual air temperature, but the controls on their distribution in lake sediments are less well understood. Several studies have found a relationship between the distribution of branched GDGTs in lake sediments and average lake water pH, suggesting an aquatic source for them, besides that for soil transported to the lake via erosion. We sampled the surface water suspended particulate matter (SPM) from 23 lakes in Minnesota and Iowa (USA), that vary widely in pH, alkalinity and trophic state. The SPM was analyzed for the concentration and distributions of core lipid (presumed fossil origin) and intact polar lipid (IPL, presumed to derive from living cells) branched GDGTs. The presence of substantial amounts (18–48%) of IPL-derived branched GDGTs suggests that branched GDGTs are likely of autochthonous origin. Temperature estimates based on their distribution using lake-specific calibrations agree reasonably with water temperature at time of sampling and average air temperature of the season of sampling. Importantly, a strong correlation between the distribution of branched GDGTs and lake water pH was found (r2 0.72), in agreement with a predominant in situ production. An stronger correlation was found with lake water alkalinity (r2 0.83), although the underlying mechanism that controls the relationship is not understood. Our results raise the potential for reconstructing pH/alkalinity of past lake environments, which could provide important knowledge on past developments in lake water chemistry.  相似文献   

7.
Recently, 6-methyl branched glycerol dialkyl glycerol tetraethers (brGDGTs) were separated from 5-methyl brGDGTs, which are used in brGDGT-based proxies. Here we analyzed brGDGTs in 27 soil samples along the 400 mm isoline of mean annual precipitation in China by using tandem 2D liquid chromatography. The fractional abundance of 6-methyl brGDGTs showed a positive correlation with soil pH, while that of 5-methyl brGDGTs decreased with increasing soil pH. The abundance ratio of 6-/5-methyl brGDGTs, namely the isomerization of branched tetraethers (IBT), was calculated. The correlation of IBT with pH (pH = 6.33 − 1.28 × IBT; R2 0.89; root mean squared error, RMSE, 0.24) was much stronger than that of the traditionally used cyclization index of branched tetraethers (CBT) with pH (R2 0.52; RMSE 0.49) and comparable with that of CBT′ with pH (R2 0.88; RMSE 0.25). Compiling all available data from 319 soil samples resulted in a global calibration: pH = 6.53 − 1.55 × IBT (R2 0.72; RMSE 0.65), which has a better correlation than the CBT5ME-pH proxy (R2 0.63; RMSE 0.78), but a weaker correlation than the CBT′-pH proxy (R2 0.85; RMSE 0.52). Our result suggests that the IBT is a promising indicator for soil pH, particularly in cases when some compounds in the CBT′ index cannot be determined.  相似文献   

8.
Branched glycerol dialkyl glycerol tetraethers (GDGTs) are membrane lipids of unknown bacteria that are ubiquitous in soil and peat. Two indices based on the distribution of these lipids in soils, the Cyclization of Branched Tetraethers (CBT) and the Methylation of Branched Tetraethers (MBT) indices have been shown to correlate with soil pH, and mean annual air temperature (MAT) and soil pH, respectively, and can be used to reconstruct MAT in palaeoenvironments. To verify the extent to which branched GDGTs in marine sediments reflect the distribution pattern on land and whether these proxies are applicable for palaeoclimate reconstruction in high latitude environments with a MAT of <0 °C, we compared the branched GDGT distribution in Svalbard soils and nearby fjord sediments. Although branched GDGT concentrations in the soil are relatively low (0.02–0.95 μg/g dry weight (dw)) because of the cold climate and the short growing season, reconstructed MATs based on the MBT/CBT proxy are ca. ?4 °C, close to the measured MAT (ca. ?6 °C). Concentrations of branched GDGTs (0.01–0.20 μg/g dw) in fjord sediments increased towards the open ocean and the distribution was strikingly different from that in soil, i.e. dominated by GDGTs with one cyclopentane moiety. This resulted in MBT/CBT-reconstructed MAT values of 11–19 °C, well above measured MAT. The results suggest that at least part of the branched GDGTs in marine sediments in settings with a low soil organic matter (OM) input may be produced in situ. In these cases, the application of the MBT/CBT palaeothermometer will generate unrealistic MAT reconstructions. The MBT/CBT proxy should therefore only be used at sites with a substantial input of soil OM relative to the amount of marine OM, i.e. at sites close to the mouth of rivers with a catchment area where sufficient soil formation takes place and the soil thus contains substantial amounts of branched GDGTs.  相似文献   

9.
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10.
Carbon isotope ratio (δ13C) values of lipid biomarkers from plants can be used to assess water use efficiency and to reconstruct environmental conditions in the past. We assessed the effect of salinity on the δ13C values for leaf wax n-C31 and n-C33 alkanes, bulk leaf matter and leaf total lipid extracts from Avicennia marina (gray mangrove) trees growing along the Brisbane River estuary in Queensland, Australia. We observed an increase in 0.19 ± 0.053‰ (R2 0.61, p 0.008) and 0.16 ± 0.052‰ (R2 0.55, p 0.01) per salinity unit for the two n-alkanes, respectively, and of 0.087 ± 0.028‰ (R2 0.41, p 0.009) for whole leaves per salinity unit, indicating that water use efficiency of A. marina increased with the salt content of water. There was no correlation between δ13C values of total lipid extracts and salinity, perhaps because of a decrease in lipid concentration at higher salinity or because of varying contributions of different lipid classes to the extract. The robust relationship between salinity and δ13C values of leaf wax lipids provides a means of quantitatively reconstructing past salinity from carbon isotope ratios of mangrove lipid biomarkers in sediments. When paired with measurements of the hydrogen isotope ratio values of the same compounds, the approach should facilitate quantitative reconstruction of the hydrogen isotope composition of environmental water. In order for the method to successfully reconstruct past salinity and water isotopes, a mangrove source for leaf wax would need to be confirmed by palynological or other evidence, or the isotopic composition of a more source specific biomarker, such as taraxerol, would need to be measured.  相似文献   

11.
Porewater advection stimulates nutrient exchange and microbial activity in shallow marine sediments, whereas element cycling in deeper diffusion-dominated sediments is comparatively slow due to limited nutrient supply. We studied the vertical distribution of microbial communities and organic matter (OM) cycling in these contrasting porewater regimes down to 5 m depth at an intertidal flat of the southern North Sea. Archaea, Bacteria and Eukarya were targeted, combining intact polar lipid (IPL) analysis with qualitative and quantitative molecular biological techniques. The largely sandy section 1 of the core (<75 cm) is characterized by rapid burial of fresh marine OM and intense porewater advection. This supply fuels heterotrophic microbes, as evident from the 13C isotopic composition of total organic carbon and IPL derivatives. Major sources of OM are algae and cyanobacteria, as suggested by the elevated amount of eukaryotic 18S rRNA gene copies and phosphate-free IPLs. The relative abundance of most phospholipids remained largely constant over the entire core, except for diphosphatidylglycerol, which represented about half of total IPL abundance in the lower part of section 1 (>50 cm) and the diffusion-dominated section 2 (75–490 cm). This suggests bacteria adapting their membranes in response to increasing physicochemical stress and starvation in the nutrient limited, fine grained sediments of section 2 with less bioavailable, predominantly terrestrial, OM. Relative amounts of bacterial acyl ether and diether phospholipids increased in this lower section and were assigned to sulfate reducers and yet uncultured myxobacteria. Archaea were an order of magnitude less abundant than Bacteria, and were affiliated mainly with Methanosarcinales and Methanomicrobiales. Accordingly, the archaeal IPL composition was typical for a methanogenic community. IPLs not exclusively derived from in situ microbial production emphasize that these biomarkers have to be interpreted with caution in sediments with complex hydrogeology. Our results demonstrate that contrasting subsurface flow regimes significantly impact on the vertical zonation of biogeochemical properties and microorganisms in marine sediments.  相似文献   

12.
Radiocarbon dates from known age, pre-bomb eastern oyster (Crassostrea virginica) shells provide local marine reservoir corrections (?R) for Chesapeake Bay and the Middle Atlantic coastal area of eastern North America. These data suggest subregional variability in ?R, ranging from 148 ± 46 14C yr on the Potomac River to ? 109 ± 38 14C yr at Swan Point, Maryland. The ?R weighted mean for the Chesapeake's Western Shore (129 ± 22 14C yr) is substantially higher than the Eastern Shore (? 88 ± 23 14C yr), with outer Atlantic Coast samples falling between these values (106 ± 46 and 2 ± 46 14C yr). These differences may result from a combination of factors, including 14C-depleted freshwater that enters the bay from some if its drainages, 14C-depleted seawater that enters the bay at its mouth, and/or biological carbon recycling. We advocate using different subregional ?R corrections when calibrating 14C dates on aquatic specimens from the Chesapeake Bay and coastal Middle Atlantic region of North America.  相似文献   

13.
Glycerol dialkyl glycerol tetraether (GDGT) lipids are membrane lipids which were long thought to be synthesized mainly by archaea, organisms thought to be limited to extreme environments. Analysis of environmental samples over the last decade has shown, however, that their structural diversity and sources are much wider than anticipated and that they occur ubiquitously in a wide range of environments, such as oceans and lakes, and their (sub)surface sediments, as well as soils. Several GDGTs have been unambiguously identified and can be used as biomarker lipids, since they are preserved in immature sediments <140 Ma. Close examination of the distributions has led to the discovery that GDGTs might be used as proxies for certain environmental parameters, such as the input of soil organic matter to marine environments, soil pH, air temperature and sea and lake water temperature. Here, we review the progress made over the last decade in the analysis, occurrence and recognition of sources of GDGTs, their applications as biomarker lipids, and the development and application of proxies based on their distributions.  相似文献   

14.
Branched glycerol dialkyl glycerol tetraether lipids (GDGTs) are membrane lipids of soil bacteria that occur ubiquitously in soil, but their occurrence as intact polar lipids (IPLs) has not been well studied. Here, we report the identification and distribution of IPL-branched GDGTs throughout a depth profile of a Swedish peat bog. In addition to two reported glycosidic IPL branched GDGTs, we identified IPL branched GDGTs with a hexose-glycuronic acid, phospho-hexose, or hexose-phosphoglycerol head group, based on mass spectrometry. A selected reaction monitoring (SRM) assay was developed to monitor changes in head group distribution with depth. The abundance of the IPL branched GDGTs increased below the water table, suggesting that they were primarily produced in this part of the peat. This was supported by the concentrations of core lipid and IPL-derived branched GDGTs, which also substantially increased below the water table. However, individual IPL trends differed, which may be due to changes in the microbial community composition with depth or to different degradation rates for the different IPL branched GDGTs. The SRM method was also applied to two different soil types, which showed that similar IPL branched GDGTs as those in peat were present, albeit with different distributions.  相似文献   

15.
Four representatives of methanogenic Euryarchaeota (Methanosarcina mazei strain Gö1, Methanosphaera stadtmanae, Methanobrevibacter smithii and Methanosaeta thermophila), the hyperthermophilic euryarchaeon Thermococcus kodakarensis and the halophilic euryarchaeon Haloferax volcanii were studied for their glycerol ether lipid composition. The predominant core membrane lipid in all of them was archaeol, which was accompanied by variable quantities of sn-2-hydroxyarchaeol in the methanogens M. mazei (Methanosarcinales) and M. stadtmanae (Methanobacteriales). All methanogenic and hyperthermophilic Euryarchaeota also contained comparatively high abundances of the glycerol dialkyl glycerol tetraether without a cyclopentane moiety (GDGT-0). The methanoarchaeon M. stadtmanae, in addition to GDGT-0, contained GDGT core lipid structures with 1–4 cyclopentane moieties (GDGTs 1–4). We also found minor amounts of a glycerol trialkyl glycerol tetraether (GTGT) and a glycerol dialkanol diether (GDD), both of which did not contain cyclopentane moieties, as well as methylated and dimethylated GDGT-0 in all the archaea with the exception of H. volcanii. Like its GDGT distribution, M. stadtmanae showed an extended range of GDD structures with up to two cyclopentane ring systems. Our results thus indicate that both methanogenic and hyperthermophilic Euryarchaeota may represent source organisms of GTGT-0, GDDs and methylated-GDGTs in natural environments. All the latter components have recently been reported to be ubiquitously distributed in marine sediments but their biological origin is largely unknown. Moreover, a suite of unsaturated GDGTs without a cyclopentane moiety and up to four double bonds in the hyperthermophile T. kodakarensis was tentatively assigned.  相似文献   

16.
The relative abundances and distributions of branched glycerol dialkyl glycerol tetraethers (brGDGTs) in marine and lacustrine sediments have been recently used as paleo-environmental proxies for the input of soil organic matter and past continental temperatures, respectively. The putative main source of brGDGTs is soil bacteria. Therefore, these biomarkers are also part of the soil organic matter stock that accumulates in the terrigenous environment. Here we present a method for isolating and purifying these compounds from lake sediments, soils and peat for radiocarbon (14C) measurement using a combination of normal and reversed phase high performance liquid chromatography, allowing complete separation of co-eluting compounds. Radiocarbon analysis was performed on an accelerator mass spectrometer system equipped with a gas ion source. We assessed the accuracy and the necessary corrections with modern and radiocarbon-dead procedural blanks. Blank assessment revealed that the reverse phase step introduced significant amounts of extraneous carbon, while the normal phase step did not. We show that with our method and instrumentation it is possible to obtain accurate and precise 14C analyses of brGDGTs with sample amounts as small as 10 μg C. Finally we demonstrate the application of the measurement of 14C concentrations of several brGDGTs isolated from lake sediments and peat soils.  相似文献   

17.
《Quaternary Science Reviews》1999,18(10-11):1185-1203
A 13 m long core from the lake-swamp at Pobochnoye (53°01′30″ N, 51°50′30″ E) in the Buzuluk pine forest in the middle part of the Volga River basin, Russia was studied for pollen, peat stratigraphy, mollusc, δ18O/δ16O and δ13C/δ12C analyses and radiocarbon dating. For the first time the environment history of the east European Russia has been reconstructed for the last 14,000 years; ca 14,000–13,000 BP cold dry steppes spread across the basin of the Samara River. Isotope data indicate that the main climate shift occurred ca 10,000 BP at the Lateglacial–Holocene transition when climate became warmer and forests expanded. Pinus sylvestris L. expanded 10,000 BP. Ca 9,000 BP Ulmus, Quercus and Corylus appeared in the Buzuluk forest followed at ca. 7,000 BP by Alnus, then Tilia and Acer at 6000 BP. Between 6000 and 4500 BP the climatic conditions were optimal for the forest growth in the Samara River basin. 5500–5000 BP the lake became shallower and was transformed into the eutrophic peat swamp. Between 4500–3500 BP climate became drier and hotter and forest less abundant. Between 3500–2400 BP the forest cover again increased. Between 2400–2000 BP the pine forest area has reduced, apparently due to increased dryness, and around 2000 BP the modern environment in the Buzuluk area has been in existence.  相似文献   

18.
High-frequency spectral decay factor, kappa (k), in the accelerograms of the Wenchuan mainshock was measured using strong motion data from 52 stations within 311 km of the epicenter. The derived k range from 0.0034 s to 0.0468 s. The correlation of k versus fault distance was given, which is k = 0.01288 + 5.9068 × 10–5 R for the N-S component, k = 0.01881 + 1.4219 × 10–5 R for the E-W component, and k = 0.00855 + 5.6086 × 10–5 R for the U-D component. The analysis on the spatial variation of k demonstrates that k relates to source effect and propagation effect besides local site effect. Ground motions for the 52 stations were simulated using derived k and compared to actual recordings in terms of waveforms, amplitude spectra and response spectra. The results show agreement at shorter periods (<1 s), but a slight overestimation at longer periods (1–7 s).  相似文献   

19.
Significant amounts of sulfuric acid (H2SO4) rich saline water can be produced by the oxidation of sulfide minerals contained in inland acid sulfate soils (IASS). In the absence of carbonate minerals, the dissolution of phyllosilicate minerals is one of very few processes that can provide long-term acid neutralisation. It is therefore important to understand the acid dissolution behavior of naturally occurring clay minerals from IASS under saline–acidic solutions. The objective of this study was to investigate the dissolution of a natural clay-rich sample under saline–acidic conditions (pH 1–4; ionic strengths = 0.01 and 0.25 M; 25 °C) and over a range of temperatures (25–45 °C; pH 1 and pH 4). The clay-rich sample referred to as Bottle Bend clay (BB clay) used was from an IASS (Bottle Bend lagoon) in south-western New South Wales (Australia) and contained smectite (40%), illite (27%), kaolinite (26%) and quartz (6%). Acid dissolution of the BB clay was initially rapid, as indicated by the fast release of cations (Si, Al, K, Fe, Mg). Relatively higher Al (pH 4) and K (pH 2–4) release was obtained from BB clay dissolution in higher ionic strength solutions compared to the lower ionic strength solutions. The steady state dissolution rate (as determined from Si, Al and Fe release rates; RSi, RAl, RFe) increased with decreasing solution pH and increasing temperature. For example, the highest log RSi value was obtained at pH 1 and 45 °C (−9.07 mol g−1 s−1), while the lowest log RSi value was obtained at pH 4 and 25 °C (−11.20 mol g−1 s−1). A comparison of these results with pure mineral dissolution rates from the literature suggests that the BB clay dissolved at a much faster rate compared to the pure mineral samples. Apparent activation energies calculated for the clay sample varied over the range 76.6 kJ mol−1 (pH 1) to 37.7 kJ mol−1 (pH 4) which compare very well with the activation energy values for acidic dissolution of monomineralic samples e.g. montmorillonite from previous studies. The acid neutralisation capacity (ANC) of the clay sample was calculated from the release of all structural cations except Si (i.e. Al, Fe, K, Mg). According to these calculations an ANC of 1.11 kg H2SO4/tonne clay/day was provided by clay dissolution at pH 1 (I = 0.25 M, 25 °C) compared to an ANC of 0.21 kg H2SO4/tonne clay/day at pH 4 (I = 0.25 M, 25 °C). The highest ANC of 6.91 kg H2SO4/tonne clay/day was provided by clay dissolution at pH 1 and at 45 °C (I = 0.25 M), which is more than three times higher than the ANC provided under the similar solution conditions at 25 °C. In wetlands with little solid phase buffering available apart from clay minerals, it is imperative to consider the potential ANC provided by the dissolution of abundantly occurring phyllosilicate minerals in devising rehabilitation schemes.  相似文献   

20.
Small angle neutron scattering techniques have been applied to investigate the phase behavior of CO2 injected into coal and possible changes in the coal pore structure that may result from this injection. Three coals were selected for this study: the Seelyville coal from the Illinois Basin (Ro = 0.53%), Baralaba coal from the Bowen Basin (Ro = 0.67%), and Bulli 4 coal from the Sydney Basin (Ro = 1.42%). The coals were selected from different depths to represent the range of the underground CO2 conditions (from subcritical to supercritical) which may be realized in the deep subsurface environment. The experiments were conducted in a high pressure cell and CO2 was injected under a range of pressure conditions, including those corresponding to in-situ hydrostatic subsurface conditions for each coal. Our experiments indicate that the porous matrix of all coals remains essentially unchanged after exposure to CO2 at pressures up to 200 bar (1 bar = 105 Pa). Each coal responds differently to the CO2 exposure and this response appears to be different in pores of various sizes within the same coal. For the Seelyville coal at reservoir conditions (16 °C, 50 bar), CO2 condenses from a gas into liquid, which leads to increased average fluid density in the pores (ρpore) with sizes (r) 1 × 105 ≥ r ≥ 1 × 104 Å (ρpore ≈ 0.489 g/cm3) as well as in small pores with size between 30 and 300 Å (ρpore ≈ 0.671 g/cm3). These values are by a factor of three to four higher than the density of bulk CO2 (ρCO2) under similar thermodynamic conditions (ρCO2 ≈ 0.15 g/cm3). At the same time, in the intermediate size pores with r ≈ 1000 Å the average fluid density is similar to the density of bulk fluid, which indicates that adsorption does not occur in these pores. At in situ conditions for the Baralaba coal (35 OC, 100 bar), the average fluid density of CO2 in all pores is lower than that of the bulk fluid (ρpore / ρCO2 ≈ 0.6). Neutron scattering from the Bulli 4 coal did not show any significant variation with pressure, a phenomenon which we assign to the extremely small amount of porosity of this coal in the pore size range between 35 and 100,000 Å.  相似文献   

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