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1.
南海全新世大暖期海表水的高酸性证据   总被引:1,自引:1,他引:0       下载免费PDF全文
利用正热电离质谱高精度测定了南海化石珊瑚样品的δ11B 比值,定量地重建了中晚全新世以来南海海表水的pH值。结果显示南海海表水pH值并不像预先设想的那样稳定。其中古海水pH值最低为6100aB.P.前的7.91;   最高为4300aB.P.前和1200aB.P.前的8.29。南海海表水pH值从全新世大暖期开始,整体上呈缓慢增加趋势,而到现代以后明显下降。珊瑚δ11B记录表明南海海表水在中晚全新世有两个高酸性的时期,一个发生在全新世大暖期,一个为现代。全新世大暖期时南海出现的高海平面、偏强的东亚夏季风和偏弱的冬季风可能是导致其海表水出现高酸性的原因。现代南海海表水pH值显著偏低,背离了中晚全新世以来南海海表水pH值逐渐增加的趋势,这很可能说明人类大量排放的CO2确实改变了南海海表水自然变化的规律,南海在变酸。  相似文献   

2.
Evidence for ocean acidification in the Great Barrier Reef of Australia   总被引:1,自引:0,他引:1  
Geochemical records preserved in the long-lived carbonate skeleton of corals provide one of the few means to reconstruct changes in seawater pH since the commencement of the industrial era. This information is important in not only determining the response of the surface oceans to ocean acidification from enhanced uptake of CO2, but also to better understand the effects of ocean acidification on carbonate secreting organisms such as corals, whose ability to calcify is highly pH dependent. Here we report an ∼200 year δ11B isotopic record, extracted from a long-lived Porites coral from the central Great Barrier Reef of Australia. This record covering the period from 1800 to 2004 was sampled at yearly increments from 1940 to the present and 5-year increments prior to 1940. The δ11B isotopic compositions reflect variations in seawater pH, and the δ13C changes in the carbon composition of surface water due to fossil fuel burning over this period. In addition complementary Ba/Ca, δ18O and Mg/Ca data was obtained providing proxies for terrestrial runoff, salinity and temperature changes over the past 200 years in this region. Positive thermal ionization mass spectrometry (PTIMS) method was utilized in order to enable the highest precision and most accurate measurements of δ11B values. The internal precision and reproducibility for δ11B of our measurements are better than ±0.2‰ (2σ), which translates to a precision of better than ±0.02 pH units. Our results indicate that the long-term pre-industrial variation of seawater pH in this region is partially related to the decadal-interdecadal variability of atmospheric and oceanic anomalies in the Pacific. In the periods around 1940 and 1998 there are also rapid oscillations in δ11B compositions equivalent changes in pH of almost 0.5 U. The 1998 oscillation is co-incident with a major coral bleaching event indicating the sensitivity of skeletal δ11B compositions to loss of zooxanthellate symbionts. Importantly, from the 1940s to the present-day, there is a general overall trend of ocean acidification with pH decreasing by about 0.2-0.3 U, the range being dependent on the value assumed for the fractionation factor α(B3-B4) of the boric acid and borate species in seawater. Correlations of δ11B with δ13C during this interval indicate that the increasing trend towards ocean acidification over the past 60 years in this region is the result of enhanced dissolution of CO2 in surface waters from the rapidly increasing levels of atmospheric CO2, mainly from fossil fuel burning. This suggests that the increased levels of anthropogenic CO2 in atmosphere has already caused a significant trend towards acidification in the oceans during the past decades. Observations of surprisingly large decreases in pH across important carbonate producing regions, such as the Great Barrier Reef of Australia, raise serious concerns about the impact of Greenhouse gas emissions on coral calcification.  相似文献   

3.
MIS 11 is often considered to be the best climatic analogue for the Holocene. Many studies have suggested, however, that it is a period of extreme climate warmth comparable in temperatures to the Middle and Late Pliocene. In Britain deposits of the Hoxnian interglacial are correlated to MIS 11 and multi-proxy techniques can be used to reconstruct the climate of this interglacial. Soil, groundwater and freshwater carbonates are common in Hoxnian deposits and the stable isotopic composition of these precipitates can be used to increase our understanding of MIS 11 environments in Britain. Carbonates from Marks Tey, Clacton, Swanscombe, Elveden and West Stow are studied, the stratigraphic context of which indicates that their formation is broadly synchronous (in the mid-Hoxnian, pollen zones Ho II to Ho III). The carbon isotopic composition of groundwater and pedogenic carbonates is typically depleted with respect to δ13C (ca −9 to −8‰ VPDB) reflecting uptake of plant respired CO2 during water migration/recharge. The carbon isotopic composition of lacustrine carbonate is more enriched with respect to δ13C (ca 0-1‰VPDB) reflecting the equilibration of lake waters with atmospheric CO2. The δ18O of groundwater and pedogenic carbonates is slightly more enriched than modern soil carbonates but not as enriched as soil carbonates formed under interglacials that were warmer than the Holocene (i.e. the Cromerian). The stable isotopic composition of Hoxnian carbonates does not, therefore, indicate that this interglacial was characterised by uniquely warm climates in the context of other Middle Pleistocene interglacials and the Holocene. This is contrary to many marine and littoral records from around the world but consistent with environmental records from Britain and Europe.  相似文献   

4.
Boron isotope compositions (δ11B) and B concentrations of rains and snows were studied in order to characterize the sources and fractionation processes during the boron atmospheric cycle. The 11B/10B ratios of instantaneous and cumulative rains and snows from coastal and continental sites show a large range of variations, from −1.5 ± 0.4 to +26.0 ± 0.5‰ and from −10.2 ± 0.5 to +34.4 ± 0.2‰, respectively. Boron concentrations in rains and snows vary between 0.1 and 3.0 ppb. All these precipitation samples are enriched in 10B compared to the ocean value (δ11B = +39.5‰). An empirical rain-vapour isotopic fractionation of +31‰ is estimated from three largely independent methods. The deduced seawater-vapour fractionation is +25.5‰, with the difference between the rain and seawater fractionations principally reflecting changes in the speciation of boron in the liquid with ∼100% B(OH)3 present in precipitations. A boron meteoric water line, δD = 2.6δ11B − 133, is proposed which describes the relationship between δD and δ11B in many, but not all, precipitations. Boron isotopic compositions of precipitations can be related to that of the seawater reservoir by the seawater-vapour fractionation and one or more of (1) the rain-vapour isotopic fractionation, (2) evolution of the δ11B value of the atmospheric vapour reservoir via condensation-precipitation processes (Rayleigh distillation process), (3) any contribution of vapour from the evaporation of seawater aerosols, and (4) any contribution from particulate matter, principally sea salt, continental dust and, perhaps more regionally, anthropogenic sources (burning of biomass and fossil fuels). From the δ11B values of continental precipitations, a sea salt contribution cannot be more than a percent or so of the total B in precipitation over these areas.  相似文献   

5.
Boron isotope composition of marine carbonates has been proposed as a paleo-pH proxy and potential tool to reconstruct atmospheric pCO2. The precise knowledge of the boron isotopic composition of ancient seawater represents the fundamental prerequisite for any paleo-pH reconstruction. This contribution presents boron isotope values for Silurian to Permian brachiopod calcite that might be used to reconstruct pH or boron isotope composition of past oceans. All brachiopod shells were screened for diagenetic recrystallization by means of cathodoluminescence microscopy, trace element geochemistry (B, Fe, Mn, Sr) as well as SEM. Only nonluminescent shells revealing well-preserved microstructures, high strontium and boron concentrations as well as low iron and manganese contents were accepted for boron isotope analysis. The boron isotope ratios of Silurian, Devonian, Pennsylvanian and Permian brachiopod calcite range from 6.8 to 11.0‰, 7.3 to 14.9‰, 12.4 to 15.8‰ and 10.1 to 11.7‰, respectively. These δ11B values are significantly lower in comparison to δ11B values of modern biogenic carbonates and indicate that the Paleozoic oceans were depleted in 11B by up to 10‰. Box modeling of the boron geochemical cycle suggests that the significant depletion of 11B in the oceanic reservoir may have been initiated by an enhanced continental boron discharge. Our data support the earlier made conclusion that boron isotopes may not be used in the geological past as reliable paleo-pH proxy unless the boron isotopic composition of ancient oceans can be constrained by further studies.  相似文献   

6.
We present one millennium-long (1171-year), and three 100 year long annually resolved δ13C tree-ring chronologies from ecologically varying Juniperus stands in the Karakorum Mountains (northern Pakistan), and evaluate their response to climatic and atmospheric CO2 changes. All δ13C records show a gradual decrease since the beginning of the 19th century, which is commonly associated with a depletion of atmospheric δ13C due to fossil fuel burning. Climate calibration of high-frequency δ13C variations indicates a pronounced summer temperature signal for all sites. The low-frequency component of the same records, however, deviates from long-term temperature trends, even after correction for changes in anthropogenic CO2. We hypothesize that these high-elevation trees show a response to both climate and elevated atmospheric CO2 concentration and the latter might explain the offset with target temperature data. We applied several corrections to tree-ring δ13C records, considering a range of potential CO2 discrimination changes over the past 150 years and calculated the goodness of fit with the target via calibration/verification tests (R2, residual trend, and Durbin-Watson statistics). These tests revealed that at our sites, carbon isotope fixation on longer timescales is affected by increasing atmospheric CO2 concentrations at a discrimination rate of about 0.012‰/ppmv. Although this statistically derived value may be site related, our findings have implications for the interpretation of any long-term trends in climate reconstructions using tree-ring δ13C, as we demonstrate with our millennium-long δ13C Karakorum record. While we find indications for warmth during the Medieval Warm Period (higher than today’s mean summer temperature), we also show that the low-frequency temperature pattern critically depends on the correction applied. Patterns of long-term climate variation, including the Medieval Warm Period, the Little Ice Age, and 20th century warmth are most similar to existing evidence when a strong influence of increased atmospheric CO2 on plant physiology is assumed.  相似文献   

7.
Pedogenic goethites in each of two Early Permian paleosols appear to record mixing of two isotopically distinct CO2 components—atmospheric CO2 and CO2 from in situ oxidation of organic matter. The δ13C values measured for the Fe(CO3)OH component in solid solution in these Permian goethites are −13.5‰ for the Lower Leonardian (∼283 Ma BP) paleosol (MCGoeth) and −13.9‰ for the Upper Leonardian (∼270 Ma BP) paleosol (SAP). These goethites contain the most 13C-rich Fe(CO3)OH measured to date for pedogenic goethites crystallized in soils exhibiting mixing of the two aforementioned CO2 components. δ13C measured for 43 organic matter samples in the Lower Leonardian (Waggoner Ranch Fm.) has an average value of −20.3 ± 1.1‰ (1s). The average value yields a calculated Early Permian atmospheric Pco2 value of about 1 × PAL, but the scatter in the measured δ13C values of organic matter permits a calculated maximum Pco2 of 11 × PAL (PAL = present atmospheric level). Measured values of the mole fraction of Fe(CO3)OH in MCGoeth and SAP correspond to soil CO2 concentrations in the Early Permian paleosol profiles of 54,000 and 50,000 ppmV, respectively. Such high soil CO2 concentrations are similar to modern soils in warm, wet environments.The average δ13C values of pedogenic calcite from 9 paleosol profiles stratigraphically associated with MCGoeth (Waggoner Ranch Fm.) range from −6.5‰ to −4.4‰, with a mean δ13C value for all profiles of −5.4‰. Thus, the value of Δ13C between the pedogenic calcite data set and MCGoeth is 8.1 (±0.9)‰, which is in reasonable accord with the value of 7.7‰ expected if atmospheric Pco2 and organic matter δ13C values were the same for both paleosol types. Furthermore, the atmospheric Pco2 calculated for the Early Permian from the average measured carbon isotopic compositions of the paleosol calcite and organic matter is also analytically indistinguishable from 1 × PAL, with a maximum calculated atmospheric Pco2 (permitted by one standard deviation of the organic matter δ13C value) of ∼5 × PAL.If, however, measured average δ13C values of the plant organic matter are more positive than the original soil organic matter as a result of diagenetic loss of 13C-depleted, labile organic compounds, calculated Permian atmospheric Pco2 using these 13C-enriched organic values would underestimate the actual atmospheric Pco2 using either goethite or calcite. This is the first stratigraphically constrained, intrabasinal study to compare ancient atmospheric CO2 concentrations calculated from pedogenic goethite and calcite. These results demonstrate that the two different proxies record the same information about atmospheric CO2.The Fe(CO3)OH component in pedogenic goethite from a Triassic paleosol in Utah is significantly enriched in 13C relative to Fe(CO3)OH in goethites from soils in which there are mixtures of two isotopic CO2 components. Field-relationships and the δ13C value (−1.9‰) of the Triassic goethite indicate that this ancient paleosol profile experienced mixing of three isotopically distinct CO2 components at the time of goethite crystallization. The three components were probably atmospheric CO2, CO2 from in situ oxidation of organic matter and CO2 from in situ dissolution of preexisting calcite. Although mixing of three isotopically distinct CO2 components, as recorded by Fe(CO3)OH in goethite, has been described in modern soil, this is the first example from a documented paleosol. Its preservation affirms the need for careful, case-by-case assessment of ancient paleosols to establish that goethite in any particular soil is likely to be a valid proxy of atmospheric Pco2.  相似文献   

8.
Uptake of anthropogenic CO2 by the oceans is altering seawater chemistry with potentially serious consequences for coral reef ecosystems due to the reduction of seawater pH and aragonite saturation state (Ωarag). The objectives of this long-term study were to investigate the viability of two ecologically important reef-building coral species, massive Porites sp. and Stylophora pistillata, exposed to high pCO2 (or low pH) conditions and to observe possible changes in physiologically related parameters as well as skeletal isotopic composition. Fragments of Porites sp. and S. pistillata were kept for 6-14 months under controlled aquarium conditions characterized by normal and elevated pCO2 conditions, corresponding to pHT values of 8.09, 7.49, and 7.19, respectively. In contrast with shorter, and therefore more transient experiments, the long experimental timescale achieved in this study ensures complete equilibration and steady state with the experimental environment and guarantees that the data provide insights into viable and stably growing corals. During the experiments, all coral fragments survived and added new skeleton, even at seawater Ωarag < 1, implying that the coral skeleton is formed by mechanisms under strong biological control. Measurements of boron (B), carbon (C), and oxygen (O) isotopic composition of skeleton, C isotopic composition of coral tissue and symbiont zooxanthellae, along with physiological data (such as skeletal growth, tissue biomass, zooxanthellae cell density, and chlorophyll concentration) allow for a direct comparison with corals living under normal conditions and sampled simultaneously. Skeletal growth and zooxanthellae density were found to decrease, whereas coral tissue biomass (measured as protein concentration) and zooxanthellae chlorophyll concentrations increased under high pCO2 (low pH) conditions. Both species showed similar trends of δ11B depletion and δ18O enrichment under reduced pH, whereas the δ13C results imply species-specific metabolic response to high pCO2 conditions. The skeletal δ11B values plot above seawater δ11B vs. pH borate fractionation curves calculated using either the theoretically derived αB value of 1.0194 (Kakihana et al. (1977) Bull. Chem. Soc. Jpn.50, 158) or the empirical αB value of 1.0272 (Klochko et al. (2006) EPSL248, 261). However, the effective αB must be greater than 1.0200 in order to yield calculated coral skeletal δ11B values for pH conditions where Ωarag ? 1. The δ11B vs. pH offset from the seawater δ11B vs. pH fractionation curves suggests a change in the ratio of skeletal material laid down during dark and light calcification and/or an internal pH regulation, presumably controlled by ion-transport enzymes. Finally, seawater pH significantly influences skeletal δ13C and δ18O. This must be taken into consideration when reconstructing paleo-environmental conditions from coral skeletons.  相似文献   

9.
Soft corals and black corals are useful proxy tools for paleoceanographic reconstructions. However, most work has focused on deep-water taxa and few studies have used these corals as proxy organisms in shallow water (<200 m). To facilitate the use of stable nitrogen and carbon isotope (δ15N and δ13C) records from shallow-water soft coral and black coral taxa for paleoceanographic reconstructions, quantification of the inherent variability in skeletal isotope values between sites, across depth, and among taxa is needed. Here, skeletal δ15N and δ13C values were measured in multiple colonies from eleven genera of soft corals and two genera of black corals from across a depth transect (5-105 m) at two sites in Palau located in the tropical western Pacific Ocean. Overall, no difference in skeletal δ15N and δ13C values between sites was present. Skeletal δ15N values significantly increased and δ13C values decreased with depth. This is consistent with changes in isotope values of suspended particulate organic matter (POM) across the photic zone, suggesting that the primary food source to these corals is suspended POM and that the stable isotopic composition of POM controls the skeletal isotopic composition of these corals. Thus, to compare the isotope records of corals collected across a depth range in the photic zone, first order depth corrections of −0.013‰ m−1 and +0.023‰ m−1 are recommended for δ15N and δ13C, respectively. Average depth-corrected δ15N values were similar between black corals and soft corals, indicating that corals in these orders feed at a similar trophic level. In contrast, average depth-corrected δ13C values of black corals were significantly lower than that of soft corals, potentially resulting from metabolic processes associated with differing skeletal compositions among the orders (i.e., gorgonin vs. chitin based). Thus, a correction of +1.0‰ is recommended for black corals when comparing their δ13C-based proxy records to soft corals. After correcting for both the depth and order effects, variability in δ15N values among corals within each genera was low (standard deviation (SD) of the mean <±0.5‰), with the exception of Acanthorgorgia. The calculated SD of <±0.5‰ provides a first order guideline for the amount of variability that could be expected in a δ15N record, and suggests that these corals may be useful for δ15N-based paleoceanographic reconstructions. Variability in δ13C values among corals within genera was also low (standard deviation of the mean <±0.5‰) with the exception of Rhipidipathes and Villogorgia. Similar to δ15N, records from the genera studied here with the exception of Rhipidipathes and Villogorgia may be useful for δ13C-based paleoceanographic reconstructions. Overall, using the recommendations developed here, stable isotope records from multiple sites, depths and taxa of these corals can be more rigorously compared.  相似文献   

10.
The origin of δ13C variations within the skeletons of zooxanthellate scleractinian corals is still a matter of considerable debate. In particular, the role respired CO2 plays in controlling the eventual δ13C of the skeleton remains unclear. In this study, the temporal variability of the δ13C of respired CO2 produced by Montastraea faveolata has been measured at approximately monthly intervals over a 1-year period. In these experiments, three corals maintained on a platform at 8 m depth near Molasses Reef in the Florida Keys were incubated in closed chambers for 24-h periods and samples of the incubation water analyzed for the δ13C of the dissolved inorganic carbon (ΣCO2) at ∼3-h intervals. Throughout the incubation, the concentration of O2 was measured continuously within the chamber. Our results show that during daylight, the δ13C of the ΣCO2 in the incubation water becomes enriched in 13C as a result of fractionation during the fixation of C by photosynthesis, whereas at night the δ13C of the ΣCO2 becomes more negative. The δ13C of the respiratory CO2 ranges from −9‰ in the late spring to values as low as −17‰ in the autumn. The lighter values are significantly more negative than those reported by previous workers for coral tissue and zooxanthellae. An explanation for this discrepancy may be that the corals respire a significant proportion of isotopically negative substances, such as lipids, which are known to have values up to 10‰ lighter compared to the bulk δ13C of the tissue. The clear seasonal cycle in the δ13C of the respiratory CO2 suggests that there is also seasonal variability in either the δ13C of the coral tissue or the type and/or amount of organic material being respired. A similar temporal pattern and magnitude of change was observed in the δ13C of the coral tissue samples collected from a nearby reef at monthly intervals between 1995 and 1997. These patterns are similar in timing to the δ13C measured in the coral skeletons. We have also calculated an annual mean value for the fractionation factor between dissolved CO2 in the external environment and photosynthate fixed by the zooxanthellae of 1.0121 (±0.003). This value is inversely correlated with the ratio of photosynthesis to respiration (P/R) of the entire organism and shows the highest values during the summer months.  相似文献   

11.
Ocean acidification due to anthropogenic CO2 emissions is a dominant driver of long-term changes in pH in the open ocean, raising concern for the future of calcifying organisms, many of which are present in coastal habitats. However, changes in pH in coastal ecosystems result from a multitude of drivers, including impacts from watershed processes, nutrient inputs, and changes in ecosystem structure and metabolism. Interaction between ocean acidification due to anthropogenic CO2 emissions and the dynamic regional to local drivers of coastal ecosystems have resulted in complex regulation of pH in coastal waters. Changes in the watershed can, for example, lead to changes in alkalinity and CO2 fluxes that, together with metabolic processes and oceanic dynamics, yield high-magnitude decadal changes of up to 0.5 units in coastal pH. Metabolism results in strong diel to seasonal fluctuations in pH, with characteristic ranges of 0.3 pH units, with metabolically intense habitats exceeding this range on a daily basis. The intense variability and multiple, complex controls on pH implies that the concept of ocean acidification due to anthropogenic CO2 emissions cannot be transposed to coastal ecosystems directly. Furthermore, in coastal ecosystems, the detection of trends towards acidification is not trivial and the attribution of these changes to anthropogenic CO2 emissions is even more problematic. Coastal ecosystems may show acidification or basification, depending on the balance between the invasion of coastal waters by anthropogenic CO2, watershed export of alkalinity, organic matter and CO2, and changes in the balance between primary production, respiration and calcification rates in response to changes in nutrient inputs and losses of ecosystem components. Hence, we contend that ocean acidification from anthropogenic CO2 is largely an open-ocean syndrome and that a concept of anthropogenic impacts on marine pH, which is applicable across the entire ocean, from coastal to open-ocean environments, provides a superior framework to consider the multiple components of the anthropogenic perturbation of marine pH trajectories. The concept of anthropogenic impacts on seawater pH acknowledges that a regional focus is necessary to predict future trajectories in the pH of coastal waters and points at opportunities to manage these trajectories locally to conserve coastal organisms vulnerable to ocean acidification.  相似文献   

12.
Oxygen isotopes of goethite from ferricrete deposits were measured from both northern and southern Rocky Mountain localities to assess geographic variability in regional Holocene paleoclimate change. A ∼3.7‰ increase in oxygen isotope values of 14C-dated goethites in the northern Rocky Mountains suggests a regional-scale relative increase in amounts of isotopically heavy summer precipitation since the early Holocene. In contrast, oxygen isotope values from the southern Rocky Mountains increase abruptly ∼2.1‰ at ∼6200 14C yr B.P., then decrease ∼2.4‰ between ∼2000 14C yr B.P. and the present. We interpret this period of relatively high δ18O values as evidence for a middle Holocene warm period combined with a relatively strong summer monsoon. These variable climate records suggest that the Rocky Mountains of the western United States have had a spatially heterogeneous Holocene climate history.  相似文献   

13.
Here we calibrate the carbonate clumped isotope thermometer in modern deep-sea corals. We examined 11 specimens of three species of deep-sea corals and one species of a surface coral spanning a total range in growth temperature of 2-25 °C. External standard errors for individual measurements ranged from 0.005‰ to 0.011‰ (average: 0.0074‰) which corresponds to ∼1-2 °C. External standard errors for replicate measurements of Δ47 in corals ranged from 0.002‰ to 0.014‰ (average: 0.0072‰) which corresponds to 0.4-2.8 °C. We find that skeletal carbonate from deep-sea corals shows the same relationship of Δ47 (the measure of 13C-18O ordering) to temperature as does inorganic calcite. In contrast, the δ13 C and δ18O values of these carbonates (measured simultaneously with Δ47 for every sample) differ markedly from equilibrium with seawater; i.e., these samples exhibit pronounced ‘vital effects’ in their bulk isotopic compositions. We explore several reasons why the clumped isotope compositions of deep-sea coral skeletons exhibit no evidence of a vital effect despite having large conventional isotopic vital effects.  相似文献   

14.
Pagani et al. [Pagani M., Lemarchand D., Spivack A., and Gaillardet J. (2005). A critical evaluation of the boron isotope-pH proxy: the accuracy of ancient ocean pH estimates. Geochim. Cosmochim. Acta69(4), 953-961] use data from previous boron isotope studies to suggest that the fractionation between boric acid and borate in seawater as well as the history of δ11B in seawater are poorly understood, thus limiting our ability to capture realistic ocean pH with this proxy. Although we agree with the authors that the long recognized uncertainty in the secular variation of δ11Bseawater imposes a temporal limit on paleo-pH reconstructions, their evaluation of the δ11B/pH relationship in carbonates is flawed. Potential complications from vital, temperature and dissolution effects reported in that paper are based on studies that are experimentally and/or analytically poorly constrained. Using published validation studies we will demonstrate that many of the problems outlined by Pagani et al. have already been addressed, or are based on misinterpretations of previous work. Most importantly, statistical evaluation suggests empirical data are best described by a fractionation of ∼20‰. Recent paleoreconstructions confirm that the boron isotope proxy can be used with confidence, if sample selection and analyses are done carefully.  相似文献   

15.
Laboratory experiments on the branching, symbiont-bearing coral genus Porites and Acropora have been carried out to determine the dependence of the skeletal boron isotopic composition (δ11B) on the pH of seawater. The results show a clear relationship similar to previously established empirical calibrations for planktonic foraminifera and inorganic calcite. A −0.6‰ offset exists between P. cylindrica and A. nobilis which is systematic over the pH range of 7.7-8.2. To test whether the δ11B of coral skeletons changes with physiological processes such as photosynthesis and respiration, corals were grown along a depth transect in their natural environment and under controlled conditions in the laboratory at varying light intensities and food supply. Although we also observe an isotopic offset between P. compressa and Montipora verrucosa, neither experimental treatment systematically changed the δ11B of the two species. These findings are encouraging for using the boron isotope paleo-pH proxy in corals, because it appears that seawater pH is the dominant control on the boron isotopic composition in corals.  相似文献   

16.
Measured mole fractions (X) and δ13C values of the Fe(CO3)OH component in pedogenic goethite from a mid-latitude Oxisol of Early Eocene age (≈52 Ma B.P.) range from 0.0014 to 0.0064 and −20.1 to −15.4‰, respectively. These values of X imply that concentrations of CO2 gas in the paleosol were ≈7400 to ≈34,000 ppm. δ13C and 1/X are correlated and define a linear, soil-CO2 diffusive mixing line with a positive slope. Such positive slopes are characteristic of mixing of two isotopically distinct CO2 endmembers (atmospheric CO2 and CO2 from oxidation of soil organic matter). From the intercept of the mixing line, it is calculated that the δ 13C value of organic matter in the ancient soil was ≈−28.0‰. The magnitude of the slope implies an Early Eocene atmospheric CO2 concentration of ≈2700 ppm.A simple model for forest soils suggests that a “canopy effect” may cause atmospheric CO2 concentrations deduced from pedogenic minerals to underestimate the actual concentrations of atmospheric CO2. If a significant forest canopy were present at the time of formation of pedogenic goethite in the Ione Fm, the concentration of 2700 ppm calculated for atmospheric CO2 could be slightly low, but the underestimate is expected to be < ≈300 ppm (i.e., less than the analytical uncertainty). The relatively high concentration of 2700 ppm inferred for atmospheric CO2 at ≈52 Ma B.P. would have been coincident with the Early Eocene climatic optimum. This result seems to support the case for an important role for variations of atmospheric CO2 in the modification of global paleoclimate.  相似文献   

17.
We have developed a quantitative model of CO2 and H2O isotopic mixing between magmatic and hydrothermal gases for the fumarolic emissions of the La Fossa crater (Vulcano Island, Italy). On the basis of isotope balance equations, the model takes into account the isotope equilibrium between H2O and CO2 and extends the recent model of chemical and energy two-end-member mixing by Nuccio et al. (1999). As a result, the H2O and CO2 content and the δD, δ18O, and δ13C isotope compositions for both magmatic and hydrothermal end-members have been assessed. Low contributions of meteoric steam, added at a shallow depth, have been also recognized and quantified in the fumaroles throughout the period from 1988 to 1998. Nonequilibrium oxygen isotope exchange also seems to be occurring between ascending gases and wall rocks along some fumarolic conduits.The δ13CCO2 of the magmatic gases varies around −3 to 1‰ vs. Peedee belemnite (PDB), following a perfect synchronism with the variations of the CO2 concentration in the magmatic gases. This suggests a process of isotope fractionation because of vapor exsolution caused by magma depressurization. The hydrogen isotopes in the magmatic gases (−1 to −‰ vs. standard mean ocean water [SMOW]), as well as the above δ13CCO2 value, are coherent with a convergent tectonic setting of magma generation, where the local mantle is widely contaminated by fluids released from the subducted slab. Magma contamination in the crust probably amplifies this effect.The computed isotope composition of carbon and hydrogen in the hydrothermal vapors has been used to calculate the δD and δ13C of the entire hydrothermal system, including mixed H2O-CO2 vapor, liquid water, and dissolved carbon. We have computed values of about 10‰ vs. SMOW for water and −2 to −6.5‰ vs. PDB for CO2. On these grounds, we think that Mediterranean marine water (δDH2O ≈ 10‰) feeds the hydrothermal system. It infiltrates at depth throughout the local rocks, reaching oxygen isotope equilibrium at high temperatures. Interaction processes between magmatic gases and the evolving seawater also seem to occur, causing the dissolution of isotopically fractionated aqueous CO2 and providing the source for hydrothermal carbon. These results have important implications concerning fluid circulation beneath Vulcano and address the more convenient routine of geochemical surveillance.  相似文献   

18.
The isotopic composition of fossil fuels is an important component of many studies of C sources and sinks based on atmospheric measurements of CO2. In C budget studies, the isotopic composition of crude petroleum and CH4 are often used as a proxy for the isotopic composition of CO2 emissions from combustion. In this study, the C isotope composition (δ13C) of exhaust from the major fossil fuel emission sources in Salt Lake City, USA, was characterized with 159 measurements of vehicle exhaust of various types and eight measurements of residential furnace exhaust. These two sources were found to be isotopically distinct, and differed from global-scale estimates based on average values for crude petroleum and CH4. Vehicle-specific factors such as engine load and operation time had no effect on δ13C of vehicle exhaust. A small difference was found between the mean δ13C of vehicle exhaust collected randomly from different vehicles and the mean δ13C of gasoline collected from multiple fueling stations representing major gasoline distributors in Salt Lake City and the surrounding area. However, a paired comparison of δ13C of exhaust and gasoline for six different vehicles did not show any consistent C isotope fractionation during vehicle combustion. The mean δ13C of crude petroleum processed for local distribution differed slightly from refined gasoline collected at multiple fueling stations, but time lags between processing and transportation cannot be ruled out as an uncontrollable contributing factor. Measured isotope ratios were then combined with fuel consumption statistics to predict the annual cycle of δ13C of fossil fuel emissions for the Salt Lake City metropolitan area. The results showed that the isotopic composition of CO2 emissions from fossil fuel combustion varied by almost 3‰ over the course of the 2002 calendar year. This study illustrates that on a regional scale, the isotopic composition of fossil fuel emissions shows a high degree of both spatial and temporal variability that may influence characterization of C sources and sinks with atmospheric measurements.  相似文献   

19.
We investigated the Sea-Rain-Lake relation during the Last Glacial-Holocene in the East Mediterranean region by comparing the δ18O and δ13C records of authigenic aragonite deposited in Lake Lisan, the Dead Sea, Mediterranean foraminifera, and speleothems. The Lisan Formation data display long- and short-term variations of δ18O, representing steady-state conditions of the lake (e.g., 5.6‰ ± 0.5‰ and 4.5‰ ± 1‰ in the Upper and Lower Members of the Lisan Formation, respectively), and short-term excursions reflecting large floods and droughts. The long-term (steady-state) δ18O values of the Lisan aragonites show similarity to the corresponding time-equivalent records of the Eastern Mediterranean foraminifera and Judea Mountain speleothems: The Last Glacial deposits are in all of them 2‰-3‰ heavier than the Holocene ones. We interpret this similarity as reflecting the significance of the source effect on the long-term behavior of isotopic reservoirs: Speleothem δ18O is strongly influenced by the marine reservoir that contributes its vapor to rain formation; the lake δ18O is dominated by the composition of the inflowing water. Short-term variations in the isotopic composition of rainfall are dominated by the amount effect and the temperature and those of the Lake’s upper water mass by the lake’s water balance.δ13C values are more variable than δ18O in the same Lisan sequences (e.g., δ13C in the Lower Member is 1.0‰ ± 1.7‰, whereas δ18O is 4.6‰ ± 0.7‰) and are 1‰ to 1.5‰ higher in the Upper Member than in the Lower and Middle Members of the Lisan Formation. These variations reflect significant increase in primary productivity of the lake and algal bloom activity. It appears that the hypersaline-saline lakes were not as “dead” as the Dead Sea is and that algal activity had an important impact upon the geochemistry of Lake Lisan.The δ18O data combined with independent geochemical and limnologic information (e.g., level fluctuations) indicate that Lisan time was characterized by high precipitation-high lake stands-high atmospheric humidity, whereas the Holocene Dead Sea shows the opposite behavior. This paleoclimatic reconstruction is consistent with independent evidence for significantly wetter conditions in the East Mediterranean region during the Last Glacial period.  相似文献   

20.
The budget of atmospheric CO2 is widely studied using records of temporal and spatial variations of concentrations, δ13C and δ18O values. However, the number and diversity of sources and sinks prevents these alone from fully constraining the budget. Molecules containing two rare isotopes can serve as additional tracers and potentially provide additional, independent, constraints. We present data documenting seasonal and diurnal variations of CO2 having a mass of 47 u (mostly 13C18O16O) in air from Pasadena, CA. We report these data using the ‘mass 47 anomaly’ (Δ47), which is defined as the deviation of R47(=[47]/[44]) from that expected for a random distribution of isotopologues. Between February 2004 and December 2005, Δ47 showed a seasonal pattern that differed significantly from that expected based on thermodynamic equilibrium. During the year 2004 Δ47 was 0.76‰ in winter, increased to 0.87‰ in summer and gradually decreased through the autumn to 0.81‰ at the end of the year. Δ47 then increased again through the winter and spring of 2005 to 0.97‰ in summer followed by a decrease to 0.88‰ at the end of 2005. The seasonal variations cannot be accounted for by variations in the relative contribution of local fossil fuel sources. Diurnal variations were the combined effect of both fuel combustion and respiration having Δ47 values of 0.41‰ and ca. 0.77‰, respectively. The seasonal cycle may be interpreted as a competition between low Δ47 values in respiration and higher Δ47 values resulting from CO2-water exchange in photosynthesis.  相似文献   

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