| 1. |
- Naafs, B. D. A., et al.
(author)
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Introducing global peat-specific temperature and pH calibrations based on brGDGT bacterial lipids
- 2017
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In: Geochimica et Cosmochimica Acta. - : PERGAMON-ELSEVIER SCIENCE LTD. - 0016-7037 .- 1872-9533. ; 208, s. 285-301
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Journal article (peer-reviewed)abstract
- Glycerol dialkyl glycerol tetraethers (GDGTs) are membrane-spanning lipids from Bacteria and Archaea that are ubiquitous in a range of natural archives and especially abundant in peat. Previous work demonstrated that the distribution of bacterial branched GDGTs (brGDGTs) in mineral soils is correlated to environmental factors such as mean annual air temperature (MAAT) and soil pH. However, the influence of these parameters on brGDGT distributions in peat is largely unknown. Here we investigate the distribution of brGDGTs in 470 samples from 96 peatlands around the world with a broad mean annual air temperature (-8 to 27 degrees C) and pH (3-8) range and present the first peat-specific brGDGT-based temperature and pH calibrations. Our results demonstrate that the degree of cyclisation of brGDGTs in peat is positively correlated with pH, pH = 2.49 x CBTpeat + 8.07 (n = 51, R-2 = 0.58, RMSE = 0.8) and the degree of methylation of brGDGTs is positively correlated with MAAT, MAAT(peat) (degrees C) = 52.18 x MBT'(5me) - 23.05 (n = 96, R-2 = 0.76, RMSE = 4.7 degrees C). These peat-specific calibrations are distinct from the available mineral soil calibrations. In light of the error in the temperature calibration (similar to 4.7 degrees C), we urge caution in any application to reconstruct late Holocene climate variability, where the climatic signals are relatively small, and the duration of excursions could be brief. Instead, these proxies are well-suited to reconstruct large amplitude, longer-term shifts in climate such as deglacial transitions. Indeed, when applied to a peat deposit spanning the late glacial period (similar to 15.2 kyr), we demonstrate that MAAT(peat) yields absolute temperatures and relative temperature changes that are consistent with those from other proxies. In addition, the application of MAAT(peat) to fossil peat (i.e. lignites) has the potential to reconstruct terrestrial climate during the Cenozoic. We conclude that there is clear potential to use brGDGTs in peats and lignites to reconstruct past terrestrial climate.
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| 2. |
- Bosch, Carme, et al.
(author)
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Source Apportionment of Polycyclic Aromatic Hydrocarbons in Central European Soils with Compound-Specific Triple Isotopes (delta C-13, Delta C-14, and delta H-2)
- 2015
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In: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 49:13, s. 7657-7665
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Journal article (peer-reviewed)abstract
- This paper reports the first study applying a triple-isotope approach for source apportionment of polycyclic aromatic hydrocarbons (PAHs). The C-13/C-12, and H-2/H-1 isotope ratios of PAHs were determined in forest soils from mountainous areas of the Czech Republic, European Union. Statistical modeling applying a Bayesian Markov chain Monte Carlo (MCMC) framework to the environmental triple isotope PAR data and an end-member PAR isotope database allowed comprehensive accounting of uncertainties and quantitative constraints on the PAR sources among biomass combustion, liquid fossil fuel combustion, and coal combustion at low and high temperatures. The results suggest that PAHs in this central European region had a clear predominance of coal combustion sources (75 +/- 6%; uncertainties represent 1 SD), mainly coal pyrolysis at low temperature (similar to 650 degrees C; 61 +/- 8%). Combustion of liquid fossil fuels and biomass represented 16 +/- 3 and 9 + 3% of the total PAR burden (Sigma PAH(14)), respectively. Although some soils were located close to potential PAR point sources, the source distribution was within a narrow range throughout the region. These observation-based top-down constraints on sources of environmental PARS provide a reference for both improved bottom-up emission inventories and guidance for efforts to mitigate PAR emissions.
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| 3. |
- Inglis, Gordon N., et al.
(author)
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Global mean surface temperature and climate sensitivity of the early Eocene Climatic Optimum (EECO), Paleocene-Eocene Thermal Maximum (PETM), and latest Paleocene
- 2020
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In: Climate of the Past. - : Copernicus GmbH. - 1814-9324 .- 1814-9332. ; 16:5, s. 1953-1968
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Journal article (peer-reviewed)abstract
- Accurate estimates of past global mean surface temperature (GMST) help to contextualise future climate change and are required to estimate the sensitivity of the climate system to CO2 forcing through Earth's history. Previous GMST estimates for the latest Paleocene and early Eocene (similar to 57 to 48 million years ago) span a wide range (similar to 9 to 23 degrees C higher than pre-industrial) and prevent an accurate assessment of climate sensitivity during this extreme greenhouse climate interval. Using the most recent data compilations, we employ a multi-method experimen- tal framework to calculate GMST during the three DeepMIP target intervals: (1) the latest Paleocene (similar to 57 Ma), (2) the Paleocene-Eocene Thermal Maximum (PETM; 56 Ma), and (3) the early Eocene Climatic Optimum (EECO; 53.3 to 49.1 Ma). Using six different methodologies, we find that the average GMST estimate (66% confidence) during the latest Paleocene, PETM, and EECO was 26.3 degrees C (22.3 to 28.3 degrees C), 31.6 degrees C (27.2 to 34.5 degrees C), and 27.0 degrees C (23.2 to 29.7 degrees C), respectively. GMST estimates from the EECO are similar to 10 to 16 degrees C warmer than pre-industrial, higher than the estimate given by the Intergovernmental Panel on Climate Change (IPCC) 5th Assessment Report (9 to 14 degrees C higher than pre-industrial). Leveraging the large signal associated with these extreme warm climates, we combine estimates of GMST and CO2 from the latest Paleocene, PETM, and EECO to calculate gross estimates of the average climate sensitivity between the early Paleogene and today. We demonstrate that bulk equilibrium climate sensitivity (ECS; 66% confidence) during the latest Paleocene, PETM, and EECO is 4.5 degrees C (2.4 to 6.8 degrees C), 3.6 degrees C (2.3 to 4.7 degrees C), and 3.1 degrees C (1.8 to 4.4 degrees C) per doubling of CO2. These values are generally similar to those assessed by the IPCC (1.5 to 4.5 ffiC per doubling CO2) but appear incompatible with low ECS values (< 1 :5 per doubling CO2).
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| 4. |
- Schouten, Stefan, et al.
(author)
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An interlaboratory study of TEX86 and BIT analysis of sediments, extracts, and standard mixtures
- 2013
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In: Geochemistry Geophysics Geosystems. - 1525-2027. ; 14:12, s. 5263-5285
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Journal article (peer-reviewed)abstract
- Two commonly used proxies based on the distribution of glycerol dialkyl glycerol tetraethers (GDGTs) are the TEX86 (TetraEther indeX of 86 carbon atoms) paleothermometer for sea surface temperature reconstructions and the BIT (Branched Isoprenoid Tetraether) index for reconstructing soil organic matter input to the ocean. An initial round-robin study of two sediment extracts, in which 15 laboratories participated, showed relatively consistent TEX86 values (reproducibility +/- 3-4 degrees C when translated to temperature) but a large spread in BIT measurements (reproducibility +/- 0.41 on a scale of 0-1). Here we report results of a second round-robin study with 35 laboratories in which three sediments, one sediment extract, and two mixtures of pure, isolated GDGTs were analyzed. The results for TEX86 and BIT index showed improvement compared to the previous round-robin study. The reproducibility, indicating interlaboratory variation, of TEX86 values ranged from 1.3 to 3.0 degrees C when translated to temperature. These results are similar to those of other temperature proxies used in paleoceanography. Comparison of the results obtained from one of the three sediments showed that TEX86 and BIT indices are not significantly affected by interlaboratory differences in sediment extraction techniques. BIT values of the sediments and extracts were at the extremes of the index with values close to 0 or 1, and showed good reproducibility (ranging from 0.013 to 0.042). However, the measured BIT values for the two GDGT mixtures, with known molar ratios of crenarchaeol and branched GDGTs, had intermediate BIT values and showed poor reproducibility and a large overestimation of the true (i.e., molar-based) BIT index. The latter is likely due to, among other factors, the higher mass spectrometric response of branched GDGTs compared to crenarchaeol, which also varies among mass spectrometers. Correction for this different mass spectrometric response showed a considerable improvement in the reproducibility of BIT index measurements among laboratories, as well as a substantially improved estimation of molar-based BIT values. This suggests that standard mixtures should be used in order to obtain consistent, and molar-based, BIT values.
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| 5. |
- Wiegert, Charline, 1980-, et al.
(author)
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Carbon and Chlorine Isotope Fractionation During Microbial Degradation of Tetra- and Trichloroethene
- 2013
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In: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 47:12, s. 6449-6456
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Journal article (peer-reviewed)abstract
- Two-dimensional compound-specific isotope analysis (2D-CSIA), combining stable carbon and chlorine isotopes, holds potential for monitoring of natural attenuation of chlorinated ethenes (CEs), in contaminated soil and groundwater. However, interpretation of 2D-CSIA data sets is challenged by a shortage of experimental Cl isotope enrichment factors. Here, isotope enrichments factors for C and Cl (i.e., epsilon(C) and epsilon(Cl)) were determined for biodegradation of tetrachloroethene (PCE) and trichloroethene (TCE) using microbial enrichment cultures from a heavily CE-contaminated aquifer. The obtained values were epsilon(C) = -5.6 +/- 0.7 parts per thousand (95% CI) and epsilon(Cl) = -2.0 +/- 0.5 parts per thousand for PCE degradation and epsilon(C) = -8.8 +/- 0.2 parts per thousand and epsilon(Cl) = -3.5 +/- 0.5 parts per thousand for TCE degradation. Combining the values for both epsilon(C) and epsilon(Cl) yielded mechanism-diagnostic epsilon(Cl)/epsilon(C) ratios of 0.35 +/- 0.11 and 0.37 +/- 0.11 degradation of PCE and TCE, respectively. Application of the obtained epsilon(C) and epsilon(Cl) values to a previously investigated field site gave similar estimates for the fraction of degraded contaminant as in the previous study, but with a reduced uncertainty in assessment of the natural attenuation. Furthermore, 16S rRNA gene clone library analyses were performed on three samples from the PCE degradation experiments. A species closely related to Desulfitobacterium aromaticivorans UKTL dominated the reductive dechlorination process. This study contributes to the development of 2D-CSIA as a tool for evaluating remediation strategies of CEs at contaminated sites.
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| 6. |
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| 7. |
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| 8. |
- Wiegert, Charline, 1980-, et al.
(author)
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Dual carbon chlorine stable isotope investigation of sources and fate of chlorinated ethenes in contaminated groundwater
- 2012
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In: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 46:20, s. 10918-10925
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Journal article (peer-reviewed)abstract
- Chlorinated ethenes (CEs) are ubiquitous groundwater contaminants, yet there remains a need for a method to efficiently monitor their in situ degradation. We report here the first field application of combined stable carbon and chlorine isotope analysis of tetrachloroethene (PCE) and trichloroethene (TCE) to investigate their biodegradation in a heavily contaminated aquifer. The two-dimensional Compound Specific Isotope Analysis (2D-CSIA) approach was facilitated by a recently developed gas chromatography-quadrupole mass spectrometry (GCqMS) method for delta Cl-37 determination. Both C and Cl isotopes showed evidence of ongoing PCE transformation. Applying published C isotope enrichment factors (epsilon(C)) enabled evaluation of the extent of in situ PCE degradation (11-78%). We interpreted C and Cl isotopes using a numerical reactive transport model along a 60-m flow path. It revealed that combined PCE and TCE mass load was dechlorinated by less than 10%, and that cis-dichloroethene was not further dechlorinated. Furthermore, the 2D-CSIA approach allowed estimation of Cl isotope enrichment factors epsilon(Cl) (-7.8 to -0.8 parts per thousand) and characteristic epsilon(Cl)/epsilon(C) values (0.42-1.12) for reductive PCE dechlorination at this field site. This investigation demonstrates the benefit of 2D-CSIA to assess in situ degradation of CEs and the applicability of Cl isotope fractionation to evaluate PCE and TCE dechlorination.
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