| 1. |
- Bosch, Carme, et al.
(författare)
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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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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 49:13, s. 7657-7665
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Tidskriftsartikel (refereegranskat)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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| 2. |
- Wiegert, Charline, 1980-, et al.
(författare)
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Carbon and Chlorine Isotope Fractionation During Microbial Degradation of Tetra- and Trichloroethene
- 2013
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 47:12, s. 6449-6456
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Tidskriftsartikel (refereegranskat)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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| 3. |
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| 4. |
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| 5. |
- Wiegert, Charline, 1980-, et al.
(författare)
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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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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 46:20, s. 10918-10925
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Tidskriftsartikel (refereegranskat)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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| 6. |
- Brehm, Nicolas, et al.
(författare)
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Tree-rings reveal two strong solar proton events in 7176 and 5259 BCE
- 2022
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 13:1
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Tidskriftsartikel (refereegranskat)abstract
- The Sun sporadically produces eruptive events leading to intense fluxes of solar energetic particles (SEPs) that dramatically disrupt the near-Earth radiation environment. Such events have been directly studied for the last decades but little is known about the occurrence and magnitude of rare, extreme SEP events. Presently, a few events that produced measurable signals in cosmogenic radionuclides such as 14C, 10Be and 36Cl have been found. Analyzing annual 14C concentrations in tree-rings from Switzerland, Germany, Ireland, Russia, and the USA we discovered two spikes in atmospheric 14C occurring in 7176 and 5259 BCE. The ~2% increases of atmospheric 14C recorded for both events exceed all previously known 14C peaks but after correction for the geomagnetic field, they are comparable to the largest event of this type discovered so far at 775 CE. These strong events serve as accurate time markers for the synchronization with floating tree-ring and ice core records and provide critical information on the previous occurrence of extreme solar events which may threaten modern infrastructure.
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| 8. |
- Naafs, B. D. A., et al.
(författare)
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Introducing global peat-specific temperature and pH calibrations based on brGDGT bacterial lipids
- 2017
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Ingår i: Geochimica et Cosmochimica Acta. - : PERGAMON-ELSEVIER SCIENCE LTD. - 0016-7037 .- 1872-9533. ; 208, s. 285-301
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Tidskriftsartikel (refereegranskat)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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| 9. |
- Webb, Emily C., et al.
(författare)
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Compound-specific amino acid isotopic proxies for detecting freshwater resource consumption
- 2015
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Ingår i: Journal of Archaeological Science. - : Elsevier BV. - 0305-4403 .- 1095-9238. ; 63, s. 104-114
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Tidskriftsartikel (refereegranskat)abstract
- Of central importance to palaeodietary reconstruction is a clear understanding of relative contributions of different terrestrial (i.e., C3 vs. C4 plants) and aquatic (i.e., freshwater vs. marine) resources to human diet. There are, however, significant limitations associated with the ability to reconstruct palaeodiet using bulk collagen stable isotope compositions in regions where diverse dietary resources are available. Recent research has determined that carbon-isotope analysis of individual amino acids has considerable potential to elucidate dietary protein source where bulk isotopic compositions cannot. Using δ13CAA values for human and faunal remains from Zvejnieki, Latvia (8th – 3rd millennia BCE), we test several isotopic proxies focused on distinguishing freshwater protein consumption from both plant-derived and marine protein consumption. We determined that the Δ13CGly-Phe and Δ13CVal-Phe proxies can effectively discriminate between terrestrial and aquatic resource consumption, and the relationship between essential δ13CAA values and the Δ13CGly-Phe and Δ13CVal-Phe proxies can differentiate among the four protein consumption groups tested here. Compound-specific amino acid carbon-isotope dietary proxies thus enable an enhanced understanding of diet and resource exploitation in the past, and can elucidate complex dietary behaviour.
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| 10. |
- Webb, Emily C., et al.
(författare)
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Compound-specific amino acid isotopic proxies for distinguishing between terrestrial and aquatic resource consumption
- 2018
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Ingår i: Archaeological and Anthropological Sciences. - : Springer Science and Business Media LLC. - 1866-9557 .- 1866-9565. ; 10:1, s. 1-18
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Tidskriftsartikel (refereegranskat)abstract
- Compound-specific amino acid carbon-isotope compositions have shown particular promise for elucidating dietary behaviors in complex environmental contexts, and may also be able to mitigate the effect of many of the limitations inherent to palaeodietary reconstructions. Here, we investigate the efficacy of compound-specific amino acid isotopic proxies in characterizing the consumption of different dietary protein sources using amino acid carbon-isotope compositions for humans and fauna from Rössberga (Early to Middle Neolithic), Köpingsvik (Mesolithic and Middle Neolithic), and Visby (Medieval Period), Sweden. We also assess the explanatory capabilities of an isotopic mixing model when used with essential amino acid carbon-isotope compositions of humans and local fauna. All three isotopic proxies distinguished among humans from the three sites consistently and informatively, and were able to enhance the broad interpretations made using bulk isotopic compositions. The mixing model palaeodietary reconstruction revealed considerable diversity in relative protein source contributions among individuals at both Köpingsvik and Visby. Comparing the mixing model for bulk carbon- and nitrogen-isotope compositions to the model for essential amino acid isotopic compositions further demonstrated the likelihood of underestimation and overestimation of marine protein consumption for both aquatic-dominant and mixed marine-terrestrial diets when using bulk isotopic compositions.
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