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  • 1
    Publication Date: 2014-06-25
    Description: wo 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°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°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.
    Repository Name: EPIC Alfred Wegener Institut
    Type: Article , isiRev
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  • 2
    Publication Date: 2022-05-25
    Description: © The Author(s), 2015. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Biogeosciences 12 (2015): 4841-4860, doi:10.5194/bg-12-4841-2015.
    Description: Hydrolyzable organic carbon (OC) comprises a significant component of sedimentary particulate matter transferred from land into oceans via rivers. Its abundance and nature are however not well studied in Arctic river systems, and yet may represent an important pool of carbon whose fate remains unclear in the context of mobilization and related processes associated with a changing climate. Here, we examine the molecular composition and source of hydrolyzable compounds isolated from sedimentary particles derived from nine rivers across the pan-Arctic. Bound fatty acids (b-FAs), hydroxy FAs, n-alkane-α,ω-dioic acids (DAs) and phenols were the major components released upon hydrolysis of these sediments. Among them, b-FAs received considerable inputs from bacterial and/or algal sources, whereas ω-hydroxy FAs, mid-chain substituted acids, DAs, and hydrolyzable phenols were mainly derived from cutin and suberin of higher plants. We further compared the distribution and fate of suberin- and cutin-derived compounds with those of other terrestrial biomarkers (plant wax lipids and lignin phenols) from the same Arctic river sedimentary particles and conducted a benchmark assessment of several biomarker-based indicators of OC source and extent of degradation. While suberin-specific biomarkers were positively correlated with plant-derived high-molecular-weight (HMW) FAs, lignin phenols were correlated with cutin-derived compounds. These correlations suggest that, similar to leaf-derived cutin, lignin was mainly derived from litter and surface soil horizons, whereas suberin and HMW FAs incorporated significant inputs from belowground sources (roots and deeper soil). This conclusion is supported by the negative correlation between lignin phenols and the ratio of suberin-to-cutin biomarkers. Furthermore, the molecular composition of investigated biomarkers differed between Eurasian and North American Arctic rivers: while lignin dominated in the terrestrial OC of Eurasian river sediments, hydrolyzable OC represented a much larger fraction in the sedimentary particles from Colville River. Hence, studies exclusively focusing on either plant wax lipids or lignin phenols will not be able to fully unravel the mobilization and fate of bound OC in Arctic rivers. More comprehensive, multi-molecular investigations are needed to better constrain the land–ocean transfer of carbon in the changing Arctic, including further research on the degradation and transfer of both free and bound components in Arctic river sediments.
    Description: X. Feng acknowledges support from the Chinese National Key Development Program for Basic Research (2014CB954003, 2015CB954201). The ISSS program is supported by the Knut and Alice Wallenberg Foundation, headquarters of the Russian Academy of Sciences, the Swedish Research Council, the US National Oceanic and Atmospheric Administration, the Russian Foundation of Basic Research (#13-05-12028, 13-05-12041), the Swedish Polar Research Secretariat and the Nordic Council of Ministers (Arctic Co-Op and TRI-DEFROST programs). Collection of the Mackenzie sediment samples was supported by Fisheries and Oceans Canada and Indian and Northern Affairs Canada as part of the NOGAP B.6 project. Ö. Gustafsson acknowledges an Academy Research Fellow grant from the Swedish Royal Academy of Sciences. I. P. Semiletov and O. V. Dudarev thank the Government of the Russian Federation (#2013-220-04-157) for support as well as A. I. Khanchuk personally. T. I. Eglinton acknowledges support from Swiss National Science foundation (SNF) grant no. 200021_140850, and grants OCE-9907129, OCE-0137005, and OCE-0526268 from the US National Science Foundation (NSF), the Stanley Watson Chair for Excellence in Oceanography, and ETH Zurich. J. E. Vonk is thankful for support from NWO Rubicon (#825.10.022) and Veni (#863.12.004). B. E. van Dongen is thankful for support from the UK NERC (NE/I024798/1). R. M. Holmes acknowledges support from NSF 0436118, NSF 0732555, and NSF 1107774. X. Feng thanks WHOI for a postdoctoral scholar fellowship and for postdoctoral support from ETH Zurich.
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 3
    Publication Date: 2022-05-25
    Description: Author Posting. © American Geophysical Union, 2015. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Global Biogeochemical Cycles 29 (2015): 1855–1873, doi:10.1002/2015GB005204.
    Description: Distinguishing the sources, ages, and fate of various terrestrial organic carbon (OC) pools mobilized from heterogeneous Arctic landscapes is key to assessing climatic impacts on the fluvial release of carbon from permafrost. Through molecular 14C measurements, including novel analyses of suberin- and/or cutin-derived diacids (DAs) and hydroxy fatty acids (FAs), we compared the radiocarbon characteristics of a comprehensive suite of terrestrial markers (including plant wax lipids, cutin, suberin, lignin, and hydroxy phenols) in the sedimentary particles from nine major arctic and subarctic rivers in order to establish a benchmark assessment of the mobilization patterns of terrestrial OC pools across the pan-Arctic. Terrestrial lipids, including suberin-derived longer-chain DAs (C24,26,28), plant wax FAs (C24,26,28), and n-alkanes (C27,29,31), incorporated significant inputs of aged carbon, presumably from deeper soil horizons. Mobilization and translocation of these “old” terrestrial carbon components was dependent on nonlinear processes associated with permafrost distributions. By contrast, shorter-chain (C16,18) DAs and lignin phenols (as well as hydroxy phenols in rivers outside eastern Eurasian Arctic) were much more enriched in 14C, suggesting incorporation of relatively young carbon supplied by runoff processes from recent vegetation debris and surface layers. Furthermore, the radiocarbon content of terrestrial markers is heavily influenced by specific OC sources and degradation status. Overall, multitracer molecular 14C analysis sheds new light on the mobilization of terrestrial OC from arctic watersheds. Our findings of distinct ages for various terrestrial carbon components may aid in elucidating fate of different terrestrial OC pools in the face of increasing arctic permafrost thaw.
    Description: Chinese National Key Development Program for Basic Research Grant Numbers: 2014CB954003, 2015CB954201; Knut and Alice Wallenberg Foundation; Headquarters of the Russian Academy of Sciences; Swedish Research Council; US National Oceanic and Atmospheric Administration; Russian Foundation of Basic Research Grant Numbers: (13-05-12028, 13-05-12041; Swedish Polar Research Secretariat; Nordic Council of Ministers; Government of the Russian Federation Grant Number: 2013-220-04-157; Swiss National Science foundation. Grant Number: (200021_140850 US National Science Foundation (NSF) Grant Numbers: OCE-9907129, OCE-0137005, OCE-0526268; Stanley Watson Chair for Excellence in Oceanography Grant Number: 825.10.022; ETH Zürich; NWO Rubicon; Veni Grant Number: 863.12.004; UK NERC Grant Number: NE/I024798/1; NSF. Grant Numbers: 0436118, 0732555, 1107774
    Description: 2016-05-02
    Keywords: Compound-specific radiocarbon analysis ; Terrestrial carbon markers ; Pan-arctic rivers ; Diacids ; Lignin ; Plant wax lipids
    Repository Name: Woods Hole Open Access Server
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  • 4
    Publication Date: 2022-05-26
    Description: Author Posting. © American Geophysical Union, 2013. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Geochemistry, Geophysics, Geosystems 14 (2013): 5263–5285, doi:10.1002/2013GC004904.
    Description: 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°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°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.
    Description: S.S. thanks the Netherlands Organisation for Scientific Research (NWO) for financial support through a VICI grant and Jaap van der Meer for advice and support on the statistical analysis. A.P. thanks Susan Carter for laboratory assistance and NSF-OCE for funding. A.R.M. thanks Jordi Coello and N uria Moraleda for advice and support on the statistical analysis and Spanish Ministry for research and innovation (MICIIN) for funding. V.G. thanks Xavier Philippon and Carl Johnson for technical assistance. K.G. and M.W. thank the Australian Research Council and John de Laeter Centre for funding toward the LC-MS system, and ARC Fellowship awarded to K.G. C.L.Z. thanks the State Key Laboratory of Marine Geology and the Chinese ‘‘National Thousand Talents’’ program for supporting the LC-MS work performed at Tongji University.
    Description: 2014-06-20
    Keywords: TEX86 ; BIT ; GDGT ; Round robin
    Repository Name: Woods Hole Open Access Server
    Type: Article
    Format: text/plain
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  • 5
    Publication Date: 2022-05-26
    Description: Author Posting. © The Author(s), 2013. This is the author's version of the work. It is posted here by permission of National Academy of Sciences for personal use, not for redistribution. The definitive version was published in Proceedings of the National Academy of Sciences of the United States of America 110 (2013): 14168–14173, doi:10.1073/pnas.1307031110.
    Description: Mobilization of Arctic permafrost carbon is expected to increase with warming-induced thawing. However, this effect is challenging to assess due to the diverse processes controlling the release of various organic carbon (OC) pools from heterogeneous Arctic landscapes. Here, by radiocarbon dating various terrestrial OC components in fluvially- and coastally-integrated estuarine sediments, we present a unique framework for deconvoluting the contrasting mobilization mechanisms of surface versus deep (permafrost) carbon pools across the climosequence of the Eurasian Arctic. Vascular-plant-derived lignin phenol 14C contents reveal significant inputs of young carbon from surface sources whose delivery is dominantly controlled by river runoff. In contrast, plant wax lipids predominantly trace ancient (permafrost) OC that is preferentially mobilized from discontinuous permafrost regions where hydrological conduits penetrate deeper into soils and thermokarst erosion occurs more frequently. As river runoff has significantly increased across the Eurasian Arctic in recent decades, we estimate from an isotopic mixing model that, in tandem with an increased transfer of young surface carbon, the proportion of mobilized terrestrial OC accounted for by ancient carbon has increased by 3-6% between 1985-2004. These findings suggest that, while partly masked by surface-carbon export, climate-change-induced mobilization of old permafrost carbon is well under way in the Arctic.
    Description: The ISSS program is supported by the Knut and Alice Wallenberg Foundation, the Far Eastern Branch of the Russian Academy of Sciences, the Swedish Research Council, the US National Oceanic and Atmospheric Administration, the Russian Foundation of Basic Research, the Swedish Polar Research Secretariat and the Nordic Council of Ministers (Arctic Co-Op and TRI-DEFROST programs). Ö.G. acknowledges an Academy Research Fellow grant from the Swedish Royal Academy of Sciences. Grants OCE-9907129, OCE-0137005, and OCE-0526268 from the US National Science Foundation (NSF), the Stanley Watson Chair for Excellence in Oceanography (to T.I.E.) and ETH Zürich enabled this research. J.E.V. thanks support from NWO-Rubicon (#825.10.022). B.E.v.D thanks support from the UK NERC (NE/I024798/1). X.F. thanks WHOI for a postdoctoral scholar fellowship and for postdoctoral support from ETH Zürich.
    Description: 2014-01-01
    Keywords: Fluvial mobilization ; Compound-specific 14C ; Hydrogeographic control
    Repository Name: Woods Hole Open Access Server
    Type: Preprint
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  • 6
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  • 8
    Publication Date: 2012-02-01
    Print ISSN: 0038-0717
    Electronic ISSN: 1879-3428
    Topics: Biology , Geosciences , Agriculture, Forestry, Horticulture, Fishery, Domestic Science, Nutrition
    Published by Elsevier
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  • 9
    Publication Date: 2012-11-29
    Print ISSN: 0236-5731
    Electronic ISSN: 1588-2780
    Topics: Chemistry and Pharmacology , Energy, Environment Protection, Nuclear Power Engineering
    Published by Springer
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  • 10
    Publication Date: 2020-03-11
    Electronic ISSN: 1664-302X
    Topics: Biology
    Published by Frontiers Media
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