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  • 1
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    High-sensitivity measurement of diverse vascular plant-derived biomarkers in high-altitude ice cores (2010)
    American Geophysical Union
    Details
    Publication Date: 2022-05-25
    Description: Author Posting. © American Geophysical Union, 2009. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Geophysical Research Letters 36 (2009): L13501, doi:10.1029/2009GL037643.
    Description: Semi-volatile organic compounds derived from burned and fresh vascular plant sources and preserved in high-altitude ice fields were detected and identified through use of recently developed analytical tools. Specifically, stir bar sorptive extraction and thermal desorption coupled with gas chromatography/time-of-flight mass spectrometry allowed measurement of multiple biomarkers in small sample volumes (≤30 ml). Among other compounds of interest, several diterpenoids, which suggest inputs from conifers and conifer burning, were identified in post-industrial era and older Holocene ice from the Sajama site in the Bolivian Andes, but not in a glacial period sample, consistent with aridity changes. Differences in biomarker assemblages between sites support the use of these compounds as regionally constrained recorders of vegetation and climate change. This study represents the first application of these analytical techniques to ice core research and the first indication that records of vegetation fires may be reconstructed from diterpenoids in ice.
    Description: This project was supported in part by NSF-OCE (0402533), and NSF-EAR (0094475).
    Keywords: Biomass burning ; Molecular markers
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 2
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    Radiocarbon dating of alkenones from marine sediments : II. Assessment of carbon process blanks (2011)
    Dept. of Geosciences, University of Arizona
    Details
    Publication Date: 2022-05-25
    Description: Author Posting. © Arizona Board of Regents on behalf of the University of Arizona, 2005. This article is posted here by permission of Dept. of Geosciences, University of Arizona for personal use, not for redistribution. The definitive version was published in Radiocarbon 47 (2005): 413-424.
    Description: We evaluate potential process blanks associated with radiocarbon measurement of microgram to milligram quantities of alkenones at the National Ocean Sciences Accelerator Mass Spectrometry (NOSAMS) facility. Two strategies to constrain the contribution of blanks to alkenone 14C dates were followed: 1) dating of samples of known age and 2) multiple measurements of identical samples. We show that the potential contamination associated with the procedure does not lead to a systematic bias of the results of alkenone dating to either younger or older ages. Our results indicate that alkenones record Δ14C of ambient DIC with an accuracy of approximately 10‰. A conservative estimate of measurement precision is 17‰ for modern samples. Alkenone 14C ages are expected to be reliable within 500 yr for samples younger than 10,500 14C yr.
    Description: This research was funded by NSF grant # OCE-0327405 and DFG project # SCHN621 and a WHOI-NOSAMS postdoctoral scholarship to GM.
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 3
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    Tracing river chemistry in space and time : dissolved inorganic constituents of the Fraser River, Canada (2014)
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    Publication Date: 2022-05-25
    Description: Author Posting. © The Author(s), 2013. This is the author's version of the work. It is posted here by permission of Elsevier for personal use, not for redistribution. The definitive version was published in Geochimica et Cosmochimica Acta 124 (2014): 283-308, doi:10.1016/j.gca.2013.09.006.
    Description: The Fraser River basin in southwestern Canada bears unique geologic and climatic features which make it an ideal setting for investigating the origins, transformations and delivery to the coast of dissolved riverine loads under relatively pristine conditions. We present results from sampling campaigns over three years which demonstrate the lithologic and hydrologic controls on fluxes and isotope compositions of major dissolved inorganic runoff constituents (dissolved nutrients, major and trace elements, 87Sr/86Sr, δD). A time series record near the Fraser mouth allows us to generate new estimates of discharge-weighted concentrations and fluxes, and an overall chemical weathering rate of 32 t km-2 y-1. The seasonal variations in dissolved inorganic species are driven by changes in hydrology, which vary in timing across the basin. The time series record of dissolved 87Sr/86Sr is of particular interest, as a consistent shift between higher (“more radiogenic”) values during spring and summer and less radiogenic values in fall and winter demonstrates the seasonal variability in source contributions throughout the basin. This seasonal shift is also quite large (0.709 – 0.714), with a discharge-weighted annual average of 0.7120 (2 s.d. = 0.0003). We present a mixing model which predicts the seasonal evolution of dissolved 87Sr/86Sr based on tributary compositions and water discharge. This model highlights the importance of chemical weathering fluxes from the old sedimentary bedrock of headwater drainage regions, despite their relatively small contribution to the total water flux.
    Description: This work was supported by the WHOI Academic Programs Office and MIT PAOC Houghton Fund to BMV, a WHOI Arctic Research Initiative grant to ZAW, NSF-ETBC grant OCE-0851015 to BPE and TIE, and NSF grant EAR-1226818 to BPE.
    Repository Name: Woods Hole Open Access Server
    Type: Preprint
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  • 4
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    Radiocarbon dating of alkenones from marine sediments : I. Isolation protocol (2011)
    Dept. of Geosciences, University of Arizona
    Details
    Publication Date: 2022-05-25
    Description: Author Posting. © Arizona Board of Regents on behalf of the University of Arizona, 2005. This article is posted here by permission of Dept. of Geosciences, University of Arizona for personal use, not for redistribution. The definitive version was published in Radiocarbon 47 (2005): 401-412.
    Description: The chemical and isotopic compositions of long-chain (C36–C39) unsaturated ketones (alkenones), a unique class of algal lipids, encode surface ocean properties useful for paleoceanographic reconstruction. Recently, we have sought to extend the utility of alkenones as oceanic tracers through measurement of their radiocarbon contents. Here, we describe a method for isolation of alkenones from sediments as a compound class based on a sequence of wet chemical techniques. The steps involved, which include silica gel column chromatography, urea adduction, and silver nitrate-silica gel column chromatography, exploit various structural attributes of the alkenones. Amounts of purified alkenones estimated by GC/FID measurements were highly correlated with CO2 yields after sample combustion, indicating purities of greater than 90% for samples containing ≥100 μg C. The degree of alkenone unsaturation ( ) also varied minimally through the procedure. We also describe a high-performance liquid chromatography (HPLC) method to isolate individual alkenones for molecular-level structural and isotopic determination.
    Description: This work was funded through grants from the National Science Foundation (OCE-9809624; OCE- 9907129) and the Japan Society for the Promotion of Science.
    Repository Name: Woods Hole Open Access Server
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  • 5
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    14C and 13C characteristics of higher plant biomarkers in Washington margin surface sediments (2013)
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    Publication Date: 2022-05-25
    Description: Author Posting. © The Author(s), 2012. This is the author's version of the work. It is posted here by permission of Elsevier for personal use, not for redistribution. The definitive version was published in Geochimica et Cosmochimica Acta 105 (2013): 14-30, doi:10.1016/j.gca.2012.11.034.
    Description: Plant wax lipids and lignin phenols are the two most common classes of molecular markers that are used to trace vascular plant-derived OM in the marine environment. However, their 13C and 14C compositions have not been directly compared, which can be used to constrain the flux and attenuation of terrestrial carbon in marine environment. In this study, we describe a revised method of isolating individual lignin phenols from complex sedimentary matrices for 14C analysis using high pressure liquid chromatography (HPLC) and compare this approach to a method utilizing preparative capillary gas chromatography (PCGC). We then examine in detail the 13C and 14C compositions of plant wax lipids and lignin phenols in sediments from the inner and mid shelf of the Washington margin that are influenced by discharge of the Columbia River. Plant wax lipids (including n-alkanes, n-alkanoic (fatty) acids, n-alkanols, and n-aldehydes) displayed significant variability in both δ13C (-28.3 to -37.5 ‰) and ∆14C values (-204 to +2 ‰), suggesting varied inputs and/or continental storage and transport histories. In contrast, lignin phenols exhibited similar δ13C values (between -30 to -34 ‰) and a relatively narrow range of ∆14C values (-45 to -150 ‰; HPLC-based mesurement) that were similar to, or younger than, bulk OM (-195 to -137 ‰). Moreover, lignin phenol 14C age correlated with the degradation characteristics of this terrestrial biopolymer in that vanillyl phenols were on average ~500 years older than syringyl and cinnamyl phenols that degrade faster in soils and sediments. The isotopic characteristics, abundance, and distribution of lignin phenols in sediments suggest that they serve as promising tracers of recently biosynthesized terrestrial OM during supply to, and dispersal within the marine environment. Lignin phenol 14C measurements may also provide useful constraints on the vascular plant end member in isotopic mixing models for carbon source apportionment, and for interpretation of sedimentary records of past vegetation dynamics. Key words: 14C and 13C composition, radiocarbon age, plant wax lipids, lignin phenols, Washington margin, marine carbon cycling, terrestrial organic matter
    Description: Grants OCE-9907129, OCE-0137005, and OCE-0526268 (to TIE) from the National Science Foundation (NSF) supported this research.
    Keywords: 14C and 13C composition ; Radiocarbon age ; Plant wax lipids ; Lignin phenols ; Washington margin ; Marine carbon cycling ; Terrestrial organic matter
    Repository Name: Woods Hole Open Access Server
    Type: Preprint
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  • 6
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    Differential mobilization of terrestrial carbon pools in Eurasian Arctic river basins (2013)
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    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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  • 7
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    Spatial variability in the abundance, composition, and age of organic matter in surficial sediments of the East China Sea (2014)
    John Wiley & Sons
    Details
    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 Journal of Geophysical Research: Biogeosciences 118 (2013): 1495–1507, doi:10.1002/2013JG002286.
    Description: Understanding the sources and fate of organic matter (OM) sequestered in continental margin sediments is of importance because the mode and efficiency of OM burial impact the carbon cycle and the regulation of atmospheric CO2 over long time scales. We carried out molecular (lignin-derived phenols from CuO oxidation), elemental, isotopic (δ13C, Δ14C), and sedimentological (grain size and mineral surface area) analyses in order to examine spatial variability in the abundance, source, age of surface sediments of the East China Sea. Higher terrigenous organic matter values were found in the main accumulating areas of fluvial sediments, including the Changjiang (Yangtze) Estuary and Zhejiang-Fujian coastal zone. Isotopic and biomarker data suggest that the sedimentary OM in the inner shelf region was dominated by aged (Δ14C = −423 ± 42‰) but relatively lignin-rich OM (Λ = 0.94 ± 0.57 mg/100 mg OC) associated with fine-grained sediments, suggesting important contributions from soils. In contrast, samples from the outer shelf, while of similar age (Δ14 C = −450 ± 99‰), are lignin poor (Λ = 0.25 ± 0.14 mg/100 mg OC) and associated with coarse-grained material. Regional variation of lignin phenols and OM ages indicates that OM content is fundamentally controlled by hydrodynamic sorting (especially, sediment redistribution and winnowing) and in situ primary production. Selective sorption of acid to aldehyde in clay fraction also modified the ratios of lignin phenols. The burial of lignin in East China Sea is estimated to be relatively efficient, possibly as a consequence of terrigenous OM recalcitrance and/or relatively high sedimentation rates in the Changjiang Estuary and the adjacent Zhejing-Fujian mud belt.
    Description: This study was funded by the Natural Science Foundation of China (41021064), Ministry of Science and Technology (2011CB409802), and others such as (41076052, 2010DFA24590). WY acknowledges financial support from the Alexander von Humboldt Foundation and SKLCE RCD and 111 projects. TE acknowledges financial support from a WHOI Senior Scientist Chair.
    Description: 2014-05-15
    Keywords: Radiocarbon ages ; Lignin phenols ; Sediment
    Repository Name: Woods Hole Open Access Server
    Type: Article
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