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  • 1
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    Relationships between carbon isotopic composition and mode of binding of natural organic matter in selected marine sediments (2008)
    Details
    Publication Date: 2022-05-25
    Description: Author Posting. © Elsevier B.V., 2007. This is the author's version of the work. It is posted here by permission of Elsevier B.V. for personal use, not for redistribution. The definitive version was published in Organic Geochemistry 38 (2007):1824-1837, doi:10.1016/j.orggeochem.2007.07.008.
    Description: We have investigated the relationships between radiocarbon (14C) and stable carbon (13C) isotopic composition and the different modes of binding of organic matter (OM) present in surficial sediments from near-shore and continental margin sites that vary in terms of input and depositional conditions. To improve our understanding of the entire OM pool, isotopic analysis of sedimentary sub-fractions, as opposed to individual compounds, was performed. This was achieved by sequentially treating sediments by solvent extraction to examine unbound compounds, followed by saponification to cleave ester linked moieties. Isotopic analysis was then performed on the bulk sediment and resulting residues. The molecular composition of the extracts was examined using gas chromatography/mass spectrometry (GC/MS), and the relative contributions of terrestrial and marine biomarkers were assessed. Radiocarbon abundances (Δ14C) of the bulk sediment reflect a mixture of modern, pre-aged and fossil carbon. Offsets in Δ14C between the bulk sediment and sediment residues demonstrate varying associations of these carbon pools. For the majority of sites, a negative offset between extracted (EX2 RES) and saponified (SA-RES) sediment 1 residues results from the removal of relatively 4C-rich material during saponification. Saponification extracts (SAEs) are mainly composed of short chain (n-C12 to n-C24) alkanoic acids with an even/odd dominance indicating a predominantly marine algal or microbial source. This provides evidence for the protection of labile marine carbon by chemical binding. This study aims to bridge the gap between molecular level and bulk OM analyses in marine sediments.
    Description: The work was supported by funds from the National Science Foundation (CHE-0089172; OCE-0526268).
    Keywords: Radiocarbon ; Stable carbon ; Marine ; Sediments ; Biomarker
    Repository Name: Woods Hole Open Access Server
    Type: Preprint
    Format: application/pdf
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  • 2
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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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  • 3
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    Multimolecular tracers of terrestrial carbon transfer across the pan-Arctic : 14C characteristics of sedimentary carbon components and their environmental controls (2016)
    John Wiley & Sons
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    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
    Type: Article
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  • 4
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    Relevance of carbon stocks of marine sediments for national greenhouse gas inventories of maritime nations (2017)
    Springer
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    Publication Date: 2022-05-25
    Description: © The Author(s), 2017. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Carbon Balance and Management 12 (2017): 10, doi:10.1186/s13021-017-0077-x.
    Description: Determining national carbon stocks is essential in the framework of ongoing climate change mitigation actions. Presently, assessment of carbon stocks in the context of greenhouse gas (GHG)-reporting on a nation-by-nation basis focuses on the terrestrial realm, i.e., carbon held in living plant biomass and soils, and on potential changes in these stocks in response to anthropogenic activities. However, while the ocean and underlying sediments store substantial quantities of carbon, this pool is presently not considered in the context of national inventories. The ongoing disturbances to both terrestrial and marine ecosystems as a consequence of food production, pollution, climate change and other factors, as well as alteration of linkages and C-exchange between continental and oceanic realms, highlight the need for a better understanding of the quantity and vulnerability of carbon stocks in both systems. We present a preliminary comparison of the stocks of organic carbon held in continental margin sediments within the Exclusive Economic Zone of maritime nations with those in their soils. Our study focuses on Namibia, where there is a wealth of marine sediment data, and draws comparisons with sediment data from two other countries with different characteristics, which are Pakistan and the United Kingdom. Results indicate that marine sediment carbon stocks in maritime nations can be similar in magnitude to those of soils. Therefore, if human activities in these areas are managed, carbon stocks in the oceanic realm—particularly over continental margins—could be considered as part of national GHG inventories. This study shows that marine sediment organic carbon stocks can be equal in size or exceed terrestrial carbon stocks of maritime nations. This provides motivation both for improved assessment of sedimentary carbon inventories and for reevaluation of the way that carbon stocks are assessed and valued. The latter carries potential implications for the management of human activities on coastal environments and for their GHG inventories.
    Description: We acknowledge research support from ETH Zurich and the Swiss National Science Foundation.
    Keywords: Carbon stocks ; Sediments ; Oceans ; Climate change ; Exclusive Economic Zone ; Carbon inventory
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 5
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    On the origin of aged sedimentary organic matter along a river-shelf-deep ocean transect (2020)
    American Geophysical Union
    Details
    Publication Date: 2022-10-26
    Description: Author Posting. © American Geophysical Union, 2019. 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 124(8), (2019): 2582-2594, doi: 10.1029/2019JG005107.
    Description: To assess the influences of carbon sources and transport processes on the 14C age of organic matter (OM) in continental margin sediments, we examined a suite of samples collected along a river‐shelf‐deep ocean transect in the East China Sea (ECS). Ramped pyrolysis‐oxidiation was conducted on suspended particulate matter in the Yangtze River and on surface sediments from the ECS shelf and northern Okinawa Trough. 14C ages were determined on OM decomposition products within different temperature windows. These measurements suggest that extensive amounts of pre‐old (i.e., millennial age) organic carbon (OC) are subject to degradation within and beyond the Yangtze River Delta, and this process is accompanied by an exchange of terrestrial and marine OM. These results, combined with fatty acid concentration data, suggest that both the nature and extent of OM preservation/degradation as well as the modes of transport influence the 14C ages of sedimentary OM. Additionally, we find that the age of (thermally) refractory OC increases during across‐shelf transport and that the age offset between the lowest and highest temperature OC decomposition fractions also increases along the shelf‐to‐trough transect. Amplified interfraction spread or 14C heterogeneity is the greatest in the Okinawa Trough. Aged sedimentary OM across the transect may be a consequence of several reasons including fossil OC input, selective degradation of younger OC, hydrodynamic sorting processes, and aging during lateral transport. Consequently, each of them should be considered in assessing the 14C results of sedimentary OM and its implications for the carbon cycle and interpretation of sedimentary records.
    Description: This study was supported by Doc. Mobility Fellowship (P1EZP2_159064; R. B.) from the Swiss National Science Foundation (SNSF). This study was also supported by SNF “CAPS‐LOCK” project 200021_140850 (T. I. E.), by the National Natural Science Foundation of China (NSFC; grants 41520104009 and 41630966, M. Z.), and by the “111” project (B13030). We are grateful for support of the NOSAMS staff in the execution of this project. We also appreciate the assistance from Yushuang Zhang (Ocean University of China) at NOSAMS and members of the Laboratory for Ion Beam Physics at ETH Zurich for AMS measurements. We acknowledge Lei Xing, Haidong Zhang, Guodong Song, Meng Yu, Yonghao Jia, and Shanshan Duan (Ocean University of China) for sampling assistance on the cruises. Assistance at sea by the crews of R/V Dongfanghong II and R/V Hakuhu Maru is also acknowledged. Readers can access or find the data from figures and tables in the supporting information.
    Keywords: Radiocarbon ; Carbon cycle ; Sediments ; Organic carbon ; Hydrodynamic processes
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 6
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    Arctic deltaic lake sediments as recorders of fluvial organic matter deposition (2017)
    Frontiers Media
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    Publication Date: 2022-05-26
    Description: © The Author(s), 2016. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Frontiers in Earth Science 4 (2016): 77, doi:10.3389/feart.2016.00077.
    Description: Arctic deltas are dynamic and vulnerable regions that play a key role in land-ocean interactions and the global carbon cycle. Delta lakes may provide valuable historical records of the quality and quantity of fluvial fluxes, parameters that are challenging to investigate in these remote regions. Here we study lakes from across the Mackenzie Delta, Arctic Canada, that receive fluvial sediments from the Mackenzie River when spring flood water levels rise above natural levees. We compare downcore lake sediments with suspended sediments collected during the spring flood, using bulk (% organic carbon, % total nitrogen, δ13C, Δ14C) and molecular organic geochemistry (lignin, leaf waxes). High-resolution age models (137Cs, 210Pb) of downcore lake sediment records (n = 11) along with lamina counting on high-resolution radiographs show sediment deposition frequencies ranging between annually to every 15 years. Down-core geochemical variability in a representative delta lake sediment core is consistent with historical variability in spring flood hydrology (variability in peak discharge, ice jamming, peak water levels). Comparison with earlier published Mackenzie River depth profiles shows that (i) lake sediments reflect the riverine surface suspended load, and (ii) hydrodynamic sorting patterns related to spring flood characteristics are reflected in the lake sediments. Bulk and molecular geochemistry of suspended particulate matter from the spring flood peak and lake sediments are relatively similar showing a mixture of modern higher-plant derived material, older terrestrial permafrost material, and old rock-derived material. This suggests that deltaic lake sedimentary records hold great promise as recorders of past (century-scale) riverine fluxes and may prove instrumental in shedding light on past behavior of arctic rivers, as well as how they respond to a changing climate.
    Description: Funding was provided by the US National Science Foundation as part of the Arctic Great Rivers Observatory (NSF-0732522 and NSF-1107774), as well as the Netherlands Organization for Scientific Research (Rubicon #825.10.022, and Veni #863.12.004). Additional funding for the lake coring was provided from WHOI through its Ocean and Climate Change Institute.
    Keywords: Lignin ; Biomarkers ; Mackenzie River ; Carbon isotopes ; Lake sediments
    Repository Name: Woods Hole Open Access Server
    Type: Article
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