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  • 1
    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
    Format: application/pdf
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  • 2
    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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  • 3
    Publication Date: 2022-05-25
    Description: Author Posting. © American Geophysical Union, 2017. 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: Oceans 122 (2017): 4539–4553, doi:10.1002/2016JC012549.
    Description: Biogenic matter characteristics and radiocarbon contents of organic carbon (OC) were examined on sinking particle samples intercepted at three nominal depths of 1000 m, 2000 m, and 3000 m (∼50 m above the seafloor) during a 3 year sediment trap program on the New England slope in the Northwest Atlantic. We have sought to characterize the sources of sinking particles in the context of vertical export of biogenic particles from the overlying water column and lateral supply of resuspended sediment particles from adjacent margin sediments. High aluminum (Al) abundances and low OC radiocarbon contents indicated contributions from resuspended sediment which was greatest at 3000 m but also significant at shallower depths. The benthic source (i.e., laterally supplied resuspended sediment) of opal appears negligible based on the absence of a correlation with Al fluxes. In comparison, CaCO3 fluxes at 3000 m showed a positive correlation with Al fluxes. Benthic sources accounted for 42 ∼ 63% of the sinking particle flux based on radiocarbon mass balance and the relationship between Al flux and CaCO3 flux. Episodic pulses of Al at 3000 m were significantly correlated with the near-bottom current at a nearby hydrographic mooring site, implying the importance of current variability in lateral particle transport. However, Al fluxes at 1000 m and 2000 m were coherent but differed from those at 3000 m, implying more than one mode of lateral supply of particles in the water column.
    Description: NSF Ocean Sciences Chemical Oceanography program Grant Numbers: OCE-0425677, OCE-0851350; Ocean and Climate Change Institute of WHOI
    Description: 2017-12-01
    Keywords: Sinking particle flux ; Biological carbon pump ; Radiocarbon ; Lateral particle supply ; Sediment resuspension ; Northwest Atlantic ; Sediment trap
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 4
    Publication Date: 2022-05-25
    Description: © The Author(s), 2018. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Geophysical Research Letters 45 (2018): 8425-8434, doi:10.1029/2018GL078904.
    Description: Compound‐specific radiocarbon analysis was performed on different grain‐size fractions of surficial sediments to examine and compare lateral transport times (LTTs) of organic carbon. 14C aging of long‐chain leaf wax fatty acids along two dispersal pathways of fluvially derived material on adjacent continental margins implies LTTs over distances of ~30 to 500 km that range from hundreds to thousands of years. The magnitude of aging differs among grain size fractions. Our finding suggests that LTTs vary both temporally and spatially as a function of the specific properties of different continental shelf settings. Observations suggest that 14C aging is widespread during lateral transport over continental shelves, with hydrodynamic particle sorting inducing age variations among organic components residing in different grain sizes. Consideration of these phenomena is of importance for understanding carbon cycle processes and interpretation on sedimentary records on continental margins.
    Description: National Natural Science Foundation of China Grant Numbers: 41520104009, 41521064; MOE; JSPS Grant Numbers: A‐1003, 2‐1304, B‐0904, B‐0903, 22310014, 23651021, 25550020; NIES; SNSF Grant Number: 200021_140850
    Keywords: Radiocarbon ; Lateral particle transport time ; Organic carbon aging ; Continental shelf sediments ; Grain size fractions
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 5
    Publication Date: 2022-05-25
    Description: Author Posting. © American Geophysical Union, 2018. 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 123 (2018): 2908-2921, doi:10.1029/2017JG004285.
    Description: Information on the age dynamics of particulate organic matter (POM) in large river systems is currently sparse and represents an important knowledge gap in our understanding of the global carbon cycle. Here we examine variations in organic geochemical characteristics of suspended sediments from the Changjiang (Yangtze River) system collected between 1997 and 2010. Higher particulate organic carbon content (POC%) values were observed in the middle reach, especially after 2003, and are attributed to the increase of in situ (aquatic) primary production associated with decreased total suspended matter concentrations. Corresponding Δ14C values from depth profiles taken in 2009 and 2010 indicate spatial and temporal variations in POC sources within the basin. Two isotopic mass balance approaches were explored to quantitatively apportion different sources of Changjiang POM. Results indicate that contributions of biomass and pre‐aged soil organic matter are dominant, regardless of hydrological conditions, with soil‐derived organic carbon comprising 17–56% of POC based on a Monte Carlo three‐end‐member mixing model. In contrast, binary mixing model calculations suggest that up to 80% of POC (2009 samples only) derived from biospheric sources. The emplacement of the Three Gorges Dam and resulting trapping of sediment from the upper reach of the watershed resulted in a modification of POM 14C ages in the reservoir. With the resulting decline in sediment load and increase in the proportion of modern POC in the lower reach, these changes in POM flux and composition of the Changjiang have significant implications for downstream carbon cycle processes.
    Description: Natural Science Foundation of China Grant Numbers: 41530960, 41276081
    Description: 2019-03-15
    Keywords: Organic carbon ; Changjiang ; Radiocarbon ; Suspended particulate matter ; Three Gorges Dam
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 6
    Publication Date: 2022-05-25
    Description: Author Posting. © The Author(s), 2018. This is the author's version of the work. It is posted here under a nonexclusive, irrevocable, paid-up, worldwide license granted to WHOI. It is made available for personal use, not for redistribution. The definitive version was published in Geochimica et Cosmochimica Acta 244 (2019): 502-521, doi:10.1016/j.gca.2018.09.034.
    Description: Relatively little is known about the amount of time that lapses between the photosynthetic fixation of carbon by vascular land plants and its incorporation into the marine sedimentary record, yet the dynamics of terrestrial carbon sequestration have important implications for the carbon cycle. Vascular plant carbon may encounter multiple potential intermediate storage pools and transport trajectories, and the age of vascular plant carbon accumulating in marine sediments will reflect these different predepositional histories. Here, we examine down-core 14C profiles of higher plant leaf waxderived fatty acids isolated from high fidelity sedimentary sequences spanning the socalled “bomb-spike”, and encompassing a ca. 60-degree latitudinal gradient from tropical (Cariaco Basin), temperate (Saanich Inlet), and polar (Mackenzie Delta) watersheds to constrain integrated vascular plant carbon storage/transport times (“residence times”). Using a modeling framework, we find that, in addition to a "young" (conditionally defined as 〈 50 y) carbon pool, an old pool of compounds comprises 49 to 78 % of the fractional contribution of organic carbon (OC) and exhibits variable ages reflective of the environmental setting. For the Mackenzie Delta sediments, we find a mean age of the old pool of 28 ky (±9.4, standard deviation), indicating extensive pre-aging in permafrost soils, whereas the old pools in Saanich Inlet and Cariaco Basin sediments are younger, 7.9 (±5.0) and 2.4 (±0.50) to 3.2 (±0.54) ky, respectively, indicating less protracted storage in terrestrial reservoirs. The "young" pool showed clear annual contributions for Saanich Inlet and Mackenzie Delta sediments (comprising 24% and 16% of this pool, respectively), likely reflecting episodic transport of OC from steep hillside slopes surrounding Saanich Inlet and annual spring flood deposition in the Mackenzie Delta, respectively. Contributions of 5-10 year old OC to the Cariaco Basin show a short delay of OC inflow, potentially related to transport time to the offshore basin. Modeling results also indicate that the Mackenzie Delta has an influx of young but decadal material (20-30 years of age), pointing to the presence of an intermediate reservoir. Overall, these results show that a significant fraction of vascular plant C undergoes pre-aging in terrestrial reservoirs prior to accumulation in deltaic and marine sediments. The age distribution, reflecting both storage and transport times, likely depends on landscape-specific factors such as local topography, hydrographic characteristics, and mean annual temperature of the catchment, all of which affect the degree of soil buildup and preservation. We show that catchment-specific carbon residence times across landscapes can vary by an order of magnitude, with important implications both for carbon cycle studies and for the interpretation of molecular terrestrial paleoclimate records preserved in sedimentary sequences.
    Description: Financial support was provided by a Schlanger Ocean Drilling Graduate Fellowship (NJD), an EPA STAR Graduate Fellowship (NJD), a Dutch NWO Veni grant #825.10.022 (JEV), US NSF grants #OCE-0137005 (TIE and KAH), #OCE-052626800 (TIE), #OCE-0961980 (ERMD), and #EAR-0447323 (ERMD and JRS), a Swiss SNF grant #200021_140850 (TIE), a Swedish Research Council grant #2013-05204 (MS), as well as the Stanley Watson Chair for Excellence in Oceanography at WHOI (TIE) and the WHOI Arctic Research Initiative (TIE and LG).
    Keywords: Terrestrial carbon ; Organic matter ; Radiocarbon ; Leaf waxes ; Sediment ; Residence time
    Repository Name: Woods Hole Open Access Server
    Type: Preprint
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  • 7
    Publication Date: 2022-10-26
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Eglinton, T. I., Galy, V. V., Hemingway, J. D., Feng, X., Bao, H., Blattmann, T. M., Dickens, A. F., Gies, H., Giosan, L., Haghipour, N., Hou, P., Lupker, M., McIntyre, C. P., Montluçon, D. B., Peucker-Ehrenbrink, B., Ponton, C., Schefuß, E., Schwab, M. S., Voss, B. M., Wacker, L., Wu, Y., & Zhao, M. Climate control on terrestrial biospheric carbon turnover. Proceedings of the National Academy of Sciences of the United States of America, 118(8), (2021): e2011585118, htps://doi.org/ 10.1073/pnas.2011585118.
    Description: Terrestrial vegetation and soils hold three times more carbon than the atmosphere. Much debate concerns how anthropogenic activity will perturb these surface reservoirs, potentially exacerbating ongoing changes to the climate system. Uncertainties specifically persist in extrapolating point-source observations to ecosystem-scale budgets and fluxes, which require consideration of vertical and lateral processes on multiple temporal and spatial scales. To explore controls on organic carbon (OC) turnover at the river basin scale, we present radiocarbon (14C) ages on two groups of molecular tracers of plant-derived carbon—leaf-wax lipids and lignin phenols—from a globally distributed suite of rivers. We find significant negative relationships between the 14C age of these biomarkers and mean annual temperature and precipitation. Moreover, riverine biospheric-carbon ages scale proportionally with basin-wide soil carbon turnover times and soil 14C ages, implicating OC cycling within soils as a primary control on exported biomarker ages and revealing a broad distribution of soil OC reactivities. The ubiquitous occurrence of a long-lived soil OC pool suggests soil OC is globally vulnerable to perturbations by future temperature and precipitation increase. Scaling of riverine biospheric-carbon ages with soil OC turnover shows the former can constrain the sensitivity of carbon dynamics to environmental controls on broad spatial scales. Extracting this information from fluvially dominated sedimentary sequences may inform past variations in soil OC turnover in response to anthropogenic and/or climate perturbations. In turn, monitoring riverine OC composition may help detect future climate-change–induced perturbations of soil OC turnover and stocks.
    Description: This work was supported by grants from the US NSF (OCE-0928582 to T.I.E. and V.V.G.; OCE-0851015 to B.P.-E., T.I.E., and V.V.G.; and EAR-1226818 to B.P.-E.), Swiss National Science Foundation (200021_140850, 200020_163162, and 200020_184865 to T.I.E.), and National Natural Science Foundation of China (41520104009 to M.Z.).
    Keywords: Radiocarbon ; Plant biomarkers ; Carbon turnover times ; Fluvial carbon ; Carbon cycle
    Repository Name: Woods Hole Open Access Server
    Type: Article
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