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  • 1
    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
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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
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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
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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
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  • 5
    Publication Date: 2022-05-25
    Description: Author Posting. © The Author(s), 2015. 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 171 (2015): 100-120, doi:10.1016/j.gca.2015.08.005.
    Description: The Mackenzie River in Canada is by far the largest riverine source of sediment and organic carbon (OC) to the Arctic Ocean. Therefore the transport, degradation and burial of OC along the land-to-ocean continuum for this riverine system is important to study both regionally and as a dominant representative of Arctic rivers. Here, we apply sedimentological (grain size, mineral surface area), and organic and inorganic geochemical techniques (%OC, δ13C-OC and Δ14C-OC, 143Nd/144Nd,δ2H and δ18O, major and trace elements) on particulate, bank, channel and lake surface sediments from the Mackenzie Delta, as well as on surface sediments from the Mackenzie shelf in the Beaufort Sea. Our data show a hydrodynamic sorting effect resulting in the accumulation of finer-grained sediments in lake and shelf deposits. A general decrease in organic carbon (OC) to mineral surface area ratios from river-to-sea furthermore suggests a loss of mineral-bound terrestrial OC during transport through the delta and deposition on the shelf. The net isotopic value of the terrestrial OC that is lost en route, derived from relationships between δ13C, OC and surface area, is -28.5‰ for δ13C and -417‰ for Δ14C. We calculated that OC burial efficiencies are around 55%, which are higher (~20%) than other large river systems such as the Amazon. Old sedimentary OC ages, up to 12 14C-ky, suggest the delivery of both a petrogenic OC source (with an estimated contribution of 19±9%) as well as a pre-aged terrestrial OC source. We calculated the 14C-age of this pre-aged, biogenic, component to be about 6100 yrs, or -501‰, which illustrates that terrestrial OC in the watershed can reside for millennia in soils before being released into the river. Surface sediments in lakes across the delta (n=20) showed large variability in %OC (0.92% to 5.7%) and δ13C (-30.7‰ to -23.5‰). High-closure lakes, flooding only at exceptionally high water levels, hold high sedimentary OC contents (〉 2.5%) and young biogenic OC with a terrestrial or an autochthonous source whereas no-closure lakes, permanently connected to a river channel, hold sediments with pre-aged, terrestrial OC. The intermediate low-closure lakes, flooding every year during peak discharge, display the largest variability in OC content, age and source, likely reflecting variability in for example the length of river-lake connections, the distance to sediment source and the number of intermediate settling basins. Bank, channel and suspended sediment show variable 143Nd/144Nd values, yet there is a gradual but distinct spatial transition in 143Nd/144Nd (nearly three ε units; from -11.4 to -13.9) in the detrital fraction of lake surface sediments from the western to the eastern delta. This reflects the input of younger Peel River catchment material in the west and input of older geological source material in the east, and suggests that lake sediments can be used to assess variability in source watershed patterns across the delta.
    Description: We would like to acknowledge financial support from the WHOI Arctic Research Initiative, the US NSF Arctic Natural Sciences (ARC #0909377), the US NSF Arctic GRO (#0732522 and #1107774), NWO Rubicon (#825.10.022) and NWO Veni (#863.12.004), and ETH Zürich.
    Repository Name: Woods Hole Open Access Server
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  • 6
    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
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  • 7
    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
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  • 8
    Publication Date: 2022-05-26
    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): 5597-5618, doi:10.5194/bg-12-5597-2015.
    Description: Rapid changes in the volume and sources of discharge during the spring freshet lead to pronounced variations in biogeochemical properties in snowmelt-dominated river basins. We used daily sampling during the onset of the freshet in the Fraser River (southwestern Canada) in 2013 to identify rapid changes in the flux and composition of dissolved material, with a focus on dissolved organic matter (DOM). Previous time series sampling (at twice monthly frequency) of dissolved inorganic species in the Fraser River has revealed smooth seasonal transitions in concentrations of major ions and tracers of water and dissolved load sources between freshet and base flow periods. In contrast, daily sampling reveals a significant increase in dissolved organic carbon (DOC) concentration (200 to 550 μmol L−1) occurring over a matter of days, accompanied by a shift in DOM optical properties, indicating a transition towards higher molecular weight, more aromatic DOM composition. Comparable changes in DOM composition, but not concentration, occur at other times of year, underscoring the role of seasonal climatology in DOM cycling. A smaller data set of total and dissolved Hg concentrations also showed variability during the spring freshet period, although dissolved Hg dynamics appear to be driven by factors beyond DOM as characterized here. The time series records of DOC and particulate organic carbon (POC) concentrations indicate that the Fraser River exports 0.25–0.35 % of its annual basin net primary productivity. The snowmelt-dominated hydrology, forested land cover, and minimal reservoir impoundment of the Fraser River may influence the DOC yield of the basin, which is high relative to the nearby Columbia River and of similar magnitude to that of the Yukon River to the north. Anticipated warming and decreased snowfall due to climate changes in the region may cause an overall decrease in DOM flux from the Fraser River to the coastal ocean in coming decades
    Description: This work was partially supported by a WHOI Ocean Ventures Fund award to BMV and NSF grants EAR-1226818 to BPE, OCE-0851015 to TIE, BPE, and VG, and OCE-0851101 to RGMS, and support to BPE from Jane and James Orr.
    Repository Name: Woods Hole Open Access Server
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  • 9
    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
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