Compositional pattern of lignin derived phenols of sediments as a proxy of accumulation of terrestrial organic matter in coastal zone of the Laptev Sea

Author(s):  
Alexander Ulyantsev ◽  
Svetlana Bratskaya ◽  
Nikolay Belyaev ◽  
Oleg Dudarev ◽  
Igor Semiletov

<p>The modern East Siberian Arctic shelf represents a fascinating area with a vast expansion of subsea permafrost that holds a large pool of frozen immobilised organic carbon (OC). Amplified climate change at high latitudes has raised growing concerns about potential positive carbon–climate feedbacks. Degradation of permafrost in the Arctic could constitute a positive feedback to climate change due to activation of this OC stock, while recognizing the origin and peculiarities of organic matter (OM) is useful for predicting the potential for involving the ancient OC in modern carbon cycling. This paper emphasises the molecular composition of lignin-derived phenols (LDP) in bottom sediments and subsea permafrost from the Laptev Sea shelf as a proxy to describe the main sources, distribution, and preservation of terrestrial OM. The compositional pattern and concentration of LDP revealed irregular dynamics of terrigenous OM supply in the study area, that were governed primarily by continental flows. The OC concentration in the studied sediments varied from 0.04% to 23.1% (mean 1.74%, median 1.07%). The concentration of LDP in the studied 126 samples from five sediment cores obtained from Buor-Khaya Bay varied from 0.7 to 13191 (mean 539, median 63.5) µg/g of dry sediment as the sum of vanillyl, syringyl, and cinnamyl (VSC) compounds and from 0.03 to 27.6 (mean 1.61, median 0.76) mg/100 mg of OC content. All OC-rich samples showed higher concentrations of LDP and virtually non-oxidized lignin. Vegetation proxies suggested that vascular plant tissues account for a significant fraction of the lignin in the examined samples, with a strong share of gymnosperms. The concentration of LDP correlates to OC content, indicating a strong supply of terrestrial OC to the study area. Degradation proxies indicate a predominant supply of wood-rich non-oxidized terrestrial OM. The well-preserved lignin revealed in the studied deposits represents a specific feature of Quaternary lithodynamics of the Laptev Sea and is not typical for the majority of bottom sediments of the World Ocean. Good correlation between OC and lignin concentration suggests that terrigenous fluxes were the main contributor to OM supply. Distribution of specific lignin phenols and related ratios coupled with lithology and grain size revealed that fluvial processes have been leading here.</p><p>This research was supported through the Russian Scientific Foundation (grant no. 19-77-10044) within the framework of the state assignment of the Shirshov Institute of Oceanology RAS (grant no. 0149-2019-0006).</p>

2020 ◽  
Author(s):  
Van Liem Nguyen ◽  
Birgit Wild ◽  
Örjan Gustafsson ◽  
Igor Semiletov ◽  
Oleg Dudarev ◽  
...  

<p>Widespread accelerated permafrost thawing is predicted for this century and beyond. This threatens to remobilize the large amounts of Mercury (Hg) currently ‘locked’ in Arctic permafrost soils to the Arctic Ocean and thus potentially lead to severe consequences for human and wildlife health. Future risks of Arctic Hg in a warmer climate are, however, poorly understood. One crucial knowledge gap to fill is the fate of Hg once it enters the marine environment on the continental shelves. Arctic rivers are already today suggested to be the main source of Hg into the Arctic Ocean, with dissolved and particulate organic matter (DOM and POM, respectively) identified as important vectors for the land to sea transport.</p><p>In this study, we have investigated total Hg (HgT) and monomethylmercury (MeHg) concentrations in surface sediments from the East Siberian Arctic Shelf (ESAS) along a transect from the Lena river delta to the Laptev Sea continental slope. The ESAS is the world’s largest continental shelf and receives large amounts of organic carbon by the great Arctic Russian rivers (e.g., Lena, Indigirka and Kolyma), remobilized from continuous and discontinuous permafrost regions in the river catchments, and from coastal erosion. Data on HgT and MeHg levels in ESAS sediments is however limited. Here, we observed concentrations of Hg ranging from 30 to 96 ng Hg g<sup>-1</sup> d.w. of HgT, and 0.03 to 9.5 ng Hg g<sup>-1</sup> d.w. of MeHg. Similar concentrations of HgT were observed close to the river delta (54 ± 19 ng Hg g<sup>-1</sup> d.w.), where >95 % of the organic matter is of terrestrial origin, and the other section of the transect (42 ± 7 ng Hg g<sup>-1</sup> d.w.) where the terrestrial organic matter is diluted with carbon from marine sources. In contrast, we observed higher concentrations of MeHg close to the river delta (0.72 ± 0.71 ng Hg g<sup>-1</sup> d.w. as MeHg) than further out on the continental shelf (0.031 ± 0.71 ng Hg g<sup>-1</sup> d.w. as MeHg). We also observed a positive correlation between the MeHg:Hg ratio and previously characterized molecular markers of terrestrial organic matter (Bröder et al. Biogeosciences (2016) & Nature Com. (2018)). We thus suggest riverine inputs, rather than in situ MeHg formation, to explain observed MeHg trends.</p>


2019 ◽  
Vol 16 (13) ◽  
pp. 2693-2713 ◽  
Author(s):  
Bennet Juhls ◽  
Pier Paul Overduin ◽  
Jens Hölemann ◽  
Martin Hieronymi ◽  
Atsushi Matsuoka ◽  
...  

Abstract. River water is the main source of dissolved organic carbon (DOC) in the Arctic Ocean. DOC plays an important role in the Arctic carbon cycle, and its export from land to sea is expected to increase as ongoing climate change accelerates permafrost thaw. However, transport pathways and transformation of DOC in the land-to-ocean transition are mostly unknown. We collected DOC and aCDOM(λ) samples from 11 expeditions to river, coastal and offshore waters and present a new DOC–aCDOM(λ) model for the fluvial–marine transition zone in the Laptev Sea. The aCDOM(λ) characteristics revealed that the dissolved organic matter (DOM) in samples of this dataset are primarily of terrigenous origin. Observed changes in aCDOM(443) and its spectral slopes indicate that DOM is modified by microbial and photo-degradation. Ocean colour remote sensing (OCRS) provides the absorption coefficient of coloured dissolved organic matter (aCDOM(λ)sat) at λ=440 or 443 nm, which can be used to estimate DOC concentration at high temporal and spatial resolution over large regions. We tested the statistical performance of five OCRS algorithms and evaluated the plausibility of the spatial distribution of derived aCDOM(λ)sat. The OLCI (Sentinel-3 Ocean and Land Colour Instrument) neural network swarm (ONNS) algorithm showed the best performance compared to in situ aCDOM(440) (r2=0.72). Additionally, we found ONNS-derived aCDOM(440), in contrast to other algorithms, to be partly independent of sediment concentration, making ONNS the most suitable aCDOM(λ)sat algorithm for the Laptev Sea region. The DOC–aCDOM(λ) model was applied to ONNS-derived aCDOM(440), and retrieved DOC concentration maps showed moderate agreement to in situ data (r2=0.53). The in situ and satellite-retrieved data were offset by up to several days, which may partly explain the weak correlation for this dynamic region. Satellite-derived surface water DOC concentration maps from Medium Resolution Imaging Spectrometer (MERIS) satellite data demonstrate rapid removal of DOC within short time periods in coastal waters of the Laptev Sea, which is likely caused by physical mixing and different types of degradation processes. Using samples from all occurring water types leads to a more robust DOC–aCDOM(λ) model for the retrievals of DOC in Arctic shelf and river waters.


2019 ◽  
Vol 98 ◽  
pp. 06006
Author(s):  
Elena Gershelis ◽  
Ivan Goncharov ◽  
Oleg Dudarev ◽  
Alexey Ruban ◽  
Igor Semiletov

Here we present lithological and geochemical characteristics of the core drilled in coastal part of the Laptev Sea (Ivashkina Lagoon, Bykovsky Peninsula). It is shown that for sediments accumulated in specific lagoon conditions the increased content of organic carbon is confined to fine-grained lacustrine and lagoonal sediments in the uppermost layers. Pyrolytic analysis results indicate a sharp variability in the content of total organic carbon and volatile organic compounds across the studied horizons. The distribution of n-alkanes is characterized by the dominance of high molecular weight homologues, which indicates the ubiquitous contribution of higher terrestrial vegetation discharged with river and coastal thermo abrasion fluxes to the organic matter of bottom sediments.


2020 ◽  
Author(s):  
Elena Gershelis ◽  
Roman Kashapov ◽  
Alexey Ruban ◽  
Andrey Grin'ko ◽  
Oleg Dudarev ◽  
...  

<p>The East Siberian Arctic shelf (ESAS), the world’s largest continental shelf, receives substantial input of terrestrial organic carbon (TerrOC) both from increasing river discharge and from amplifying coastal erosion. Increasing TerrOC supply directly affects the Arctic marine carbon cycle, and, therefore, the fate of TerrOC upon its translocation to the Arctic continental margin has been the subject of growing interest in recent decades. Previous studies reported a strong decrease in sedimentary bulk TerrOC and terrestrial biomarkers with increasing distance from the coast during cross-shelf transport with much higher extent of degradation in the ESAS nearshore zone. Despite major progress has been made in estimating TerrOC inputs and quantifying its degradation rates in the Arctic land-shelf system, there are still important pieces insufficiently understood. Rock-Eval (RE) pyrolysis contributes to the traditional geochemical interpretations, based on elemental, isotopic and biomarker analyses and provides additional insight into the distribution, source and degradation state of organic carbon compounds of sedimentary organic matter.</p><p>In this study, the analytical approach included the characterization of marine and terrestrial carbon compounds using RE data coupled with organic carbon stable isotope composition. Rock-Eval analyses was performed on over 80 surface sediments samples from the Laptev Sea and western part of the East Siberian Sea collected during Arctic expeditions in 2011-2019. A track of rapidly degrading terrOC in shallow deposits may be traced using the ratios between hydrogen and oxygen indices and from the distribution of labile organic carbon fraction. Our results indicated high content of heavily degraded material with low hydrogen index, high oxygen index and a high content of residual carbon in sediments on the outer shelf of the western Laptev Sea and on the continental slope. Sharp decreasing of oxygen content in the eastern part of Laptev Sea and the western East Siberian Sea marked intensive dilution of degraded carbon with fresher material exported from New Siberian Islands. Furthermore, the RE data indicated a relatively high content of residual carbon (up to 87 %) stored in the studied surface sediments.</p><p>This research is supported by Russian Science Foundation, project # 19-77-00067.</p>


2020 ◽  
Author(s):  
Irina Oberemok ◽  
Elena Gershelis ◽  
Andrey Grin’ko ◽  
Alexey Ruban ◽  
Elizaveta Klevantseva ◽  
...  

<p>Accelerating coastal erosion and enhancing river sediment discharge are expected to greatly increase the delivery of terrestrial organic carbon (terrOC) to the Arctic Ocean. Remobilized terrOC may be buried in shallow or outer shelf sediments, degraded and translocated to the deeper basins, or remineralized in the water column causing a positive feedback to amplified global warming. The East Siberian Arctic Shelf (ESAS), represented by the Laptev Sea, the East Siberian Sea, and the Russian part of the Chukchi Sea, is the widest and shallowest continental shelf of the World Ocean. In the current study, we investigated surface sediment samples collected across the Laptev Sea shelf (from the coastline to the outer shelf) during the Arctic expedition onboard the Russian <em>R/V Academician M. Keldysh</em> during fall 2018.</p><p>We analyzed 16 samples for bulk (TOC, <em>δ</em>13C) and molecular (distribution and concentration of n-alkanes and PAHs) parameters. We also performed Rock-Eval (RE) analysis in order to compare its results with the signatures provided by traditional geochemical tracers and thereby to gain new insights into the sources of organic matter in modern surface sediments. In addition, a grain-size analysis was carried out to reveal hydrodynamic control on the organic carbon transport across the studied transect. Using a combination of traditional molecular interpretations (performed in this study and published earlier) and RE parameters (Hydrogen index, Oxygen index and T<sub>peak</sub>) we attempted to distinguish riverine input and coastal erosion and disentangle processes of terrOC degradation and its replacement with fresh/marine OC during cross-shelf transport. Overall, a strong decrease of terrigenous contribution to the sedimentary organic carbon was observed on molecular level with increasing distance from the coast. According to the RE data, intensive terrOC degradation takes place in the shallow and mid-shelf sediments which is traced by sharply increasing oxygen index. The clear correlation between OI and the clay content points toward the perception that mineral matrix do not seem to be such good protector as expected, and intensive microbial degradation of the sedimentary organic matter contained in fine particles occurs during repeated resuspension.</p><p>This research is supported by Russian Science Foundation, project # 19-77-00067.</p>


2021 ◽  
Author(s):  
Felipe Matsubara ◽  
Birgit Wild ◽  
Jannik Martens ◽  
Rickard Wennström ◽  
Oleg Dudarev ◽  
...  

<p>    Ongoing global warming is expected to accelerate the thaw of permafrost on land and to increase the input of terrigenous organic matter (terrOM) into the Arctic Ocean through coastal erosion and river discharge. Large remobilization of terrOM into the East Siberian Arctic Shelf (ESAS) dominates the organic matter in surface sediments over large parts of the shelf and its degradation contributes to ocean acidification. Previous studies have focused on the source apportionment of terrOM and the releases of CO<sub>2</sub> and CH<sub>4</sub> to the atmosphere from terrOM degradation; this study focuses on its diagenetic state during cross-shelf transport, since degradation is the link between permafrost thawing and greenhouse gases emissions. This study probes the degradation status of different terrOM components across the ESAS using various molecular and isotopic proxies and hence evaluates their differences to infer degradation.</p><p>    High-molecular weight (HMW) lipid compounds and lignin phenols are exclusively produced by terrestrial plants, providing protection, strength and rigidity to the plant structure. Owing to diagenesis, microbial degradation leads to <strong>1)</strong> <strong>loss of functional groups</strong>, thus the ratios of HMW n-alkanoic acids, HMW n-alkanols and sterols relative to HMW n-alkanes decrease; <strong>2)</strong> <strong>reduction of unsaturated to saturated carbons</strong>, so ratios of stanols relative to stenols increase; <strong>3) a higher formation of carboxylic acids in the lignin polymer</strong> and hence<strong> </strong>ratios of acids to aldehydes of vanillyl (Vd and Vl) and syringyl (Sd and Sl) increase.</p><p>    The concentrations of lipid- and lignin-derived products per sediment specific surface area decreased with offshore distance of the samples. During cross-shelf transport, the biomarker degradation proxies showed an increasing degradation for Sd/Sl, Vd/Vl, the “tannin-like” compound 3,5-dihydrobenzoic acid to vanillyl (3,5-Bd/V), β-sitostanol/ β-sitostenol and Carbon Preference Index (CPI) of HMW n-alkanes. Some other proxies showed no clear trend from inner to outer shelf and such inconsistent patterns are currently being investigated to better understand both the usefulness/response of different proxies and of the lability of terrOM in the ESAS. While β-sitostanol/β-sitostenol and CPI HMW n-alkane did not show strong differences between the East Siberian Sea and the Laptev Sea, Vd/Vl and Sd/Sl ratios indicated stronger degradation on the outer Laptev Sea and 3,5-Bd/V ratios indicated stronger degradation in the outer eastern East Siberian Sea. Such differences could reflect source properties of terrOM entering the ESAS, such as differences in source vegetation or transport pathway, i.e. coastal erosion or river discharge.</p>


2021 ◽  
Vol 62 (4) ◽  
pp. 460-473
Author(s):  
V.I. Petrova ◽  
G.I. Batova ◽  
A.V. Kursheva ◽  
I.V. Litvinenko ◽  
I.P. Morgunova

Abstract ––The main factors controlling the bulk sedimentation in the Siberian segment of the Lomonosov Ridge (axial part and western slope) and the Laptev Sea continental margin during the late Cenozoic were studied using a complex of geomorphological, lithological, and organic geochemical data. Samples for the study were collected during the cruises of R/V Akademik Fedorov in 2005 and 2007 and nuclear icebreaker Rossiya in 2007. Analysis of the group and molecular composition of the dispersed organic matter (DOM) in bottom sediments has shown that the input of terrigenous sediments enriched in the products of abrasion of lithified rocks determines sedimentation process on the continental slope of the Laptev Sea and in the Amundsen Basin. The individual characteristics of the DOM of the late Cenozoic sediments from the Lomonosov Ridge reflect the wide diversity of sedimentary sources and depositional environments. Subaqueous erosion of edaphogenic products and pre-Holocene sediments plays an important part in sedimentation together with terrigenous flow and ice transport.


2021 ◽  
Author(s):  
I. Litvinenko ◽  
A. Kursheva ◽  
V. Petrova ◽  
G. Batova ◽  
I. Morgunova ◽  
...  

2019 ◽  
Author(s):  
Bennet Juhls ◽  
Pier Paul Overduin ◽  
Jens Hölemann ◽  
Martin Hieronymi ◽  
Atsushi Matsuoka ◽  
...  

Abstract. River water is the main source of dissolved organic carbon (DOC) in the Arctic Ocean. DOC plays an important role in the Arctic carbon cycle and its export from land to sea is expected to increase as ongoing climate change accelerates permafrost thaw. However, transport pathways and transformation of DOC in the land-to-ocean transition are mostly unknown. We collected DOC and aCDOM(λ) samples from 11 expeditions to river, coastal and offshore waters and present a new DOC-aCDOM(λ) model for the fluvial-marine transition zone in the Laptev Sea The aCDOM(λ) characteristics revealed that the DOM in samples of this dataset are primarily of terrigenous origin. Observed changes in aCDOM and its spectral slopes indicate that DOM is modified by microbial- and photo-degradation. Ocean Color Remote Sensing (OCRS) provides the absorption coefficient of colored dissolved organic matter (aCDOM(λ)sat) at λ = 440 or 443 nm, which can be used to estimate DOC concentration at high temporal and spatial resolution over large regions. We tested the statistical performance of five OCRS algorithms and evaluated the plausibility of the spatial distribution of derived aCDOM(λ)sat. The ONNS algorithm showed the best performance compared to in situ aCDOM(440) (r2 = 0.72). Additionally, we found ONNS-derived aCDOM(440), in contrast to other algorithms, to be partly independent of sediment concentration, making ONNS the most suitable aCDOM(λ)sat algorithm for the Laptev Sea region. The DOC-aCDOM(λ) model was applied to ONNS-derived aCDOM(440) and retrieved DOC concentration maps showed moderate agreement to in situ data (r2 = 0.53). The in situ and satellite-retrieved data were offset by up to several days, which may partly explain the weak correlation for this dynamic region. Satellite-derived surface water DOC concentration maps from MERIS satellite data demonstrate rapid removal of DOC within short time periods in coastal waters of the Laptev Sea, which is likely caused by physical mixing and different types of degradation processes. Using samples from all occurring water types leads to a more robust DOC-aCDOM(λ) model for the retrievals of DOC in Arctic shelf and river waters.


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