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Compositional clues to sources and sinks of terrestrial organic matter transported to the Eurasian Arctic shelf
Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. (Örjan Gustafssons research group)
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The amount of organic carbon (OC) present in Siberian Arctic permafrost soils is estimated at twice the amount of carbon currently in the atmosphere. The shelf seas of the Arctic Ocean receive large amounts of this terrestrial OC from Eurasian Arctic rivers and from coastal erosion. Degradation of this land-derived material in the sea would result in the production of dissolved carbon dioxide and may then add to the atmospheric carbon dioxide reservoir. Observations from the Siberian Arctic suggest that transfer of carbon from land to the marine environment is accelerating. However, it is not clear how much of the transported OC is degraded and oxidized, nor how much is removed from the active carbon cycle by burial in marine sediment.

Using bulk geochemical parameters, total OC, d13C and D14C isotope composition, and specific molecular markers of plant wax lipids and lignin phenols, the abundance and composition of OC was determined in both dissolved and particulate carrier phases: the colloidal OC (COC; part of the dissolved OC), particulate OC (POC), and sedimentary OC (SOC). Statistical modelling was used to quantify the relative contribution of OC sources to these phases. Terrestrial OC is derived from the seasonally thawing top layer of permafrost soil (topsoil OC) and frozen OC derived from beneath the active layer eroded at the coast, commonly identified as yedoma ice complex deposit OC (yedoma ICD-OC). These carbon pools are transported differently in the aquatic conduits. Topsoil OC was found in young DOC and POC, in the river water, and the shelf water column, suggesting long-distance transport of this fraction. The yedoma ICD-OC was found as old particulate OC that settles out rapidly to the underlying sediment and is laterally transported across the shelf, likely dispersed by bottom nepheloid layer transport or via ice rafting.

These two modes of OC transport resulted in different degradation states of topsoil OC and yedoma ICD-OC. Terrestrial CuO oxidation derived biomarkers indicated a highly degraded component in the COC. In contrast, the terrestrial component of the SOC was much less degraded. In line with earlier suggestions the mineral component in yedoma ICD functions as weight and surface protection of the associated OC, which led to burial in the sediment, and limited OC degradation. The degradability of the terrestrial OC in shelf sediment was also addressed in direct incubation studies. Molecular markers indicate marine OC (from primary production) was more readily degraded than terrestrial OC. Degradation was also faster in sediment from the East Siberian Sea, where the marine contribution was higher compared to the Laptev Sea. Although terrestrial carbon in the sediment was degraded slower, the terrestrial component also contributed to carbon dioxide formation in the incubations of marine sediment.

These results contribute to our understanding of the marine fate of land-derived OC from the Siberian Arctic. The mobilization of topsoil OC is expected to grow in magnitude with climate warming and associated active layer deepening. This translocated topsoil OC component was found to be highly degraded, which suggests degradation during transport and a possible contribution to atmospheric carbon dioxide. Similarly, the yedoma ICD-OC (and or old mineral soil carbon) may become a stronger source with accelerated warming, but slow degradation may limit its impact on active carbon cycling in the Siberian Shelf Seas.

Place, publisher, year, edition, pages
Stockholm: Department of Environmental Science and Analytical Chemistry, Stockholm University , 2015. , 40 p.
Keyword [en]
organic carbon, degradation, microcosm, incubation, terrestrial biomarkers, acyl lipids, lignin phenols, radiocarbon, Eurasian Arctic shelf, East Siberian Sea, Laptev Sea, Lena River, colloidal matter, particulate matter, sedimentary matter
National Category
Earth and Related Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
URN: urn:nbn:se:su:diva-116876ISBN: 978-91-7649-195-9 (print)OAI: oai:DiVA.org:su-116876DiVA: diva2:809319
Public defence
2015-06-11, De Geersalen, Geovetenskapens hus, Svante Arrhenius väg 14, Stockholm, 13:00 (English)
Opponent
Supervisors
Note

At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 3: Manuscript. Paper 4: Manuscript.

Available from: 2015-05-20 Created: 2015-05-01 Last updated: 2015-05-29Bibliographically approved
List of papers
1. Carbon isotopes and lipid biomarker investigation of sources, transport and degradation of terrestrial organic matter in the Buor-Khaya Bay, SE Laptev Sea
Open this publication in new window or tab >>Carbon isotopes and lipid biomarker investigation of sources, transport and degradation of terrestrial organic matter in the Buor-Khaya Bay, SE Laptev Sea
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2011 (English)In: Biogeosciences, ISSN 1726-4170, E-ISSN 1726-4189, Vol. 8, no 7, 1865-1879 p.Article in journal (Refereed) Published
Abstract [en]

The world's largest continental shelf, the East Siberian Shelf Sea, receives substantial input of terrestrial organic carbon (terr-OC) from both large rivers and erosion of its coastline. Degradation of organic matter from thawing permafrost in the Arctic is likely to increase, potentially creating a positive feedback mechanism to climate warming. This study focuses on the Buor-Khaya Bay (SE Laptev Sea), an area with strong terr-OC input from both coastal erosion and the Lena river. To better understand the fate of this terr-OC, molecular (acyl lipid biomarkers) and isotopic tools (stable carbon and radiocarbon isotopes) have been applied to both particulate organic carbon (POC) in surface water and sedimentary organic carbon (SOC) collected from the underlying surface sediments. Clear gradients in both extent of degradation and differences in source contributions were observed both between surface water POC and surface sediment SOC as well as over the 100 s km investigation scale (about 20 stations). Depleted delta(13)C-OC and high HMW/LMW n-alkane ratios signaled that terr-OC was dominating over marine/planktonic sources. Despite a shallow water column (10-40 m), the isotopic shift between SOC and POC varied systematically from +2 to +5 per mil for delta(13)C and from +300 to +450 for Delta(14)C from the Lena prodelta to the Buor-Khaya Cape. At the same time, the ratio of HMW n-alkanoic acids to HMW n-alkanes as well as HMW n-alkane CPI, both indicative of degradation, were 5-6 times greater in SOC than in POC. This suggests that terr-OC was substantially older yet less degraded in the surface sediment than in the surface waters. This unusual vertical degradation trend was only recently found also for the central East Siberian Sea. Numerical modeling (Monte Carlo simulations) with delta(13)C and Delta(14)C in both POC and SOC was applied to deduce the relative contribution of - plankton OC, surface soil layer OC and yedoma/mineral soil OC. This three end-member dual-carbon-isotopic mixing model suggests quite different scenarios for the POC vs SOC. Surface soil is dominating (63 +/- 10 %) the suspended organic matter in the surface water of SE Laptev Sea. In contrast, the yedoma/mineral soil OC is accounting for 60 +/- 9% of the SOC. We hypothesize that yedoma-OC, associated with mineral-rich matter from coastal erosion is ballasted and thus quickly settles to the bottom. The mineral association may also explain the greater resistance to degradation of this terr-OC component. In contrast, more amorphous humic-like and low-density terr-OC from surface soil and recent vegetation represents a younger but more bioavailable and thus degraded terr-OC component held buoyant in surface water. Hence, these two terr-OC components may represent different propensities to contribute to a positive feedback to climate warming by converting OC from coastal and inland permafrost into CO(2).

National Category
Environmental Sciences Geosciences, Multidisciplinary Ecology
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-66878 (URN)10.5194/bg-8-1865-2011 (DOI)000294153700009 ()
Funder
EU, FP7, Seventh Framework Programme, 220424
Note

authorCount :8

Available from: 2011-12-22 Created: 2011-12-21 Last updated: 2017-12-08Bibliographically approved
2. Contrasting regimes for organic matter degradation in the East Siberian Sea and the Laptev Sea assessed through microbial incubations and molecular markers
Open this publication in new window or tab >>Contrasting regimes for organic matter degradation in the East Siberian Sea and the Laptev Sea assessed through microbial incubations and molecular markers
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2015 (English)In: Marine Chemistry, ISSN 0304-4203, E-ISSN 1872-7581, Vol. 170, 11-22 p.Article in journal (Refereed) Published
Abstract [en]

Compositional studies of organic matter on the East Siberian Arctic Shelf (ESAS) suggest that different terrestrial carbon pools have different propensities for transport and/or degradation. The current study combined laboratory-based microbial degradation experiments with earlier published degradation-diagnostic composition of several classes of terrestrial biomarkers on the same sediments to investigate differences and driving forces of terrestrial organic matter (TerrOM) degradation in two biogeochemically-contrasting regimes of the ESAS. The incubation-based anaerobic degradation rates were consistently higher (by average factor of 6) in the East Siberian Sea Kolyma Paleoriver Channel (ESS-KPC) (15 mu mol CO2 g OC-1 day(-1)) compared to the Laptev Sea Buor-Khaya Bay (LS-BKB) (2.4 mu mol CO2 g OC-1 day(-1)). The reported molecular markers show similarities between the terrestrial carbon pools in the two systems, but impose contrasting degradation regimes in combination with the incubation results. For the LS-BKB, there was a strong relationship between the degradation rates and the three lignin phenol-based degradation proxies (r(2) = 0.93-0.96, p < 0.01, linear regression) and two wax lipid-based degradation proxies (r(2) = 0.71 and 0.66, p < 0.05, linear regression). In contrast, for the ESS-KPC system, there was no relationship between incubation-based degradation rates and molecular marker-based degradation status of TerrOM. A principal component analysis indicated that short-chain fatty acids and dicarboxylic acids from CuO oxidation are mainly of terrestrial origin in the LS-BKB, but mainly of marine origin in the ESS-KPC. Hence, the microbial degradation in the western (LS-BKB) system appears to be fueled by TerrOM whereas the eastern (ESS-KPC) system degradation appears to be driven by MarOM. By combining molecular fingerprinting of TerrOM degradation state with laboratory-based degradation studies on the same ESAS sediments, a picture evolves of two distinctly different modes of TerrOM degradation in different parts of the ESAS system.

Keyword
Organic matter lability, Reactivity, Decomposition, Remineralization, Terrestrial organic carbon, Incubations, Arctic Ocean, Coastal shelf, Continental margin, Permafrost, Wax lipids, Lignin, CuO oxidation, Organic geochemistry, Sediment
National Category
Chemical Sciences Oceanography, Hydrology, Water Resources
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-116604 (URN)10.1016/j.marchem.2014.12.005 (DOI)000350938900002 ()
Note

AuthorCount:7;

Available from: 2015-05-04 Created: 2015-04-22 Last updated: 2017-12-04Bibliographically approved
3. Different sources and degradation state of dissolved, particulate and sedimentary organic matter along the Eurasian Arctic coastal margin
Open this publication in new window or tab >>Different sources and degradation state of dissolved, particulate and sedimentary organic matter along the Eurasian Arctic coastal margin
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

Thawing of permafrost in the Eurasian Arctic causes massive fluvial and erosional releases of both dissolved and particulate organic carbon (DOC and POC) to coastal waters. Here we investigate how different sources and extent of degradation of remobilized terrestrial carbon pools imprint on major recipient carbon pools and thereby affect large-scale carbon cycling.  The molecular and dual-isotope composition is compared with source end-member composition in waterborne high-molecular weight DOC (>1kD, a.k.a. colloidal OC), POC and in sedimentary OC (SOC) along coastal Kara, Laptev and East Siberian Seas.

The lignin phenol fingerprint demonstrates a clear geospatial trend in the relative contribution of different terrestrial sources to coastal OC in going from the west to the east.  The wax lipids and cutins were much less abundant in the COC compared to in the POC and SOC compartment, suggesting that different terrestrial carbon pools partition into different aquatic carrier phases.  The Δ14C signal suggests that the COC is overwhelmingly derived from contemporary carbon sources. Furthermore, degradation proxies based on terrestrial lignin phenol biomarkers suggest a highly degraded COC composition. Monte Carlo based source apportionment simulations of the δ13C/Δ14C composition constrained that the COC is dominated by terrestrial OC from topsoil permafrost (65%) and marine plankton (25%) with smaller contribution from Ice Complex Deposit (ICD) and other older stocks of permafrost carbon (9%). This contrasts starkly to the POC and especially the SOC compartment, which are dominated by old C from ICD-OC permafrost.

These results combine with other recent studies to suggest a pattern along the East Siberian Arctic margin of SOC being constantly older yet less degraded than water column POC. This study also extends this perspective spatially along the Eurasian Arctic seaboard and also to the large COC (HMW DOC) pool, which is even younger yet even more degraded than the POC. An implication is that DOC and POC pools need to be treated separately in assessments of effects on the large-scale carbon cycle (and climate feedback) of old carbon released from thawing permafrost to aquatic receptors across the Eurasian Arctic coast. 

Keyword
organic carbon, terrestrial biomarkers, acyl lipids, lignin phenols, radiocarbon, Eurasian Arctic shelf, East Siberian Sea, Laptev Sea, Lena River, colloidal matter, particulate matter, sedimentary matter
National Category
Earth and Related Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-116871 (URN)
Available from: 2015-05-01 Created: 2015-05-01 Last updated: 2016-01-29Bibliographically approved
4. Contrasting sources of dissolved and particulate organic matter along 62N-72N in the Siberian-Arctic Lena River
Open this publication in new window or tab >>Contrasting sources of dissolved and particulate organic matter along 62N-72N in the Siberian-Arctic Lena River
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

The Lena River transports large amounts of sediment and dissolved organic matter to the shallow Laptev Sea, where it may be subject to degradation and potential release of OC. We studied organic matter collected in summer 2008, along a 1450 km section of the Lena River, from near Yakutsk at 62°N to the deltaic region at 72°N, to better understand potential in-river processing of the terrestrial particulate and dissolved fractions in the river surface water.

Carbon isotopes (δ13C and Δ14C) and plant wax lipid markers combine to reveal two distinct OC pools with different behavior in the river. The molar OC/TN ratios for POC were low (6-13) which suggests contribution from (freshwater) plankton, but most of the POC was of old age (770-4500 14C years) which rather suggests a pre-aged origin - perhaps from erosion of riverbank permafrost material. Much in contrast, COC was young (20-440 14C years) and displayed a high OC/TN composition (23-56) with a steady δ13C signal along the river course (-26.7 to -27.7). There was an apparent absence of ice complex deposit permafrost (mineral soil/yedoma OC) in the COC fraction, and only small contributions to POC. The COC signal suggest contribution from contemporary plant detritus/surface soil OC. It seems as if pre-aged permafrost OC, potentially from riverbank erosion, partitions into the particulate pool and almost not at all to the DOC/COC pool.

Degradation markers indicate a highly degraded COC lipid pool and a less degraded POC - the n-alkane carbon preference index (CPI, C24-C34) was 1.0-1.3 for COC and 1.2-4.9 (on average 3.3) for POC.

Taken together DOC/COC and POC have clearly different terrestrial sources and different fates on its way to the shelf waters. Previously freeze-locked old permafrost OC remobilizes into the Lena River in particulate form which (at least temporarily) escapes degradation as it follows the river course seawards in a less degraded state.

Keyword
organic carbon, stabel carbon, radiocarbon, isotopes, Lena River, colloidal matter, particulate matter
National Category
Earth and Related Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-116872 (URN)
Available from: 2015-05-01 Created: 2015-05-01 Last updated: 2016-01-29Bibliographically approved

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