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Articles (Coppola Et Al., 2014; Salvadó Et Al., 2017; Ing “Old” Carbon That Has Been Stored in Deep Permafrost for Winiger Et Al., 2017)

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Articles (Coppola Et Al., 2014; Salvadó Et Al., 2017; Ing “Old” Carbon That Has Been Stored in Deep Permafrost for Winiger Et Al., 2017) The Cryosphere, 12, 3293–3309, 2018 https://doi.org/10.5194/tc-12-3293-2018 © Author(s) 2018. This work is distributed under the Creative Commons Attribution 4.0 License. Carbonaceous material export from Siberian permafrost tracked across the Arctic Shelf using Raman spectroscopy Robert B. Sparkes1, Melissa Maher1, Jerome Blewett2,a, Ayça Dogrul˘ Selver2,3, Örjan Gustafsson4, Igor P. Semiletov5,6,7, and Bart E. van Dongen2 1School of Science and the Environment, Manchester Metropolitan University, Manchester, UK 2School of Earth and Environmental Sciences and Williamson Research Centre for Molecular Environmental Science, University of Manchester, Manchester, UK 3Balıkesir University, Geological Engineering Department, Balıkesir, Turkey 4Department of Environmental Science and Analytical Chemistry (ACES) and the Bolin Centre for Climate Research, Stockholm University, Stockholm, Sweden 5Pacific Oceanological Institute Far Eastern Branch of the Russian Academy of Sciences, Vladivostok, Russia 6International Arctic Research Center, University of Alaska, Fairbanks, USA 7National Tomsk Research Polytechnic University, Tomsk, Russia anow at: Organic Geochemistry Unit, School of Chemistry, Cabot Institute, University of Bristol, Bristol, UK Correspondence: Robert B. Sparkes ([email protected]) Received: 19 January 2018 – Discussion started: 9 March 2018 Revised: 17 August 2018 – Accepted: 6 September 2018 – Published: 11 October 2018 Abstract. Warming-induced erosion of permafrost from grades much more slowly than lipid biomarkers and other Eastern Siberia mobilises large amounts of organic carbon traditional tracers of terrestrial organic matter and shows that and delivers it to the East Siberian Arctic Shelf (ESAS). alongside degradation of the more labile organic matter com- In this study Raman spectroscopy of carbonaceous material ponent there is also conservative transport of carbon across (CM) was used to characterise, identify and track the most re- the shelf toward the deep ocean. Thus, carbon cycle calcula- calcitrant fraction of the organic load: 1463 spectra were ob- tions must consider the nature as well as the amount of car- tained from surface sediments collected across the ESAS and bon liberated from thawing permafrost and other erosional automatically analysed for their Raman peaks. Spectra were settings. classified by their peak areas and widths into disordered, in- termediate, mildly graphitised and highly graphitised groups and the distribution of these classes was investigated across the shelf. Disordered CM was most prevalent in a permafrost 1 Introduction core from Kurungnakh Island and from areas known to have high rates of coastal erosion. Sediments from outflows of the Extensive Northern Hemisphere permafrost deposits contain Indigirka and Kolyma rivers were generally enriched in inter- approximately 40 % of the global soil organic carbon (OC) mediate CM. These different sediment sources were identi- budget (Schuur et al., 2015; Tarnocai et al., 2009). The ma- fied and distinguished along an E–W transect using their Ra- jority of this carbon is currently freeze-locked, but rapid man spectra, showing that sediment is not homogenised on warming at high latitudes is making it increasingly vulner- the ESAS. Distal samples, from the ESAS slope, contained able to mobilisation via fluvial and coastal erosion. Thawing greater amounts of highly graphitised CM compared to the also leads to degradation, both in situ and post-mobilisation, rest of the shelf, attributable to degradation or, more likely, to greenhouse gases, providing a positive feedback response winnowing processes offshore. The presence of all four spec- to warming (Stendel and Christensen, 2002; Vonk et al., tral classes in distal sediments demonstrates that CM de- 2010, 2015). The Eurasian Arctic region contains the major- ity of Northern Hemisphere permafrost OC, and the release Published by Copernicus Publications on behalf of the European Geosciences Union. 3294 R. B. Sparkes et al.: Siberian carbonaceous material export rate of both OC and sediment from this area into the Arc- investigated CM in tropical and subtropical settings, but, in tic Ocean is predicted to rise during the next century (van contrast to extractable OC, no work has been done to charac- Dongen et al., 2008; Holmes et al., 2002, 2012; O’Donnell terise or trace CM in the Arctic. The only studies on recalci- et al., 2014; Peterson et al., 2002). Deepening hydrologi- trant Arctic OC involve (usually submicron-sized) soot black cal flow paths and thermokarst erosion events are mobilis- carbon particles (Coppola et al., 2014; Salvadó et al., 2017; ing “old” carbon that has been stored in deep permafrost for Winiger et al., 2017). thousands of years (Gustafsson et al., 2011; Feng et al., 2013, Salvadó et al.(2017) measured the distribution of soot 2015; Vonk et al., 2012; Vonk and Gustafsson, 2013; IPCC, black carbon (SBC) across the ESAS. SBC was isolated us- 2013). OC delivered by fluvial erosion and transport has been ing chemothermal oxidation at 375 ◦C, a method that has identified offshore using molecular biomarkers and has been been thoroughly tested to isolate combustion-derived SBC shown to deposit and/or degrade rapidly on the shelf (Bröder from other recalcitrant species (such as coal of various degree et al., 2016; Dogrul˘ Selver et al., 2015; Karlsson et al., 2015; of maturity, pollen and other biomacromolecules; Gustafs- Sparkes et al., 2015, 2016; Tesi et al., 2014, 2016). In ad- son et al., 2001; Elmquist et al., 2006). The highest con- dition to fluvial erosion, coastal erosion delivers a significant centrations (up to 0.22 wt%SBC) and proportions (11% of amount of sediment and OC (44±10 TgOCyr−1) to the Arc- the total OC) of SBC were found at the mouths of the Lena tic Ocean (Vonk et al., 2012). Poorly lithified coastal cliffs, and Kolyma rivers, with concentrations and proportions de- combined with stormy weather, have caused erosion rates of creasing offshore as SBC was deposited and marine pri- up to 10 myr−1 (Lantuit et al., 2011). Reducing sea ice cover, mary productivity became the dominant OC source. How- and therefore increased wave fetch and storm impact, is also ever, the relative importance of the recalcitrant SBC within likely to increase coastal erosion rates during the next cen- the permafrost-derived carbon pool increased as more labile tury (Feng et al., 2015; Stein and MacDonald, 2004; Vonk material degraded during transport. This pattern was seen et al., 2010). consistently along a W–E transect from the Laptev Sea to the Eastern ESAS. The authors concluded that the source of 1.1 Recalcitrant organic matter export from SBC was not atmospheric deposition (e.g. via biomass burn- permafrost ing) but permafrost erosion. Goñi et al.(2005) report anoma- lously old radiocarbon ages for distal sediments on the Beau- Erosion of ancient carbon from Arctic permafrost may lead fort Shelf, attributed to highly recalcitrant terrestrial OC that to degradation of carbon into greenhouse gases and a positive has been matured to kerogen grade or higher, but the nature feedback effect on global climate, or the absence of degra- and origin of the material has not been investigated in detail. dation may allow this material to be used to track eroded Therefore, there is a need to assess whether the various inputs sediment across the continental shelf. Alongside modern OC of carbon to the Arctic Ocean system can explain these old transport, erosion mobilises petrogenic OC from rocks and radiocarbon ages, and whether they form an active or passive soils (also known as carbonaceous material, CM) and deliv- part of the carbon cycle. ers this to the ocean. CM consists of recalcitrant material, This study uses Raman spectroscopy to identify the such as coal, lignite, combustion-derived black carbon, kero- sources of CM in the Eastern Siberian region and tracks the gen (insoluble hydrocarbons; Durand, 1980) and graphite, export of CM from these sources across the East Siberian which is stable over millions of years. CM is (apart from Arctic Shelf (ESAS). This is the first Raman study of sedi- black carbon) formed from the maturation of buried organic mentary CM in the Arctic. Automated Raman spectra fitting matter, with the degree of diagenesis and metamorphism procedures were used to analyse > 1400 spectra measured controlling the molecular and crystalline structure (Beyssac from CM in sediments collected across 1 million km2 of the et al., 2002b, 2003a, 2007). High temperatures during burial (ESAS). Multiple heterogeneous sources of sediment were and metamorphism drive the transition from disordered kero- studied, including several of the world’s largest river catch- gen and lignite to highly crystalline graphite, allowing CM ments and thousands of kilometres of shoreline experiencing from different areas to be identified due to differences in rapid coastal erosion (Lantuit et al., 2011). the geological history of the source rocks (Sparkes et al., 2013). CM represents a major fraction of the global OC bud- 1.2 Raman spectroscopy get, sequestered in sedimentary and metamorphic rocks over million-year timescales (Bouchez et al., 2010; Galy et al., Raman spectroscopy is a precise and powerful tool for quan- 2007; Hilton, 2008; Smith et al., 2013). Any oxidation of CM tifying the degree of crystallinity within CM (Beyssac et al., during erosion, transport and burial represents a movement of 2002a, 2003b). In this study, it is used to identify permafrost- carbon between the long-term and short-term carbon cycles. sourced CM offshore. Monochromatic incident light inter- During transport, bioavailability of CM is believed to be low, acts with the crystal lattice of the targeted particle and re- but there is evidence that extremely long transport distances flects with a changed wavelength due to the energy shift can degrade disordered CM, leaving only crystalline graphite introduced by lattice vibrations (phonons). When analysed (Bouchez et al., 2010; Galy et al., 2007). Previous work has with in a Raman spectrometer, graphitic and disordered car- The Cryosphere, 12, 3293–3309, 2018 www.the-cryosphere.net/12/3293/2018/ R.
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