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25th International Meeting on Organic Geochemistry IMOG 2011

25th International Meeting on Organic Geochemistry IMOG 2011

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O-56<br />

The two largest soil organic matter pools in Arctic permafrost<br />

show different degradati<strong>on</strong> potentials up<strong>on</strong> coastal expulsi<strong>on</strong><br />

Örjan Gustafss<strong>on</strong> 1 , Jorien V<strong>on</strong>k 1,5 , Emma Karlss<strong>on</strong> 1 , Laura Sanchez-Garcia 1 , Bart van<br />

D<strong>on</strong>gen 1,2 , Igor Semiletov 3,4 , Oleg Dudarev 4 , Alex Charkin 4 , Tim Eglint<strong>on</strong> 5 , August<br />

Anderss<strong>on</strong> 1<br />

1 Stockholm University, Stockholm, Sweden, 2 University of Manchester, Manchester, United Kingdom, 3 IARC,<br />

University of Alaska, Fairbanks, United States of America, 4 Russian Academy of Sciences, Vladivostok,<br />

Russian Federati<strong>on</strong>, 5 ETH, Zürich, Switzerland (corresp<strong>on</strong>ding author:orjan.gustafss<strong>on</strong>@itm.su.se)<br />

About half of global soil organic carb<strong>on</strong> (OC) resides<br />

in the top three meters of circum-Arctic permafrost.<br />

Climate warming, particularly amplified over the<br />

Arctic, may lead to permafrost thawing and the<br />

potential for degradati<strong>on</strong> of its organic matter to<br />

greenhouse gases, a positive feedback to climate<br />

warming. However, our mechanistic understanding of<br />

the fate of Arctic soil OC in a warming climate is poor.<br />

The shelf seas around the Eurasian Arctic, the world‘s<br />

largest c<strong>on</strong>tinental shelf, provide an integrating<br />

window <strong>on</strong> the sources and fate of terrestrial organic<br />

matter (terrOM) exported from its vast drainage<br />

basins. Our investigati<strong>on</strong>s are applying lipid biomarker<br />

and 13C+14C analysis of the exported terrOM in both<br />

particulate organic carb<strong>on</strong> (POC) in surface water and<br />

sedimentary organic carb<strong>on</strong> (SOC) collected from the<br />

underlying surface sediments to deduce (a) the<br />

relative c<strong>on</strong>tributi<strong>on</strong> of various soil OC pools and (b)<br />

the propensity of the different terrestrial OC pools to<br />

degrade in the marine recipient.<br />

Clear gradients in both molecular and isotopic signals<br />

of source c<strong>on</strong>tributi<strong>on</strong>s and the extent of degradati<strong>on</strong><br />

were observed both between surface water POC and<br />

surface sediment SOC as well as over distance away<br />

from the coast in three targeted systems; the SE<br />

Laptev Sea, the central East Siberian Sea and the<br />

northernmost sub-Arctic Baltic Sea. Depleted d13C-<br />

OC and high HMW/LMW n-alkane ratios in both SOC<br />

and POC signaled that terrOM was dominating over<br />

marine/plankt<strong>on</strong>ic sources in all three systems.<br />

Despite shallow water columns (10-50 m) in the<br />

Laptev and East Siberian Seas, there was a large<br />

isotopic shift in D14C between SOC and POC of +300<br />

to +450 per mil. At the same time, the ratio of HMW<br />

n-alkanoic acids to HMW n-alkanes was much greater<br />

in the SOC than in the POC. Taken together, this<br />

suggests that the terrOM in the surface sediment was<br />

substantially older yet less degraded than in the<br />

surface waters. This degradati<strong>on</strong> trend is c<strong>on</strong>trary to<br />

what is normally observed.<br />

Numerical modeling that allowed accounting for the<br />

uncertainty in end-member compositi<strong>on</strong>, was applied<br />

to 13C and 14C in both POC and SOC to deduce the<br />

relative c<strong>on</strong>tributi<strong>on</strong> of – marine OC, soil OC from the<br />

annual thaw layer and OC from Yedoma/mineral soil.<br />

This three end-member dual-carb<strong>on</strong>-isotopic mixing<br />

model suggests quite different scenarios for the POC<br />

vs the SOC. Surface soil is dominating (63±10%) in<br />

surface water POC of SE Laptev Sea. In c<strong>on</strong>trast, the<br />

Yedoma/mineral soil OC is accounting for 60±9% of<br />

the surface sediment OC in the SE Laptev Sea and<br />

55±12% in the central East Siberian Sea.<br />

We hypothesize, that Yedoma-OC, associated with<br />

heavy mineral-rich matter is ballasted and quickly<br />

settles out. This mineral associati<strong>on</strong> is also likely to<br />

explain the greater resistance to degradati<strong>on</strong> of this<br />

terrOM comp<strong>on</strong>ent in the marine envir<strong>on</strong>ment due to<br />

physical protecti<strong>on</strong> against microbial enzymes. In<br />

c<strong>on</strong>trast, more humic-like (amorphous and buoyant)<br />

terrOM from surface soil and recent vegetati<strong>on</strong><br />

represents the younger, more bioavailable and thus<br />

degraded terrOM comp<strong>on</strong>ent of the surface waters.<br />

To address whether intrinsic chemical resistance or<br />

physical protecti<strong>on</strong> is the dominant factor in this large<br />

difference in degradati<strong>on</strong> potential between the<br />

surface soil vs mineral soil comp<strong>on</strong>ents from these<br />

high latitudes, compound-specific radiocarb<strong>on</strong><br />

analysis (CSRA) was applied. CSRA of identical<br />

HMW n-alkanes and HMW n-alkanoic acids were<br />

performed al<strong>on</strong>g an offshore transect from the mouth<br />

of the Kalix River to the central Bothnian Bay in<br />

northernmost Baltic Sea. The CSRA was performed<br />

both in SOC and here, for the first time, also in<br />

seawater POC. The CSRA revealed a remarkable<br />

fracti<strong>on</strong>ati<strong>on</strong> for structurally identical vascular plant<br />

markers (�400 ‰). This corresp<strong>on</strong>ds to an ―aging‖ of<br />

�6000 years in a system where the hydraulic and<br />

settling transport times are <strong>on</strong> the order of m<strong>on</strong>ths – a<br />

few years. The data suggest that identical lipid<br />

biomarkers of different reservoir ages and different<br />

physical protecti<strong>on</strong>s exhibit different propensity to<br />

degradati<strong>on</strong>. Hence, these two soil OC comp<strong>on</strong>ents<br />

also represent different propensity to c<strong>on</strong>tribute to a<br />

positive feedback to Arctic climate warming.<br />

117

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