Biogeochemistry of organic carbon, CO2, CH4, and trace elements in thermokarst water bodies in discontinuous permafrost zones of Western Siberia

2012 ◽  
Vol 113 (1-3) ◽  
pp. 573-593 ◽  
Author(s):  
L. S. Shirokova ◽  
O. S. Pokrovsky ◽  
S. N. Kirpotin ◽  
C. Desmukh ◽  
B. G. Pokrovsky ◽  
...  
2017 ◽  
Vol 14 (14) ◽  
pp. 3561-3584 ◽  
Author(s):  
Tatiana V. Raudina ◽  
Sergey V. Loiko ◽  
Artyom G. Lim ◽  
Ivan V. Krickov ◽  
Liudmila S. Shirokova ◽  
...  

Abstract. Mobilization of dissolved organic carbon (DOC) and related trace elements (TEs) from the frozen peat to surface waters in the permafrost zone is expected to enhance under ongoing permafrost thaw and active layer thickness (ALT) deepening in high-latitude regions. The interstitial soil solutions are efficient tracers of ongoing bio-geochemical processes in the critical zone and can help to decipher the intensity of carbon and metals migration from the soil to the rivers and further to the ocean. To this end, we collected, across a 640 km latitudinal transect of the sporadic to continuous permafrost zone of western Siberia peatlands, soil porewaters from 30 cm depth using suction cups and we analyzed DOC, dissolved inorganic carbon (DIC), and 40 major elements and TEs in 0.45 µm filtered fraction of 80 soil porewaters. Despite an expected decrease in the intensity of DOC and TE mobilization from the soil and vegetation litter to the interstitial fluids with the increase in the permafrost coverage and a decrease in the annual temperature and ALT, the DOC and many major and trace elements did not exhibit any distinct decrease in concentration along the latitudinal transect from 62.2 to 67.4° N. The DOC demonstrated a maximum of concentration at 66° N, on the border of the discontinuous/continuous permafrost zone, whereas the DOC concentration in peat soil solutions from the continuous permafrost zone was equal to or higher than that in the sporadic/discontinuous permafrost zone. Moreover, a number of major (Ca, Mg) and trace (Al, Ti, Sr, Ga, rare earth elements (REEs), Zr, Hf, Th) elements exhibited an increasing, not decreasing, northward concentration trend. We hypothesize that the effects of temperature and thickness of the ALT are of secondary importance relative to the leaching capacity of peat, which is in turn controlled by the water saturation of the peat core. The water residence time in peat pores also plays a role in enriching the fluids in some elements: the DOC, V, Cu, Pb, REEs, and Th were a factor of 1.5 to 2.0 higher in mounds relative to hollows. As such, it is possible that the time of reaction between the peat and downward infiltrating waters essentially controls the degree of peat porewater enrichments in DOC and other solutes. A 2° northward shift in the position of the permafrost boundaries may bring about a factor of 1.3 ± 0.2 decrease in Ca, Mg, Sr, Al, Fe, Ti, Mn, Ni, Co, V, Zr, Hf, Th, and REE porewater concentration in continuous and discontinuous permafrost zones, and a possible decrease in DOC, specific ultraviolet absorbency (SUVA), Ca, Mg, Fe, and Sr will not exceed 20 % of their current values. The projected increase in ALT and vegetation density, northward migration of the permafrost boundary, or the change of hydrological regime is unlikely to modify chemical composition of peat porewater fluids larger than their natural variations within different micro-landscapes, i.e., within a factor of 2. The decrease in DOC and metal delivery to small rivers and lakes by peat soil leachate may also decrease the overall export of dissolved components from the continuous permafrost zone to the Arctic Ocean. This challenges the current paradigm on the increase in DOC export from the land to the ocean under climate warming in high latitudes.


2011 ◽  
Vol 8 (11) ◽  
pp. 3341-3358 ◽  
Author(s):  
S. Audry ◽  
O. S. Pokrovsky ◽  
L. S. Shirokova ◽  
S. N. Kirpotin ◽  
B. Dupré

Abstract. This study reports the very first results on high-resolution sampling of sediments and their porewaters from three thermokarst (thaw) lakes representing different stages of ecosystem development located within the Nadym-Pur interfluve of the Western Siberia plain. Up to present time, the lake sediments of this and other permafrost-affected regions remain unexplored regarding their biogeochemical behavior. The aim of this study was to (i) document the early diagenesic processes in order to assess their impact on the organic carbon stored in the underlying permafrost, and (ii) characterize the post-depositional redistribution of trace elements and their impact on the water column. The estimated organic carbon (OC) stock in thermokarst lake sediments of 14 ± 2 kg m−2 is low compared to that reported for peat soils from the same region and denotes intense organic matter (OM) mineralization. Mineralization of OM in the thermokarst lake sediments proceeds under anoxic conditions in all the three lakes. In the course of the lake development, a shift in mineralization pathways from nitrate and sulfate to Fe- and Mn-oxyhydroxides as the main terminal electron acceptors in the early diagenetic reactions was suggested. This shift was likely promoted by the diagenetic consumption of nitrate and sulfate and their gradual depletion in the water column due to progressively decreasing frozen peat lixiviation occurring at the lake's borders. Trace elements were mobilized from host phases (OM and Fe- and Mn-oxyhydroxides) and partly sequestered in the sediment in the form of authigenic Fe-sulfides. Arsenic and Sb cycling was also closely linked to that of OM and Fe- and Mn-oxyhydroxides. Shallow diagenetic enrichment of particulate Sb was observed in the less mature stages. As a result of authigenic sulfide precipitation, the sediments of the early stage of ecosystem development were a sink for water column Cu, Zn, Cd, Pb and Sb. In contrast, at all stages of ecosystem development, the sediments were a source of dissolved Co, Ni and As to the water column. However, the concentrations of these trace elements remained low in the bottom waters, indicating that sorption processes on Fe-bounding particles and/or large-size organo-mineral colloids could mitigate the impact of post-depositional redistribution of toxic elements on the water column.


2017 ◽  
Author(s):  
Tatiana V. Raudina ◽  
Sergey V. Loiko ◽  
Artyom Lim ◽  
Ivan V. Krickov ◽  
Liudmila S. Shirokova ◽  
...  

Abstract. Mobilization of dissolved organic carbon (DOC) and related trace elements (TE) from the frozen peat to surface waters in the permafrost zone is one the major consequence of on-going permafrost thaw and active layer thickness (ALT) rise in high latitude regions. The interstitial soil solutions are efficient tracers of on-going bio-geochemical processes in the critical zone and can help to decipher the intensity of carbon and metals migration from the soil to the rivers and further to the ocean. To this end, we collected, across a 640 km latitudinal transect of sporadic to continuous permafrost zone of western Siberia peatlands, soil porewaters from 30 cm depth using suction cups and we analyzed DOC, DIC and 40 major and TE in 0.45 µm filtered fraction of 80 soil porewaters. Despite an expected decrease of the intensity of DOC and TE mobilization from the soil and vegetation litter to the interstitial fluids with the increase of the permafrost coverage, decrease in the annual temperature and ALT, the DOC and many major and trace element did not exhibit any distinct decrease in concentration along the latitudinal transect from 62.2° N to 67.4° N. The DOC demonstrated a maximum of concentration at 66° N, on the border of discontinuous/continuous permafrost zone, whereas the DOC concentration in peat soil solutions from continuous permafrost zone was equal or higher than that in sporadic/discontinuous permafrost zone. Moreover, a number of major (Ca, Mg) and trace (Al, Ti, Sr, Ga, REEs, Zr, Hf, Th) elements exhibited an increasing, not decreasing northward concentration trend. We hypothesize that the effect of temperature and thickness of the ALT are of secondary importance relative to the leaching capacity of peat which is in turn controlled by the water saturation of the peat core. The water residence time in peat pores also plays a role in enriching the fluids in some elements: the DOC, V, Cu, Pb, REE, Th were a factor of 1.5 to 2.0 higher in mounds relative to hollows. As such, it is possible that the time of reaction between the peat and downward infiltrating waters essentially controls the degree of peat pore-water enrichments in DOC and other solutes. A two-degree northward shift in the position of the permafrost boundaries may bring about a factor of 1.3 decrease in Ca, Mg, Sr, Al, Fe, Ti, Mn, Ni, Co, V, Zr, Hf, Th and REE porewater concentration in continuous and discontinuous permafrost zones, and a possible decrease in DOC, SUVA, Ca, Mg, Fe and Sr will not exceed 20 % of their actual values. The projected increase of ALT and vegetation density, northward migration of the permafrost boundary, or the change of hydrological regime are unlikely to modify chemical composition of peat pore water fluids larger than their natural variations within different micro-landscapes, i.e., within a factor of 2.


Geoderma ◽  
2021 ◽  
Vol 390 ◽  
pp. 114971
Author(s):  
Tatiana V. Raudina ◽  
Sergey V. Loiko ◽  
Daria M. Kuzmina ◽  
Liudmila S. Shirokova ◽  
Sergey P. Kulizhskiy ◽  
...  

2011 ◽  
Vol 8 (4) ◽  
pp. 8845-8894
Author(s):  
S. Audry ◽  
O. S. Pokrovsky ◽  
L. S. Shirokova ◽  
S. N. Kirpotin ◽  
B. Dupré

Abstract. This study reports the very first results on high-resolution sampling of sediments and their porewaters from three thermokarst (thaw) lakes representing different stages of ecosystem development located within the Nadym-Pur interfluve of the Western Siberia plain. Up to present time, the lake sediments of this and other permafrost-affected regions remain unexplored regarding their biogeochemical behavior. The aim of this study was to (i) document the early diagenesic processes in order to assess their impact on the organic carbon stored in the underlying permafrost, and (ii) characterize the post-depositional redistribution of trace elements and their impact on the water column. The estimated organic carbon (OC) stock in thermokarst lake sediments of 14 ± 2 kg m−2 is low compared to that reported for peat soils from the same region and denotes intense organic matter (OM) mineralization. Mineralization of OM in the thermokarst lake sediments proceeds under anoxic conditions in all the three lakes. In the course of the lake development, a shift in mineralization pathways was evidenced from nitrate and sulfate to Fe- and Mn-oxyhydroxides as the main terminal electron acceptors in the early diagenetic reactions. This shift was promoted by the diagenetic consumption of nitrate and sulfate and their gradual depletion in the water column due to progressively decreasing frozen peat lixiviation occurring at the lake's borders. Trace elements were mobilized from host phases (OM and Fe- and Mn-oxyhydroxides) and partly sequestered in the sediment in the form of authigenic Fe-sulfides. Arsenic and Sb cycling was also closely linked to that of OM and Fe- and Mn-oxyhydroxides. Shallow diagenetic enrichment of particulate Sb was observed in the less mature stages. As a result of authigenic sulfide precipitation, the sediments of the early stage of ecosystem development were a sink for water column Cu, Zn, Cd, Pb and Sb. In contrast, at all stages of ecosystem development, the sediments were a source of dissolved Co, Ni and As to the water column. However, the concentrations of these trace elements remained low in the bottom waters, indicating that sorption processes on Fe-bounding particles and/or large-size organo-mineral colloids could mitigate the impact of post-depositional redistribution of toxic elements on the water column.


2016 ◽  
Author(s):  
Zhaolian Ye ◽  
Jiashu Liu ◽  
Aijun Gu ◽  
Feifei Feng ◽  
Yuhai Liu ◽  
...  

Abstract. Knowledge on aerosol chemistry in densely populated regions is critical for reduction of air pollution, while such studies haven't been conducted in Changzhou, an important manufacturing base and polluted city in the Yangtze River Delta (YRD), China. This work, for the first time, performed a thorough chemical characterization on the fine particular matter (PM2.5) samples, collected during July 2015 to April 2016 across four seasons in Changzhou city. A suite of analytical techniques were employed to characterize organic carbon / elemental carbon (OC / EC), water-soluble organic carbon (WSOC), water-soluble inorganic ions (WSIIs), trace elements, and polycyclic aromatic hydrocarbons (PAHs) in PM2.5; in particular, an Aerodyne soot particle aerosol mass spectrometer (SP-AMS) was deployed to probe the chemical properties of water-soluble organic aerosols (WSOA). The average PM2.5 concentrations were found to be 108.3 μg m−3, and all identified species were able to reconstruct ~ 80 % of the PM2.5 mass. The WSIIs occupied about half of the PM2.5 mass (~ 52.1 %), with SO42−, NO3− and NH4+ as the major ions. On average, nitrate concentrations dominated over sulfate (mass ratio of 1.21), indicating influences from traffic emissions. OC and EC correlated well with each other and the highest OC / EC ratio (5.16) occurred in winter, suggesting complex OC sources likely including both secondarily formed and primarily emitted OA. Concentrations of eight trace elements (Mn, Zn, Al, B, Cr, Cu, Fe, Pb) can contribute up to 6.0 % of PM2.5 during winter. PAHs concentrations were also high in winter (140.25 ng m−3), which were predominated by median/high molecular weight PAHs with 5- and 6-rings. The organic matter including both water-soluble and water-insoluble species occupied ~ 20 % PM2.5 mass. SP-AMS determined that the WSOA had an average atomic oxygen-to-carbon (O / C), hydrogen-to-carbon (H / C), nitrogen-to-carbon (N / C) and organic matter-to-organic carbon (OM / OC) ratios of 0.36, 1.54, 0.11, and 1.74, respectively. Source apportionment of WSOA further identified two secondary OA (SOA) factors (a less oxidized and a more oxidized OA) and two primary OA (POA) factors (a nitrogen enriched hydrocarbon-like traffic OA and a cooking-related OA). On average, the POA contribution overweighed SOA (55 % vs. 45 %), indicating the important role of local anthropogenic emissions to the aerosol pollution in Changzhou. Our measurement also shows the abundance of organic nitrogen species in WSOA, and the source analyses suggest these species likely associated with traffic emissions, which warrants more investigations on PM samples from other locations.


Sign in / Sign up

Export Citation Format

Share Document