Macdonald Robie W.

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Macdonald
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Robie W.
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  • Preprint
    Spatial variations in geochemical characteristics of the modern Mackenzie Delta sedimentary system
    ( 2015-01) Vonk, Jorien E. ; Giosan, Liviu ; Blusztajn, Jerzy S. ; Montlucon, Daniel B. ; Graf Pannatier, Elisabeth ; McIntyre, Cameron P. ; Wacker, Lukas ; Macdonald, Robie W. ; Yunker, Mark B. ; Eglinton, Timothy I.
    The Mackenzie River in Canada is by far the largest riverine source of sediment and organic carbon (OC) to the Arctic Ocean. Therefore the transport, degradation and burial of OC along the land-to-ocean continuum for this riverine system is important to study both regionally and as a dominant representative of Arctic rivers. Here, we apply sedimentological (grain size, mineral surface area), and organic and inorganic geochemical techniques (%OC, δ13C-OC and Δ14C-OC, 143Nd/144Nd,δ2H and δ18O, major and trace elements) on particulate, bank, channel and lake surface sediments from the Mackenzie Delta, as well as on surface sediments from the Mackenzie shelf in the Beaufort Sea. Our data show a hydrodynamic sorting effect resulting in the accumulation of finer-grained sediments in lake and shelf deposits. A general decrease in organic carbon (OC) to mineral surface area ratios from river-to-sea furthermore suggests a loss of mineral-bound terrestrial OC during transport through the delta and deposition on the shelf. The net isotopic value of the terrestrial OC that is lost en route, derived from relationships between δ13C, OC and surface area, is -28.5‰ for δ13C and -417‰ for Δ14C. We calculated that OC burial efficiencies are around 55%, which are higher (~20%) than other large river systems such as the Amazon. Old sedimentary OC ages, up to 12 14C-ky, suggest the delivery of both a petrogenic OC source (with an estimated contribution of 19±9%) as well as a pre-aged terrestrial OC source. We calculated the 14C-age of this pre-aged, biogenic, component to be about 6100 yrs, or -501‰, which illustrates that terrestrial OC in the watershed can reside for millennia in soils before being released into the river. Surface sediments in lakes across the delta (n=20) showed large variability in %OC (0.92% to 5.7%) and δ13C (-30.7‰ to -23.5‰). High-closure lakes, flooding only at exceptionally high water levels, hold high sedimentary OC contents (> 2.5%) and young biogenic OC with a terrestrial or an autochthonous source whereas no-closure lakes, permanently connected to a river channel, hold sediments with pre-aged, terrestrial OC. The intermediate low-closure lakes, flooding every year during peak discharge, display the largest variability in OC content, age and source, likely reflecting variability in for example the length of river-lake connections, the distance to sediment source and the number of intermediate settling basins. Bank, channel and suspended sediment show variable 143Nd/144Nd values, yet there is a gradual but distinct spatial transition in 143Nd/144Nd (nearly three ε units; from -11.4 to -13.9) in the detrital fraction of lake surface sediments from the western to the eastern delta. This reflects the input of younger Peel River catchment material in the west and input of older geological source material in the east, and suggests that lake sediments can be used to assess variability in source watershed patterns across the delta.
  • Article
    Carbon dynamics in the western Arctic Ocean : insights from full-depth carbon isotope profiles of DIC, DOC, and POC
    (Copernicus Publications on behalf of the European Geosciences Union, 2012-03-28) Griffith, David R. ; McNichol, Ann P. ; Xu, Li ; McLaughlin, Fiona A. ; Macdonald, Robie W. ; Brown, Kristina A. ; Eglinton, Timothy I.
    Arctic warming is projected to continue throughout the coming century. Yet, our currently limited understanding of the Arctic Ocean carbon cycle hinders our ability to predict how changing conditions will affect local Arctic ecosystems, regional carbon budgets, and global climate. We present here the first set of concurrent, full-depth, dual-isotope profiles for dissolved inorganic carbon (DIC), dissolved organic carbon (DOC), and suspended particulate organic carbon (POCsusp) at two sites in the Canada Basin of the Arctic Ocean. The carbon isotope composition of sinking and suspended POC in the Arctic contrasts strongly with open ocean Atlantic and Pacific sites, pointing to a combination of inputs to Arctic POCsusp at depth, including surface-derived organic carbon (OC), sorbed/advected OC, and OC derived from in situ DIC fixation. The latter process appears to be particularly important at intermediate depths, where mass balance calculations suggest that OC derived from in situ DIC fixation contributes up to 22% of POCsusp. As in other oceans, surface-derived OC is still a dominant source to Arctic POCsusp. Yet, we suggest that significantly smaller vertical POC fluxes in the Canada Basin make it possible to see evidence of DIC fixation in the POCsusp pool even at the bulk isotope level.
  • Article
    Multimolecular tracers of terrestrial carbon transfer across the pan-Arctic : 14C characteristics of sedimentary carbon components and their environmental controls
    (John Wiley & Sons, 2015-11-02) Feng, Xiaojuan ; Gustafsson, Orjan ; Holmes, Robert M. ; Vonk, Jorien E. ; van Dongen, Bart E. ; Semiletov, Igor P. ; Dudarev, Oleg V. ; Yunker, Mark B. ; Macdonald, Robie W. ; Wacker, Lukas ; Montlucon, Daniel B. ; Eglinton, Timothy I.
    Distinguishing the sources, ages, and fate of various terrestrial organic carbon (OC) pools mobilized from heterogeneous Arctic landscapes is key to assessing climatic impacts on the fluvial release of carbon from permafrost. Through molecular 14C measurements, including novel analyses of suberin- and/or cutin-derived diacids (DAs) and hydroxy fatty acids (FAs), we compared the radiocarbon characteristics of a comprehensive suite of terrestrial markers (including plant wax lipids, cutin, suberin, lignin, and hydroxy phenols) in the sedimentary particles from nine major arctic and subarctic rivers in order to establish a benchmark assessment of the mobilization patterns of terrestrial OC pools across the pan-Arctic. Terrestrial lipids, including suberin-derived longer-chain DAs (C24,26,28), plant wax FAs (C24,26,28), and n-alkanes (C27,29,31), incorporated significant inputs of aged carbon, presumably from deeper soil horizons. Mobilization and translocation of these “old” terrestrial carbon components was dependent on nonlinear processes associated with permafrost distributions. By contrast, shorter-chain (C16,18) DAs and lignin phenols (as well as hydroxy phenols in rivers outside eastern Eurasian Arctic) were much more enriched in 14C, suggesting incorporation of relatively young carbon supplied by runoff processes from recent vegetation debris and surface layers. Furthermore, the radiocarbon content of terrestrial markers is heavily influenced by specific OC sources and degradation status. Overall, multitracer molecular 14C analysis sheds new light on the mobilization of terrestrial OC from arctic watersheds. Our findings of distinct ages for various terrestrial carbon components may aid in elucidating fate of different terrestrial OC pools in the face of increasing arctic permafrost thaw.
  • Article
    Biomass offsets little or none of permafrost carbon release from soils, streams, and wildfire : an expert assessment
    (IOPScience, 2016-03-07) Abbott, Benjamin W. ; Jones, Jeremy B. ; Schuur, Edward A. G. ; Chapin, F. Stuart ; Bowden, William B. ; Bret-Harte, M. Syndonia ; Epstein, Howard E. ; Flannigan, Michael ; Harms, Tamara K. ; Hollingsworth, Teresa N. ; Mack, Michelle C. ; McGuire, A. David ; Natali, Susan M. ; Rocha, Adrian V. ; Tank, Suzanne E. ; Turetsky, Merritt R. ; Vonk, Jorien E. ; Wickland, Kimberly ; Aiken, George R. ; Alexander, Heather D. ; Amon, Rainer M. W. ; Benscoter, Brian ; Bergeron, Yves ; Bishop, Kevin ; Blarquez, Olivier ; Bond-Lamberty, Benjamin ; Breen, Amy L. ; Buffam, Ishi ; Cai, Yihua ; Carcaillet, Christopher ; Carey, Sean K. ; Chen, Jing M. ; Chen, Han Y. H. ; Christensen, Torben R. ; Cooper, Lee W. ; Cornelissen, Johannes H. C. ; de Groot, William J. ; DeLuca, Thomas Henry ; Dorrepaal, Ellen ; Fetcher, Ned ; Finlay, Jacques C. ; Forbes, Bruce C. ; French, Nancy H. F. ; Gauthier, Sylvie ; Girardin, Martin ; Goetz, Scott J. ; Goldammer, Johann G. ; Gough, Laura ; Grogan, Paul ; Guo, Laodong ; Higuera, Philip E. ; Hinzman, Larry ; Hu, Feng Sheng ; Hugelius, Gustaf ; JAFAROV, ELCHIN ; Jandt, Randi ; Johnstone, Jill F. ; Karlsson, Jan ; Kasischke, Eric S. ; Kattner, Gerhard ; Kelly, Ryan ; Keuper, Frida ; Kling, George W. ; Kortelainen, Pirkko ; Kouki, Jari ; Kuhry, Peter ; Laudon, Hjalmar ; Laurion, Isabelle ; Macdonald, Robie W. ; Mann, Paul J. ; Martikainen, Pertti ; McClelland, James W. ; Molau, Ulf ; Oberbauer, Steven F. ; Olefeldt, David ; Paré, David ; Parisien, Marc-André ; Payette, Serge ; Peng, Changhui ; Pokrovsky, Oleg ; Rastetter, Edward B. ; Raymond, Peter A. ; Raynolds, Martha K. ; Rein, Guillermo ; Reynolds, James F. ; Robards, Martin ; Rogers, Brendan ; Schädel, Christina ; Schaefer, Kevin ; Schmidt, Inger K. ; Shvidenko, Anatoly ; Sky, Jasper ; Spencer, Robert G. M. ; Starr, Gregory ; Striegl, Robert ; Teisserenc, Roman ; Tranvik, Lars J. ; Virtanen, Tarmo ; Welker, Jeffrey M. ; Zimov, Sergey A.
    As the permafrost region warms, its large organic carbon pool will be increasingly vulnerable to decomposition, combustion, and hydrologic export. Models predict that some portion of this release will be offset by increased production of Arctic and boreal biomass; however, the lack of robust estimates of net carbon balance increases the risk of further overshooting international emissions targets. Precise empirical or model-based assessments of the critical factors driving carbon balance are unlikely in the near future, so to address this gap, we present estimates from 98 permafrost-region experts of the response of biomass, wildfire, and hydrologic carbon flux to climate change. Results suggest that contrary to model projections, total permafrost-region biomass could decrease due to water stress and disturbance, factors that are not adequately incorporated in current models. Assessments indicate that end-of-the-century organic carbon release from Arctic rivers and collapsing coastlines could increase by 75% while carbon loss via burning could increase four-fold. Experts identified water balance, shifts in vegetation community, and permafrost degradation as the key sources of uncertainty in predicting future system response. In combination with previous findings, results suggest the permafrost region will become a carbon source to the atmosphere by 2100 regardless of warming scenario but that 65%–85% of permafrost carbon release can still be avoided if human emissions are actively reduced.
  • Article
    Multi-molecular tracers of terrestrial carbon transfer across the pan-Arctic : comparison of hydrolyzable components with plant wax lipids and lignin phenols
    (Copernicus Publications on behalf of the European Geosciences Union, 2015-08-15) Feng, Xiaojuan ; Gustafsson, Orjan ; Holmes, Robert M. ; Vonk, Jorien E. ; van Dongen, Bart E. ; Semiletov, Igor P. ; Dudarev, Oleg V. ; Yunker, Mark B. ; Macdonald, Robie W. ; Montlucon, Daniel B. ; Eglinton, Timothy I.
    Hydrolyzable organic carbon (OC) comprises a significant component of sedimentary particulate matter transferred from land into oceans via rivers. Its abundance and nature are however not well studied in Arctic river systems, and yet may represent an important pool of carbon whose fate remains unclear in the context of mobilization and related processes associated with a changing climate. Here, we examine the molecular composition and source of hydrolyzable compounds isolated from sedimentary particles derived from nine rivers across the pan-Arctic. Bound fatty acids (b-FAs), hydroxy FAs, n-alkane-α,ω-dioic acids (DAs) and phenols were the major components released upon hydrolysis of these sediments. Among them, b-FAs received considerable inputs from bacterial and/or algal sources, whereas ω-hydroxy FAs, mid-chain substituted acids, DAs, and hydrolyzable phenols were mainly derived from cutin and suberin of higher plants. We further compared the distribution and fate of suberin- and cutin-derived compounds with those of other terrestrial biomarkers (plant wax lipids and lignin phenols) from the same Arctic river sedimentary particles and conducted a benchmark assessment of several biomarker-based indicators of OC source and extent of degradation. While suberin-specific biomarkers were positively correlated with plant-derived high-molecular-weight (HMW) FAs, lignin phenols were correlated with cutin-derived compounds. These correlations suggest that, similar to leaf-derived cutin, lignin was mainly derived from litter and surface soil horizons, whereas suberin and HMW FAs incorporated significant inputs from belowground sources (roots and deeper soil). This conclusion is supported by the negative correlation between lignin phenols and the ratio of suberin-to-cutin biomarkers. Furthermore, the molecular composition of investigated biomarkers differed between Eurasian and North American Arctic rivers: while lignin dominated in the terrestrial OC of Eurasian river sediments, hydrolyzable OC represented a much larger fraction in the sedimentary particles from Colville River. Hence, studies exclusively focusing on either plant wax lipids or lignin phenols will not be able to fully unravel the mobilization and fate of bound OC in Arctic rivers. More comprehensive, multi-molecular investigations are needed to better constrain the land–ocean transfer of carbon in the changing Arctic, including further research on the degradation and transfer of both free and bound components in Arctic river sediments.
  • Article
    Temporal and spatial variability of particle transport in the deep Arctic Canada Basin
    (John Wiley & Sons, 2015-04-11) Hwang, Jeomshik ; Kim, Minkyoung ; Manganini, Steven J. ; McIntyre, Cameron P. ; Haghipour, Negar ; Park, Jong Jin ; Krishfield, Richard A. ; Macdonald, Robie W. ; McLaughlin, Fiona A. ; Eglinton, Timothy I.
    To better understand the current carbon cycle and potentially detect its change in the rapidly changing Arctic Ocean, we examined sinking particles collected quasi-continuously over a period of 7 years (2004–2011) by bottom-tethered sediment trap moorings in the central Canada Basin. Total mass flux was very low (<100 mg m−2 d−1) at all sites and was temporally decoupled from the cycle of primary production in surface waters. Extremely low radiocarbon contents of particulate organic carbon and high aluminum contents in sinking particles reveal high contributions of resuspended sediment to total sinking particle flux in the deep Canada Basin. Station A (75°N, 150°W) in the southwest quadrant of the Canada Basin is most strongly influenced while Station C (77°N, 140°W) in the northeast quadrant is least influenced by lateral particle supply based on radiocarbon content and Al concentration. The results at Station A, where three sediment traps were deployed at different depths, imply that the most likely mode of lateral particle transport was as thick clouds of enhanced particle concentration extending well above the seafloor. At present, only 1%–2% of the low levels of new production in Canada Basin surface waters reaches the interior basin. Lateral POC supply therefore appears to be the major source of organic matter to the interior basin. However, ongoing changes to surface ocean boundary conditions may influence both lateral and vertical supply of particulate material to the deep Canada Basin.