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Fitzsimmons, JN, Bundy RM, Al-Subiai SN, Barbeau KA, Boyle EA.  2015.  The composition of dissolved iron in the dusty surface ocean: An exploration using size-fractionated iron-binding ligands. Marine Chemistry. 173:125-135.   10.1016/j.marchem.2014.09.002   AbstractWebsite

The size partitioning of dissolved iron and organic iron-binding ligands into soluble and colloidal phases was investigated in the upper 150 m of two stations along the GA03 U.S. GEOTRACES North Atlantic transect. The size fractionation was completed using cross-flow filtration methods, followed by analysis by isotope dilution inductively-coupled plasma mass spectrometry (ID-ICP-MS) for iron and competitive ligand exchange-adsorptive cathodic stripping voltammetry (CLE-ACSV) for iron-binding ligands. On average, 80% of the 0.1-0.65 nM dissolved iron (<0.2 mu m) was partitioned into the colloidal iron (cFe) size fraction (10 kDa < cFe <0.2 gm), as expected for areas of the ocean underlying a dust plume. The 1.3-2.0 nM strong organic iron-binding ligands, however, overwhelmingly (75-77%) fell into the soluble size fraction (<10 kDa). As a result, modeling the dissolved iron size fractionation at equilibrium using the observed ligand partitioning did not accurately predict the iron partitioning into colloidal and soluble pools. This suggests that either a portion of colloidal ligands is missed by current electrochemical methods because they react with iron more slowly than the equilibration time of our CLE-ACSV method, or part of the observed colloidal iron is actually inorganic in composition and thus cannot be predicted by our model of unbound iron-binding ligands. This potentially contradicts the prevailing view that greater than >99% of dissolved iron in the ocean is organically complexed. Disentangling the chemical form of iron in the upper ocean has important implications for surface ocean biogeochemistry and may affect iron uptake by phytoplankton. (C) 2014 Elsevier B.V. All rights reserved.

K
King, AL, Buck KN, Barbeau KA.  2012.  Quasi-Lagrangian drifter studies of iron speciation and cycling off Point Conception, California. Marine Chemistry. 128:1-12.   10.1016/j.marchem.2011.11.001   AbstractWebsite

The distribution and speciation of dissolved Fe (dFe) were measured during four quasi-Lagrangian drogued drifter studies (similar to 4 d duration each) that were conducted in the southern California Current System in May 2006 and April 2007. Three of the four drifter studies were within the coastal upwelling regime and one drifter study was in a warm-core anticyclonic eddy. Incubation bottle experiments were also conducted to determine the degree of phytoplankton Fe limitation and to assess changes in the concentration of Fe-binding ligands. In the coastal upwelling drifter studies, in situ dFe (1.4-1.8 nM) and macronutrients were initially high and declined over time. Fe addition incubation experiments indicated that the phytoplankton community was not Fe limited at the beginning of the coastal upwelling drifter experiments (when mu M nitrate:nM dFe ratios were similar to 7-8). By the end of two of the three drifter studies (when mu M nitrate:nM dFe ratios were similar to 12-19), Fe addition resulted in larger nitrate and silicic acid drawdown, and larger accumulations in chlorophyll a, particulate organic carbon and nitrogen, and diatom and dinoflagellate-specific carotenoid pigments. Fe speciation was measured in situ in three of the four drifter studies with stronger L-1-type ligands found to be present in excess of dFe in all samples. In Fe speciation incubation experiments. L-1-type ligand production was observed in conjunction with phytoplankton growth under Fe-limiting conditions. The results presented here support and add a quasi-Lagrangian perspective to previous observations of dFe and macronutrient cycling over space and time within the California coastal upwelling regime, including Fe limitation within the phytoplankton community in this region and the biological production of Fe-binding ligands concomitant with Fe limitation. (C) 2011 Elsevier B.V. All rights reserved.

King, AL, Barbeau K.  2007.  Evidence for phytoplankton iron limitation in the southern California Current System. Marine Ecology-Progress Series. 342:91-103.   10.3354/meps342091   AbstractWebsite

Observations of phytoplankton iron limitation in the world's oceans have primarily been confined to high-nutrient, low-chlorophyll (HNLC) regimes, found in the western equatorial and subarctic Pacific, Southern Ocean, and coastal upwelling zones off California and Peru. We investigated the potential for phytoplankton iron limitation in coastal transition zones (50 to 200 km offshore) of the southern California Current System, a weak upwelling regime that is relatively low in nutrients (< 4 mu mol nitrate 1(-1)) and low in chlorophyll (< 1 mu g chl a 1(-1)). In grow-out incubation experiments conducted during summer, July 2003 and 2004, phytoplankton responded to nanomolar iron additions, despite the non-HNLC initial conditions, Observed changes in phytoplankton and nutrient parameters upon iron addition were significant, although markedly lower in amplitude relative to typical grow-out experiments in HNLC regimes. While we cannot disprove alternate explanations for the observed limitation of phytoplankton growth, such as a proximate grazing control, our results indicate that phytoplankton growth in the southern California Current System is, at times, limited by the supply of iron. Based on our findings and the results of previous studies in this region, we suggest that phytoplankton biomass is generally limited by the supply of nitrate, while iron, directly or indirectly, influences macronutrient utilization, community species composition, and phytoplankton spatial and temporal distribution.

S
Semeniuk, DM, Bundy RM, Payne CD, Barbeau KA, Maldonado MT.  2015.  Acquisition of organically complexed copper by marine phytoplankton and bacteria in the northeast subarctic Pacific Ocean. Marine Chemistry. 173:222-233.   10.1016/j.marchem.2015.01.005   AbstractWebsite

Copper (Cu) is an essential micronutrient for marine phytoplankton, but can cause toxicity at elevated intracellular concentrations. The majority of Cu (>99.9%) in oceanic surface waters is bound to strong organic ligands, presumably produced by prokaryotes to detoxify Cu. Although laboratory studies have demonstrated that organically complexed Cu may be bioavailable to marine eukaryotic phytoplankton, the bioavailability of Cu organic complexes to indigenous marine phytoplankton has not been examined in detail. Using the carrier free radioisotope Cu-67 at an iron limited station in the northeast subarctic Pacific Ocean, we performed size fractionated short-term Cu uptake assays with three Cu(II)-chelates, and Cu-67 bound to the strong in situ ligands, with or without additions of weak Cu(I) ligands. Estimates of the maximum supply of inorganic Cu (Cu') to the cell surface of eukaryotic phytoplankton were unable to account for the observed Cu uptake rates from the in situ ligands and two of the three added Cu(II)-chelates. Addition of 10 nM weak organic Cu(I) ligands enhanced uptake of Cu bound to the in situ ligands. Thus, Cu within the in situ and strong artificial Cu(II) organic ligands was accessible to the phytoplankton community via various possible Cu uptake strategies, including; cell surface enzymatically mediated reduction of Cu(II) to Cu(I), the substrate of the high-affinity Cu transport system in eukaryotes; or ligand exchange between weak Cu-binding ligands and the cellular Cu transporters. During a 14-hour uptake assay, particulate Cu concentrations reached a plateau in most treatments. Losses were observed in some treatments, especially in the small size fractions (<5 mu m), corresponding with faster initial Cu uptake rates. This may indicate that Cu cycling is rapid between particulate and dissolved phases due to cellular efflux or remineralization by micrograzers. The acquisition of Cu from the strong in situ ligands puts into question the historic role attributed to Cu binding ligands in decreasing Cu bioavailability. (C) 2015 Elsevier B.V. All rights reserved.