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Equilibrium calculations of iron speciation and apparent iron solubility in the Celtic Sea at ambient seawater pH using the NICA-Donnan model
Zhu, K.; Birchill, A.J.; Milne, A.; Ussher, S.; Humphreys, M.P.; Carr, N.; Mahaffey, C.; Lohan, M.C.; Achterberg, E.P.; Gledhill, M. (2021). Equilibrium calculations of iron speciation and apparent iron solubility in the Celtic Sea at ambient seawater pH using the NICA-Donnan model. Mar. Chem. 237: 104038.

Bijhorende data:
In: Marine Chemistry. Elsevier: Amsterdam. ISSN 0304-4203; e-ISSN 1872-7581, meer
Peer reviewed article  

Beschikbaar in  Auteurs 

Author keywords
    Trace metals; Ocean acidification; Intrinsic binding constants

Auteurs  Top 
  • Zhu, K.
  • Birchill, A.J.
  • Milne, A.
  • Ussher, S.
  • Humphreys, M.P., meer
  • Carr, N.
  • Mahaffey, C.
  • Lohan, M.C.
  • Achterberg, E.P.
  • Gledhill, M.

    We used a combined ion pairing - organic matter speciation model (NICA-Donnan) to predict the organic complexation of iron (Fe) at ambient pH and temperature in the Celtic Sea. We optimized our model by direct comparison with Fe speciation determined by Adsorptive Cathodic Stripping Voltammetry using the added Fe-binding ligand 1-nitroso-2-naphthol (HNN) in the presence and absence of natural organic matter. We compared determined Fe speciation with simulated titrations obtained via application of the NICA-Donnan model with four different NICA parameter sets representing a range of binding site strengths and heterogeneities. We tested the assumption that binding sites scale to dissolved organic carbon (DOC) concentrations in marine waters. We found that a constant low DOC concentration resulted in an improved fit of our titration data to the simulated titrations, suggesting that inputs of autochthonous marine DOM may not increase the heterogeneity or concentrations of Fe binding sites. Using the optimal parameter set, we calculated pFe(III)´ (−log(∑Fe (OH)i3−i)) and apparent Fe(III) solubility (SFe(III)app) at ambient pH andtemperature in the water column of the Celtic Sea. SFe(III) app was defined as the sum of aqueous inorganic Fe(III) species and Fe(III) bound to DOM formed at a free Fe (Fe3+)concentration equal to the limiting solubility of Fe hydroxide (Fe(OH) 3(s)). SFe(III)app was within range of the determined dissolved Fe concentrations observed after winter mixing on the shelf and in waters >1500 m depth at our most offshore stations. Our study supports the hypothesis that the ocean dissolved Fe inventory is controlled by the interplay between Fe solubility and Fe binding by organic matter, although the overall number of metal binding sites in the marine environment may not be directly scalable to DOC concentrations.

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