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Trace metal speciation predictions in natural aquatic systems: incorporation of dissolved organic matter (DOM) spectroscopic quality

Mueller, Kristin K.; Lofts, Stephen; Fortin, Claude; Campbell, Peter G.C.. 2012 Trace metal speciation predictions in natural aquatic systems: incorporation of dissolved organic matter (DOM) spectroscopic quality. Environmental Chemistry, 9 (4). 356-368. 10.1071/EN11156

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Abstract/Summary

To calculate metal speciation in natural waters, modellers must choose the proportion of dissolved organic matter (DOM) that is actively involved in metal complexation, defined here as the percentage of active fulvic acid (FA); to be able to estimate this proportion spectroscopically would be very useful. In the present study, we determine the free Cd2+, Cu2+, Ni2+ and Zn2+ concentrations in eight Canadian Shield lakes and compare these measured concentrations to those predicted by the Windermere Humic Aqueous Model (WHAM VI). For seven of the eight lakes, the measured proportions of Cd2+ and Zn2+ fall within the range of values predicted by WHAM; the measured proportion of Cu2+ falls within this range for only half of the lakes sampled, whereas for Ni,WHAM systematically overestimated the proportion of Ni2+. With the aim of ascribing the differences between measured and modelled metal speciation to variations in DOM quality, the percentage of active FA needed to fit modelled and measured free metal concentrations was compared with the lake-to-lake variation in the spectroscopic quality of the DOM, as determined by absorbance and fluorescence measurements. Relationships between the percentage of active FA and DOM quality were apparent for Cd, Cu, Ni and Zn, suggesting the possibility of estimating the percentage of active FA spectroscopically and then using this information to refine model predictions. The relationships for Ni differed markedly from those observed for the other metals,suggesting that the DOM binding sites active in Cd, Cu and Zn complexation are different from those involved in Ni complexation. To our knowledge, this is the first time that such a distinction has been resolved in natural water samples.

Item Type: Publication - Article
Digital Object Identifier (DOI): 10.1071/EN11156
Programmes: CEH Topics & Objectives 2009 - 2012 > Biogeochemistry > BGC Topic 2 - Biogeochemistry and Climate System Processes > BGC - 2.1 - Quantify & model processes that control the emission, fate and bioavailability of pollutants
CEH Sections: Shore
ISSN: 1448-2517
Additional Information. Not used in RCUK Gateway to Research.: This document is the author’s final manuscript version of the journal article, incorporating any revisions agreed during the peer review process. Some differences between this and the publisher’s version remain. You are advised to consult the publisher’s version if you wish to cite from this article. The definitive version is available at www.publish.csiro.au/
NORA Subject Terms: Ecology and Environment
Chemistry
Date made live: 20 Aug 2012 13:30
URI: http://nora.nerc.ac.uk/id/eprint/19305

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