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Environ Sci Technol. 2007 Nov 15;41(22):7621-31.

Metal flux and dynamic speciation at (bio)interfaces. Part II: Evaluation and compilation of physicochemical parameters for complexes with particles and aggregates.

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Analytical and Biophysical Environmental Chemistry (CABE), University of Geneva, Sciences II, 30 quai E. Ansermet, CH-1211 Geneva 4.


The computation of metal flux in aquatic systems at consuming surfaces like organism membranes must consider the diffusion processes of metal ions, ligands, and complex species, as well as the kinetic and thermodynamic aspects of their chemical interactions. Many natural ligands, however, have complicated properties (formation of successive complexes for simple ligands, polyelectrolytic properties and chemical heterogeneity for macromolecular ligands, large size distribution and fractal structure for suspended aggregates). These properties should be properly modeled to get the correct values of the chemical rate constants and diffusion coefficients required for flux computations. The selection of the most appropriate models and parameter values is far from straightforward. In this series of papers, models and compilations of parameters for application to the three most important types of complexants found in aquatic systems, the small, simple ligands, the fulvic and humic compounds, and the colloidal "particles" or aggregates, are discussed. In particular, new approaches are presented to compute the rate constants of metal complex formation for both fulvics/humics and particles/aggregates. A method to include the site distribution of fulvics/ humics and the size distribution of particles/aggregates in metal flux computation at consuming interfaces is also discussed in detail. These models and parameters are discussed critically and presented in a single consistent framework, applicable to the computation of metal flux in presence of any of the above complexants ortheir mixtures. Part I of the series focuses on simple ligands and fulvic/ humic compounds. Part II deals with particulate and aggregate complexants.

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