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The relevance of ligand exchange kinetics in the measurement of iron speciation by CLE–AdCSV in seawater

Publié dansMarine chemistry, vol. 173, p. 100-113
Date de publication2015
Résumé

CLE–AdCSV (competitive ligand exchange–adsorptive cathodic stripping voltammetry) has proved to be a decisive technique in recognising the key role that organic matter plays in modulating the biogeochemical cycle of iron in aquatic ecosystems. As themethod requires equilibriumamong all the constituents of the solution before measurements are taken, accurate knowledge of the kinetics of the undergoing ligand exchange is essential. The kinetics of the process has beenmost frequently described in terms of a dissociative (or Eigen–Wilkins)mechanism, with some authors even claiming that, under such approach, iron complexes would dissociate during CLE so slowly that the method would be invalidated. The complexity of the processes—largely exceeding the simple mechanistic description of the Eigen–Wilkins mechanism—is discussed on the basis of a broad overview of possible reaction routes. Evidence of the role of matrix components of natural waters is presented and the impossibility of exporting kinetic constants to systems characterised by different molecular mechanics, mostly ignored in previous studies, is highlighted. Experimental evidence obtained fromvarious methodological approaches allows inferring the range of CLE equilibration times to be applied in CLE–AdCSVmeasurements and further proves that the Eigen–Wilkins mechanism is just one of the many reaction routes applicable in natural waters. Studying iron CLE mechanisms for proposed competing ligands before designing any experiment using CLE–AdCSV is recommended.

Mots-clés
  • Iron ligand exchange
  • AdCSV
  • Competing ligand equilibrium kinetics
  • Dissociative mechanism
  • Associative mechanism
Citation (format ISO)
LAGLERA BAQUER, Luis Miguel, FILELLA, Montserrat. The relevance of ligand exchange kinetics in the measurement of iron speciation by CLE–AdCSV in seawater. In: Marine chemistry, 2015, vol. 173, p. 100–113. doi: 10.1016/j.marchem.2014.09.005
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Article (Published version)
accessLevelRestricted
Identifiants
ISSN du journal0304-4203
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Création29.10.2014 16:17:00
Première validation29.10.2014 16:17:00
Heure de mise à jour14.03.2023 22:11:32
Changement de statut14.03.2023 22:11:32
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