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Coordination chemistry and hydrolysis of Fe(III) in a peat humic acid studied by X-ray absorption spectroscopy

Author:
  • Torbjoern Karlsson
  • Per Persson
Publishing year: 2010
Language: English
Pages: 30-40
Publication/Series: Geochimica et Cosmochimica Acta
Volume: 74
Document type: Journal article
Publisher: Elsevier
Additional info: 1

Abstract english

The speciation of iron (Fe) in soils, sediments and surface waters is highly dependent on chemical interactions with natural organic matter (NOM). However, the molecular structure and hydrolysis of the Fe species formed in association with NOM is still poorly described. In this study extended X-ray absorption fine structure (EXAFS) spectroscopy was used to determine the coordination chemistry and hydrolysis of Fe(III) in solution of a peat humic acid (5010-49,200 mu g Fe g(-1) dry weight, pH 3.0-7.2). Data were analyzed by both conventional EXAFS data fitting and by wavelet transforms in order to facilitate the identification of the nature of backscattering atoms. Our results show that Fe occurs predominantly in the oxidized form as ferric ions and that the speciation varies with pH and Fe concentration. At low Fe concentrations (5010-9920 mu g g(-1); pH 3.0-7.2) mononuclear Fe(III)-NOM complexes completely dominates the speciation. The determined bond distances for the Fe(III)-NOM complexes are similar to distances obtained for Fe(III) complexed by desferrioxamine B and oxalate indicating the formation of a five-membered chelate ring structure. At higher Fe concentrations (49,200 mu g g(-1); pH 4.2-6.9) we detect a mixture of mononuclear Fe(III)-NOM complexes and polymeric Fe(III) (hydr)oxides with an increasing amount of Fe(III) (hydr)oxides at higher pH. However, even at pH 6.9 and a Fe concentration of 49,200 mu g g(-1) our data indicates that a substantial amount of the total Fe (>50%) is in the form of organic complexes, Thus, in environments with significant amounts of organic matter organic Fe complexes will be of great importance for the geochemistry of Fe. Furthermore, the formation of five-membered chelate ring structures is in line with the strong complexation and limited hydrolytic polymerization of Fe(III) in our samples and also agrees with EXAFS derived structures of Fe(III) in organic soils. (C) 2009 Elsevier Ltd. All rights reserved.

Keywords

  • Earth and Related Environmental Sciences

Other

Published
  • ISSN: 0016-7037
Per Persson
E-mail: per [dot] persson [at] biol [dot] lu [dot] se

Professor

MEMEG

+46 46 222 17 96

+46 70 266 38 79

E-C350

50

Professor

Centre for Environmental and Climate Research (CEC)

+46 46 222 17 96

+46 70 266 38 79

D350

Ekologihuset, Sölvegatan 37, Lund

50