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Bacterial Formation of Tooeleite and Mixed Arsenic(III) or Arsenic(V)−Iron(III) Gels in the Carnoulès Acid Mine Drainage, France. A XANES, XRD, and SEM Study

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Laboratoire de Minéralogie Cristallographie de Paris (LMCP), UMR CNRS 7590 - Universités Paris 6 et 7 - IPGP, 4 Place Jussieu, 75252 Paris Cedex 05, France, and Laboratoire Hydrosciences Montpellier, UMR 5569, CNRS - Université Montpellier 2, Place E. Bataillon, 34095 Montpellier Cedex 05, France
Cite this: Environ. Sci. Technol. 2003, 37, 9, 1705–1712
Publication Date (Web):March 21, 2003
Copyright © 2003 American Chemical Society

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    The oxidation of Fe(II) in acid mine drainage (AMD) leads to the precipitation of Fe(III) compounds which may incorporate toxic elements, such as arsenic (As), within their structure or adsorb them at their surface, thus limiting their mobility. The present work provides evidence for spatial and seasonal variations of microbial activity that influence arsenite oxidation and As immobilization in the heavily contaminated AMD from the Carnoulès mine, Gard, France ([As III] = 80 to 280 mg·L-1 in the acidic spring draining the waste-pile). In the first tens of meters of the AMD, the rapid oxidation of Fe(II) leads to the coprecipitation of large amounts of As with Fe(III) in bacterial mats. XRD, XANES, and SEM analyses of sediments and stromatolite samples revealed the unusual formation of As(III)-rich compounds, especially nanocrystalline tooeleite, Fe6(AsO3)4(SO4)(OH)4·4H2O, a rare ferric arsenite sulfate oxy-hydroxide mineral, together with XRD-amorphous mixed As(III)/As(V)-Fe(III) oxy-hydroxide compounds. In the wet season, the suspended sediments of the upstream zone essentially consist of tooeleite associated with am-As(III)-Fe(III) oxy-hydroxides, while am-As(V)-Fe(III) oxy-hydroxides, having As:Fe molar ratios as high as 0.6−0.8, dominate in the dry season. Comparing natural and bioassay samples revealed that the formation of As(III)-rich compounds in the wet season may be related to the metabolic activity of bacterial strains able to oxidize Fe(II) but not As(III). One of these strains, having an Acidithiobacillus ferrooxidans genotype, has been isolated from the Carnoulès AMD. In contrast, the formation of As(V)-rich compounds in the dry season can be related to both biotic and abiotic oxidation of As(III) to As(V). Some Thiomonas strains isolated from the Carnoulès AMD were shown to be able to catalyze the oxidation of As(III) to As(V) in solution. Therefore, they can promote the formation of mixed As(V)-Fe(III) oxy-hydroxides, provided enough Fe(II) oxidizes. These results yield a better understanding of natural processes at this site and may help in designing efficient As-removal processes.

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     Corresponding author phone:  33 1 44 27 75 04; fax:  33 1 44 27 37 85; e-mail: [email protected]. Corresponding author address:  LMCP, case 115, 4 Place Jussieu, 75252 Paris Cedex 05, France.

     Universités Paris 6 et 7 - IPGP.


     CNRS - Université Montpellier 2.

     Deceased October 26, 1999.

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    Water chemistry data on the Carnoulès AMD sampled in February 2001, May 2001, and January 2002 (Table 3). This material is available free of charge via the Internet at

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