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            <title xml:lang="en">Structure and reactivity of As(III)- and As(V)-rich schwertmannites and amorphous ferric arsenate sulfate from the Carnoule's acid mine drainage, France: Comparison with biotic and abiotic model compounds and implications for As remediation</title>
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            <funder>CNRS - EC2CO; SES-AME IdF [1775]; NSF [EF-0830093]</funder>
            <funder>This work was supported by the CNRS – EC2CO and by SESAME IdF Grant #1775. Portions of this research were carried out at SSRL, a national user facility operated by Stanford University on behalf of the U.S. Department of Energy, Office of Basic Energy Sciences. Support was also provided by NSF Grant EF-0830093 (Center for Environmental Implications of Nanotechnology). We acknowledge SSRL, ESRF, LURE, and ELETTRA for provision of beamtime on beamlines 11-2, BM30B, D44, and XAFS, respectively. John Bargar (SSRL), Olivier Proux (ESRF), Jean-Louis Hazemann (ESRF), Denis Testemale (ESRF), Stephanie Belin (LURE/SOLEIL), Andrea Cognigi (ELETTRA), Luca Olivi (ELETTRA) are kindly acknowledged for their help in acquiring EXAFS data on these synchrotron beamlines. We are indebted to Christian Personné (HSM Montpellier) for having first isolated Tm strains B2 and B3 from the Carnoulès site. Strains CC1 was isolated from the same site and kindly donated by Violaine Bonnefoy (Laboratoire de Chimie Bactérienne, Marseille). We thank AE Owen Duckworth for handling of the manuscript and for constructive suggestions. We are also indebted to reviewer Gleb Pokrovski and an anonymous reviewer for their contribution to improve the quality of the manuscript.</funder>
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                <term xml:lang="en">GOETHITE</term>
                <term xml:lang="en">SPECIATION</term>
                <term xml:lang="en">ADSORPTION</term>
                <term xml:lang="en">FERRIHYDRITE</term>
                <term xml:lang="en">NATURAL ATTENUATION</term>
                <term xml:lang="en">ACIDITHIOBACILLUS-FERROOXIDANS</term>
                <term xml:lang="en">RAY-ABSORPTION SPECTROSCOPY</term>
                <term xml:lang="fr">ARSENITE</term>
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              <p>Poorly ordered nanocrystalline hydroxysulfate minerals of microbial origin, such as schwertmannite, Fe8O8(OH)6SO4, are important arsenic scavengers in sulfate-rich acid mine drainage (AMD) environments. However, despite the fact that As(III) and As(V) have been shown to sorb on schwertmannite, little is known about the actual mechanism of arsenic scavenging processes after microbial Fe(II) oxidation in AMD environments. The major focus of the present study is to determine the molecular-level structure of poorly ordered As(III) and As(V) bearing Fe oxyhydroxysulfate minerals from the Carnoule's AMD, France, which exhibits exceptional As(III) concentrations. Powder X-ray diffraction (XRD) and extended X-ray absorption fine structure (EXAFS) spectroscopy were used to compare field samples with a large set of synthetic analogs prepared via biotic or abiotic pathways, with As/Fe ratios typical of minerals and mineraloids ranging from nanocrystalline schwertmannite to amorphous hydroxysulfate compounds. Our results yield further evidence for the poisoning effect of As(V) in limiting the nucleation of schwertmannite. For initial dissolved As(V)/Fe(III) molar ratios P0.2, amorphous Fe(III)-As(V) hydroxysulfate forms, with a local structure consistent with that of amorphous ferric arsenate. EXAFS data for this amorphous material are consistent with corner-sharing FeO6 octahedra to which AsO4 tetrahedra attach via double- corner 2C linkages. For As(V)/Fe(III) molar ratios lower than 0.2, As(V) binds to schwertmannite via 2C surface complexes. In contrast with the As(V)-containing samples, As(III) has a lower affinity for schwertmannite following its nucleation, as this mineral phase persists up to an initial As(III)/Fe(III) molar ratio of 0.6. EXAFS data indicate that during the precipitation process, As(III) forms dominantly 2C surface complexes on schwertmannite surfaces, likely on the sides of double-chains of Fe(III)(O,OH)6 octahedra, with a smaller proportion of edge-sharing 2E surface complexes at the apexes of these chains. Importantly, dissolved As(V) concentrations in contact with As(V)-schwertmannite or ferric arsenate were found to be 10 times lower than dissolved As(III) concentrations in contact with As(III)-schwertmannite for similar As/ Fe ratios in the solid phase. Consequently, remediation of As-rich AMD environments is greatly improved by oxidation of As(III) to As(V).</p>
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