quantitative determination of elemental sulfur at the arsenopyrite surface after oxidation by ferric iron mechanistic implications定量测定的元素硫砷黄铁矿表面氧化后三价铁机械的影响.pdfVIP

Quantitative determination of elemental sulfur at the arsenopyrite surface after oxidation by ferric iron: mechanistic implications Molly M. McGuire,a Jillian F. Banfieldb and Robert J. Hamers*a aDepartment of Chemistry, 1101 University Ave, University of Wisconsin—Madison, Madison, WI 53706, USA. E-mail: rjhamers@facstaff.wisc.edu; Tel: (608) 262-6371; Fax: (608) 262-0453 bDepartment of Geology and Geophysics, 1215 W. Dayton St, University of Wisconsin— Madison, Madison, WI 53706, USA Received 10th May 2001, Accepted 13th July 2001 Published on the Web 24th July 2001First published as an Advanced Article on the web 25th August 2000 The elemental sulfur formed at the arsenopyrite surface after oxidation by ferric iron was quantitatively measured by extraction in perchloroethylene and subsequent quantitative analysis by HPLC. Reactions with ferric iron in perchloric acid solutions or in sulfuric acid solutions (both at pH 1 and 42 C, which approximate extreme acid mine drainage conditions) produced elemental sulfur in quantities greater than 50% of the total reacted sulfur. The controversy surrounding the mechanism of the oxidative dissolution of arsenopyrite is discussed in light of these measurements. Based on the observation of greater than 50% production of elemental sulfur, a mechanism by which all the sulfur from the mineral proceeds through thiosulfate can be eliminated as a possible description of the dissolution of arsenopyrite. Instead, it is likely the other constituents of the mineral lattice, Fe and As, are leached out, leaving behind a S0 lattice. Nucleation reactions will then result in the formation of stable S8 rings. Introduction In contrast, Raman spectroscopic and chromatographic inves- tigations of arsenopyrite samples oxidized