Naveau Aude, Monteil-Rivera Fanny, Guillon Emmanuel, Dumonceau Jacques
Université de Reims Champagne Ardenne, Groupe de Recherche en Chimie Inorganique, BP 1039, F-51687 Reims, France.
Environ Sci Technol. 2007 Aug 1;41(15):5376-82. doi: 10.1021/es0704481.
The present study was initiated to determine the capacity of sulfide minerals (pyrite FeS2 and chalcopyrite CuFeS2) to delay the migration of inorganic selenium species in geological formations. Interactions between Se(IV) and Se(-II) and synthetic and natural sulfide minerals were investigated under anoxic conditions using the batch method. Significant sorption of selenium occurred under acidic conditions. Analysis of the solids after Se sorption using X-ray photoelectron spectroscopy (XPS) and X-ray absorption near edge structure (XANES) demonstrated the presence of reduced selenium species on the metallic sulfide surfaces, thus suggesting an oxido-reduction process coupled with sorption. Selenium reduction occurred concomitantly with the oxidation of pyritic sulfur, whereas metallic species (Fe, Cu) were not involved in the redox process. Formation of ferroselite (FeSe2) was postulated to take place on the synthetic solid while surface complexation or ionic exchange processes were more likely on the natural solids.
开展本研究是为了确定硫化物矿物(黄铁矿FeS₂和黄铜矿CuFeS₂)在地质构造中延缓无机硒物种迁移的能力。采用批量法在缺氧条件下研究了Se(IV)和Se(-II)与合成及天然硫化物矿物之间的相互作用。在酸性条件下发生了显著的硒吸附。使用X射线光电子能谱(XPS)和X射线吸收近边结构(XANES)对硒吸附后的固体进行分析,结果表明在金属硫化物表面存在还原态硒物种,因此表明存在与吸附耦合的氧化还原过程。硒的还原与黄铁矿硫的氧化同时发生,而金属物种(Fe、Cu)不参与氧化还原过程。推测在合成固体上会形成硒铁矿(FeSe₂),而在天然固体上更可能发生表面络合或离子交换过程。