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Use of Dissolved Sulfur Species to Measure Pyrite Dissolution in Water at pH 3 and 6

机译:使用溶解的硫物种测量pH值为3和6的水中硫铁矿的溶解度

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The oxidative dissolution of pyrite (FeS_2) is difficult to study because of redox transformations of the iron and sulfur, and adsorptive and precipitative loss of products from solution. Quantitative measurement of pyrite dissolution can perhaps be done most accurately with electrochemical techniques, but monitoring of dissolution products is of interest for interpretation of water-quality data at mine drainage and other field sites where pyrite dissolution is occurring. This laboratory study was undertaken to assess the usefulness of the sum of sulfate, sulfite, and thiosulfate in solution as a reaction progress variable, or RPV, for abiotic pyrite dissolution. Sulfate was the only sulfur species detected in solution, and thus was chosen as the RPV. Previous investigators have demonstrated that ferrous iron is not reliable as an RPV because of adsorption to the pyrite surface. Results indicated that sulfate is also not a highly accurate RPV. There was a sulfate loss from solution, perhaps by adsorption, with the extent of loss varying with solution conditions. While not a highly accurate RPV for kinetics modeling, the sulfate concentration provided a measure by which relative rates of abiotic pyrite dissolution could be assessed for pH 3 and 6, and with oxygen and ferric iron as oxidants. Sulfate production was greatest at pH 6 in the presence of oxygen, but no sulfate was produced under anoxic conditions (Fe~(3+) added as oxidant) at the same pH. The sulfate release under oxic conditions at this circumneutral pH was an order of magnitude greater than the release at pH 3 under both oxic and anoxic conditions.
机译:由于铁和硫的氧化还原转变以及溶液中产物的吸附和沉淀损失,黄铁矿(FeS_2)的氧化溶解难以研究。黄铁矿溶解度的定量测量也许可以通过电化学技术最准确地完成,但是对溶解产物的监测对于解释矿井排水系统和其他发生黄铁矿溶解的现场水质数据很有用。进行了这项实验室研究,以评估溶液中硫酸盐,亚硫酸盐和硫代硫酸盐之和作为非生物黄铁矿溶解反应进度变量或RPV的有用性。硫酸盐是溶液中唯一检测到的硫物质,因此被选作RPV。先前的研究人员已经证明,由于铁吸附到黄铁矿表面,亚铁作为RPV是不可靠的。结果表明,硫酸盐也不是高度精确的RPV。溶液中硫酸盐的损失,可能是吸附引起的,损失的程度随溶液条件的变化而变化。尽管不是用于动力学建模的高精度RPV,但硫酸盐浓度提供了一种度量,通过该度量可以评估pH为3和6的非生物黄铁矿相对溶解速率,并使用氧气和三价铁作为氧化剂。在有氧条件下,pH为6时,硫酸盐的产量最大,但在缺氧条件下(相同浓度的Fe〜(3+)作为氧化剂加入)则没有硫酸盐的产生。在该环境pH下在有氧条件下的硫酸盐释放量比在有氧和无氧条件下在pH 3下的硫酸盐释放量大一个数量级。

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