Oxidation of FeS by oxygen-bearing acidic solutions

被引:101
作者
Chirita, Paul [1 ]
Descostes, Michael [2 ,3 ]
Schlegel, Michel L. [3 ,4 ]
机构
[1] Univ Craiova, Dept Inorgan Analyt & Technol Chem, Craiova 200478, Romania
[2] CEA, DEN DANS DPC SECR, Lab Radionuclides Migrat Measurements & Modeling, F-91191 Gif Sur Yvette, France
[3] Univ Evry, CNRS, CEA, UMR 8587, Evry, France
[4] CEA, DEN DANS DPC SCP, Lab React Surfaces & Interfaces, F-91191 Gif Sur Yvette, France
关键词
FeS; oxygen; kinetics; reaction mechanism;
D O I
10.1016/j.jcis.2008.01.024
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Oxidation of FeS in oxygen-bearing acidic solutions was investigated at different temperatures (25 to 45 degrees C) and pH (2.75 to 3.45). The rate of the oxidative dissolution of FeS is strongly dependent on pH. The reaction order with respect to hydrogen ions has been found to be 1.03 +/- 0.02 at 25 degrees C, and the apparent activation energy (E-a) is 41.6 +/- 10.7 kJ mol(-1) at initial pH 3.00, suggesting that the FeS oxidative dissolution is controlled by the diffusion of oxidant species across a sulfur-rich layer (SRL) that undergoes chemical transformations leading to an increase in the mean number of sulfur atoms in polysulfide chains and the rearrangement of these chains. Fourier transform infrared spectroscopy and X-ray diffraction results obtained for the FeS samples reacted for 72 It at 25 degrees C and pH between 2.75 and 3.45 indicate the formation of goethite, of lepidocrocite, and of poorly ordered solid phases (assigned as SRL) on initial surfaces. The experimental data suggest a mechanism based on the protonation of FeS surfaces followed by oxidation of FeS by dissolved oxygen to produce Fe2+, S-0, and S-n(2-). Fe2+ is unstable under oxidative conditions and transforms into Fe(OH)(3(s)), goethite and lepidocrocite. (C) 2008 Elsevier Inc. All rights reserved.
引用
收藏
页码:84 / 95
页数:12
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