Oxidation behavior and kinetics of sulfide by synthesized manganese oxide minerals

被引:21
作者
Qiu, Guohong [1 ]
Li, Qian [1 ]
Yu, Ying [1 ]
Feng, Xionghan [1 ]
Tan, Wenfeng [1 ]
Liu, Fan [1 ]
机构
[1] Huazhong Agr Univ, Coll Resources & Environm, Minist Agr, Key Lab Subtrop Agr Resource & Environm, Wuhan 430070, Peoples R China
基金
中国国家自然科学基金; 高等学校博士学科点专项科研基金;
关键词
Environmental chemistry; Manganese oxide mineral; Mn(III); Redox reaction; Soil; Sulfide; BIRNESSITE; AVAILABILITY; CRYPTOMELANE; DISSOLUTION; ADSORPTION; CR(III); SULFUR; PYRITE; RATES; STATE;
D O I
10.1007/s11368-011-0381-0
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Purpose Sulfur is distributed widely in soils and sediments. Sulfide oxidation causes acid mine wastewater, toxicity, and corrosion. Manganese oxide minerals usually affect the migration, transformation, and fate of sulfur. To understand the oxidation behaviors of S2- and influence factors, reaction process and kinetics were investigated by using different manganese oxides. Materials and methods Three types of manganese oxide minerals (birnessite I, birnessite II, and cryptomelane) were synthesized and participated in the oxidation of S2- (200 mg L-1). Oxidation products were characterized by spectrophotography, ion chromatography, X-ray diffraction, and scanning electron microscopy. The influences of pH, the amount of manganese oxides, temperature, and mineral structure on the initial oxidation rate of S2- were investigated. Reduction products of manganese oxides and the further transformation process in air were studied. Results and discussion The total conversion of S2- to SO (3) (2-) , S2O (3) (2-) , and SO (4) (2-) was no more than 15%, and S was likely to be the main oxidation product when oxidized by birnessite I (AOS 3.83). The initial oxidation rate followed a pseudo-first-order kinetic law, and the apparent rate constants (k (obs)) of S2- oxidation increased with elevating temperature, decreasing pH, and increasing the quantity and Mn(III) content of manganese oxides. Manganese oxides were deoxidized to Mn(OH)(2) and then oxidized to Mn3O4 in air, which was further transformed into beta-MnOOH. Conclusions S was the main oxidation product. The initial oxidation rate of S2- followed a pseudo-first-order kinetic law, was affected by temperature, pH, and the amount of manganese oxide, and significantly depended on the content of active Mn(III) available in manganese oxides. Oxidation ability was found to follow: birnessite II > cryptomelane > birnessite I with similar manganese AOS. Mn(OH)(2) powder can be slowly oxidized to MnOOH by O-2 in air.
引用
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页码:1323 / 1333
页数:11
相关论文
共 36 条
[21]  
Negra C, 2005, SOIL SCI SOC AM J, V69, P87
[22]   Mn (III) center availability as a rate controlling factor in the oxidation of phenol and sulfide on δ-MnO2 [J].
Nico, PS ;
Zasoski, RJ .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2001, 35 (16) :3338-3343
[23]   Importance of Mn(III) availability on the rate of Cr(III) oxidation on δ-MnO2 [J].
Nico, PS ;
Zasoski, RJ .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2000, 34 (16) :3363-3367
[24]   A short outline of the tunnel oxides [J].
Pasero, M .
MICRO- AND MESOPOROUS MINERAL PHASES, 2005, 57 :291-305
[25]   Manganese oxide minerals: Crystal structures and economic and environmental significance [J].
Post, JE .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 1999, 96 (07) :3447-3454
[26]   Metal sulfide complexes and clusters [J].
Rickard, David ;
Luther, George W., III .
SULFIDE MINERALOLGY AND GEOCHEMISTRY, 2006, 61 :421-504
[27]   Oxidation of pyrite and iron sulfide by manganese dioxide in marine sediments [J].
Schippers, A ;
Jorgensen, BB .
GEOCHIMICA ET COSMOCHIMICA ACTA, 2001, 65 (06) :915-922
[28]   Geomicrobiological and geochemical investigation of a pyrrhotite-containing mine waste tailings dam near Selebi-Phikwe in Botswana [J].
Schippers, Axel ;
Kock, Dagmar ;
Schwartz, Michael ;
Boettcher, Michael E. ;
Vogel, Horst ;
Hagger, Mike .
JOURNAL OF GEOCHEMICAL EXPLORATION, 2007, 92 (2-3) :151-158
[29]   TRANSFORMATIONS OF SYNTHETIC BIRNESSITE AS AFFECTED BY PH AND MANGANESE CONCENTRATION [J].
TU, SH ;
RACZ, GJ ;
GOH, TB .
CLAYS AND CLAY MINERALS, 1994, 42 (03) :321-330
[30]  
Valeika V, 2006, POL J ENVIRON STUD, V15, P623