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Phase transformation and surface chemistry of secondary iron minerals formed from acid mine drainage
Umeå University, Faculty of Science and Technology, Department of Chemistry.
2003 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The mining of sulphidic ore to extract metals such as zinc and copper produces huge quantities of waste material. The weathering and oxidation of the waste produces what is commonly known as Acid Mine Drainage (AMD), a dilute sulphuric acid rich in Fe(II) and heavy metals. This thesis serves to summarise five papers reporting how the precipitation of Fe(III) phases can attenuate the contamination of heavy metals by adsorption processes.

Schwertmannite (Fe8O8(OH)6SO4) is a common Fe(III) mineral precipitating in AMD environments at pH 3-4. The stability and surface chemistry of this mineral was investigated. It was shown that the stability depended strongly on pH and temperature, an increase in either promoted transformation to goethite (α-FeOOH). Two pH dependent surface species of SO42- were detected with infrared (ATR-FTIR) spectroscopy.

The adsorption of Cu(II), Pb(II) and Zn(II) to schwertmannite occurred at lower pH than to goethite, whereas Cd(II) adsorption occurred in a similar pH range on both schwertmannite and goethite. Extended x-ray absorption fine structure (EXAFS) spectroscopy suggests two surface species for Cu(II) and Cd(II) at the schwertmannite surface. Cu(II) adsorbs monodentately and Cd(II) bridging bidentately to adsorbed SO42-. Both metal ions also adsorb in a bridging bidentate mode to the surface hydroxyl groups. At pH 7.5 up to 2.7 μmol Cd(II) m-2 could be adsorbed to schwertmannite, indicating a large adsorption capacity for this mineral.

The acid-base properties of two NOM samples were characterised and could be well described as diprotic acids below pH 6. The adsorption of NOM to schwertmannite and goethite was very similar and adsorption occured in a very wide pH range.

High concentrations of NOM increased the adsorption of Cu(II) to goethite at low pH whereas a slight decrease was noted at low concentrations of NOM. No effect was detected in the schwertmannite system.

The formation of Fe(III) phases from precipitation of AMD was shown to be very pH dependent. At pH 5.5 a mixture of minerals, including schwertmannite, formed whereas at pH 7 only lepidocrocite (γ-FeOOH) formed. The concentration of Zn(II) in AMD could by adsorption/coprecipitation be reduced to environmentally acceptable levels.

Place, publisher, year, edition, pages
2003. , 71 p.
Keyword [en]
Inorganic chemistry, schwertmannite, goethite, lepidocrocite, acid mine drainage, sulphate, natural organic matter, mineral surface, infrared spectroscopy, EXAFS, XRD, ternary surface complex, copper(II), cadmium(II), lead(II), zinc(II)
Keyword [sv]
Oorganisk kemi
National Category
Inorganic Chemistry
Research subject
Inorganic Chemistry
Identifiers
URN: urn:nbn:se:umu:diva-156ISBN: 91-7305-552-2 (print)OAI: oai:DiVA.org:umu-156DiVA: diva2:141383
Public defence
2003-12-12, KB3B1, KBC, Umeå, 13:00
Opponent
Supervisors
Available from: 2003-11-14 Created: 2003-11-14 Last updated: 2017-01-23Bibliographically approved
List of papers
1. Schwertmannite precipitated from acid mine drainage: phase transformation, sulphate release and surface properties
Open this publication in new window or tab >>Schwertmannite precipitated from acid mine drainage: phase transformation, sulphate release and surface properties
2005 (English)In: Applied Geochemistry, ISSN 0883-2927, E-ISSN 1872-9134, Vol. 20, no 1, 179-191 p.Article in journal (Refereed) Published
Abstract [en]

Schwertmannite precipitated from acid mine drainage at the Kristineberg Zn-Cu mine in northern Sweden has been characterised regarding elemental composition, phase transformation as a function of pH and time. SO42- release and speciation of SO42- associated with the solid. The elemental analysis gave the composition FeSOS(OH)(5.02)(-SO4)(1.49) . 0.5H(2)O where approximately 1/3 of the SO42- is adsorbed to the surface. The conversion of schwertmannite to goethite at pH 9 was complete within 187 days; at pH 6. the conversion was still incomplete after 514 days. Lower pH and relatively high SO42- concentration decreased the conversion even further. Also temperature was shown to be an important parameter for this process and low temperature (+4 degreesC) effectively stopped the transformation at pH 3. The release of SO42- was linear with pH and X-ray photoelectron spectroscopy measurements confirming that the surface bound SO42- was released before bulk SO42-. Zeta potential measurements indicate a pH(IEP) of 7.2 for the schwertmannite sample. Prior to conversion into goethite, the SO42- associated with schwertmannite was indicated by attenuated total reflectance FTIR spectroscopy to be present both as bulk and surface species. Furthermore: the speciation of surface SO42- was shown to vary with pH and two predominating species were detected. As pH increases. SO42- is increasingly Coordinated in an outer sphere mode whereas a stronger. possibly inner sphere, complex dominates. at low pH.

Place, publisher, year, edition, pages
Oxford: Pergamon Press, 2005
Keyword
waters, ferrihydrite, iron, adsorption, goethite, complexation, solubilities, interface, AL
National Category
Geochemistry Geophysics
Identifiers
urn:nbn:se:umu:diva-13612 (URN)10.1016/j.apgeochem.2004.04.008 (DOI)000226312100013 ()
Available from: 2007-05-11 Created: 2007-05-11 Last updated: 2017-01-23Bibliographically approved
2. Adsorption of Cu(II) and Cd(II) to schwertmannite precipitated from acid mine drainage - An EXAFS study
Open this publication in new window or tab >>Adsorption of Cu(II) and Cd(II) to schwertmannite precipitated from acid mine drainage - An EXAFS study
Show others...
Manuscript (Other academic)
Identifiers
urn:nbn:se:umu:diva-2977 (URN)
Available from: 2003-11-14 Created: 2003-11-14 Last updated: 2010-01-13Bibliographically approved
3. Adsorption of Cu(II) to schwertmannite and goethite in the presence of natural organic matter
Open this publication in new window or tab >>Adsorption of Cu(II) to schwertmannite and goethite in the presence of natural organic matter
Manuscript (Other academic)
Identifiers
urn:nbn:se:umu:diva-2978 (URN)
Available from: 2003-11-14 Created: 2003-11-14 Last updated: 2010-01-13Bibliographically approved
4. Evaluation of different approaches to quantify stron organic acidity and acid-base buffering of organic-rich surface waters in Sweden
Open this publication in new window or tab >>Evaluation of different approaches to quantify stron organic acidity and acid-base buffering of organic-rich surface waters in Sweden
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2002 In: Water Research, Vol. 36, 4487-4496 p.Article in journal (Refereed) Published
Identifiers
urn:nbn:se:umu:diva-2979 (URN)
Available from: 2003-11-14 Created: 2003-11-14Bibliographically approved
5. Precipitation of secondary Fe(III) minerals from acid mine drainage
Open this publication in new window or tab >>Precipitation of secondary Fe(III) minerals from acid mine drainage
Manuscript (Other academic)
Identifiers
urn:nbn:se:umu:diva-2980 (URN)
Available from: 2003-11-14 Created: 2003-11-14 Last updated: 2010-01-13Bibliographically approved

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