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Environmental levels of thallium: influence of redox properties and anthropogenic sources
Örebro University, Department of Natural Sciences.
2006 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Thallium is a highly toxic element that humans are exposed to mainly by consumption of drinking water and vegetables grown in soil with high thallium content but also through inhalation of particles in the air. Thallium is also present in fossil fuels, alloys, and in electronic utilities. The increasing use of the element and emissions from notably energy production has lead to a higher load on the surface of the Earth. This study aims at increasing the knowledge about the behaviour of thallium in aquatic environments. Focus has been on the redox chemistry of thallium in relation to its mobility, which is of great importance because Tl(I) and Tl(III) have very different properties in this respect.

The relationship between Tl(I) and Tl(III) in surface waters from contaminated and uncontaminated environments was examined by ion chromatography connected on line to ICP-MS (inductively coupled plasma mass spectrometry). It was found in controlled systems that even though Tl(III) is thermodynamically unstable under fresh water conditions Tl(I) was oxidised in the presence of light and iron(III). This was also confirmed in field studies. When lake water samples were exposed to light, Tl(I) was oxidised and thallium was lost from the solution. The most likely explanation for this was adsorption of thallium to particle surfaces.

The concentration of thallium in Swedish lakes and soil were measured. In unpolluted lakes the concentration ranges between 4.5-12 ng/l, the sediment concentration was 0.07-1.46 mg/kg. The anthropogenic load was found to have increased since the end of the Second World War although concentrations above background were found since the early industrialisation. In contaminated areas the concentration in soil ranges from 0.64-88 mg/kg, high concentrations were found in systems with alum shale and in soil exposed to runoff from a lead and zinc enrichment plant.

The mobilisation of thallium from solid phases in contaminated areas was dependent on pH and about 50% of the leachable content was mobilised already at pH 5-6. Once it had been released to water it was highly mobile. These conditions suggest that in a large part of the Swedish environment a high mobility of thallium can be expected.

Place, publisher, year, edition, pages
Örebro: Örebro universitetsbibliotek , 2006. , 44 p.
Series
Örebro Studies in Chemistry, ISSN 1651-4270 ; 5
Keyword [en]
thallium, Tl(I), Tl(III), separation, ion chromatography, fresh water, sediment, mine waste, fly ash, redistribution, ICP-MS
National Category
Environmental Sciences
Research subject
Chemistry
Identifiers
URN: urn:nbn:se:oru:diva-356ISBN: 91-7668-474-1 (print)OAI: oai:DiVA.org:oru-356DiVA: diva2:136702
Public defence
2006-03-31, HSP1, Prismahuset, Örebro universitet, Örebro, 10:15
Opponent
Supervisors
Available from: 2006-03-09 Created: 2006-03-09 Last updated: 2011-05-26Bibliographically approved
List of papers
1. Historical pollution of seldom monitored trace elements in Sweden: Part B: sediment analysis of silver, antimony, thallium and indium
Open this publication in new window or tab >>Historical pollution of seldom monitored trace elements in Sweden: Part B: sediment analysis of silver, antimony, thallium and indium
2006 (English)In: Journal of Environmental Monitoring, ISSN 1464-0325, E-ISSN 1464-0333, Vol. 8, no 7, 732-744 p.Article in journal (Refereed) Published
Abstract [en]

Sediment cores from four boreal and remote lakes in a south to north transect in central Sweden were analysed for acid leachable silver, antimony, thallium and indium in the solid sediment phase and the corresponding porewater. Dating of the cores was made by their content of acid leachable lead and the 206Pb/207Pb ratio, in one lake also by 210Pb. The impact of diagenesis on element redistribution in the sediments was included and found to be minor except for thallium. The results show lowered concentrations towards the north and most intense accumulation after the Second World War, which is taken as evidence for atmospheric deposition being the primary source. Indium has declining concentrations in recent strata while silver and antimony increase. Thallium has lowered acid-leachable concentrations in recent strata. For all metals the impact of domestic industrialisation as well as the early industrialisation of central Europe is discernible. Only thallium appears to reach a geological background at depths that correspond to the late 18th century. For the other metals elevated levels are concluded.

National Category
Environmental Sciences Chemical Sciences
Research subject
Enviromental Science
Identifiers
urn:nbn:se:oru:diva-3053 (URN)10.1039/B601948J (DOI)
Available from: 2006-03-09 Created: 2006-03-09 Last updated: 2011-05-26Bibliographically approved
2. Assessing the release of thallium, cadmium, lead, copper and zinc from deposits with mixed wastes: a case study
Open this publication in new window or tab >>Assessing the release of thallium, cadmium, lead, copper and zinc from deposits with mixed wastes: a case study
(English)Manuscript (Other academic)
National Category
Chemical Sciences
Research subject
Chemistry
Identifiers
urn:nbn:se:oru:diva-3054 (URN)
Available from: 2006-03-09 Created: 2006-03-09 Last updated: 2016-12-13Bibliographically approved
3. Hydrogeochemical interpretations of a fly ash/municipal sludge covered sulphidic mine waste deposit: a case study of alkaline leachates in an acidic environment
Open this publication in new window or tab >>Hydrogeochemical interpretations of a fly ash/municipal sludge covered sulphidic mine waste deposit: a case study of alkaline leachates in an acidic environment
(English)Manuscript (Other academic)
National Category
Chemical Sciences
Research subject
Chemistry
Identifiers
urn:nbn:se:oru:diva-3055 (URN)
Available from: 2006-03-09 Created: 2006-03-09 Last updated: 2016-12-13Bibliographically approved
4. Separation and quantification of Tl(I) and Tl(III) in fresh water samples
Open this publication in new window or tab >>Separation and quantification of Tl(I) and Tl(III) in fresh water samples
2006 (English)In: Journal of Environmental Science and Health. Part A: Toxic/Hazardous Substances and Environmental Engineering, ISSN 1093-4529, E-ISSN 1532-4117, Vol. 41, no 7, 1155-1167 p.Article in journal (Refereed) Published
Abstract [en]

The two oxidation states of thallium, Tl(I) and Tl(III), were quantified by IC-ICP-MS using complexation of Tl3+ with DTPA (penta-carboxymethyl-diethylenetriamine) and separation on a cation exchange column according to a modification of the method devised by Coetzee et al. In order to avoid successively lowered separation efficiency and loss of resolution during a run, a gradient elution was made using HCl instead of HNO3. With an ultrasonic nebuliser instead of a V-groove nebuliser the limit of detection for Tl(I) and Tl(III) could be lowered from 25 ng/L and 3.0 ng/L to 9.0 ng/L and 0.7 ng/L, respectively, which is adequate for many fresh water systems. The stability of Tl(III) in acidic solutions was found to be concentration dependent, with an initially high reduction rate of Tl(III). Exposure of the sample to light further increased the reduction rate. Addition of DTPA (0.01 mM) and acid (HNO3, 1%) to a sample with 1 μg/L Tl(III) stabilised the Tl(III) content for at least 48 h. Analysis of field samples showed that only acidification is inadequate to maintain the original distribution of Tl(I) and Tl(III). Internal calibration (standard addition) and correction of the analytical signal (205Tl) with a non-ionic internal standard (11B) yielded almost quantitative recoveries of both Tl(I) and Tl(III). A scheme for field sample preparation is proposed, including sampling, storage and pre-analysis treatment.

National Category
Chemical Sciences
Research subject
Chemistry
Identifiers
urn:nbn:se:oru:diva-3056 (URN)10.1080/10934520600655747 (DOI)
Available from: 2006-03-09 Created: 2006-03-09 Last updated: 2011-03-28Bibliographically approved
5. The effect of light and iron(II)/iron(III) on the distribution of Tl(I)/Tl(III) in fresh water systems
Open this publication in new window or tab >>The effect of light and iron(II)/iron(III) on the distribution of Tl(I)/Tl(III) in fresh water systems
2006 (English)In: Journal of Environmental Monitoring, ISSN 1464-0325, E-ISSN 1464-0333, Vol. 8, no 6, 634-640 p.Article in journal (Refereed) Published
Abstract [en]

The distribution of aqueous Tl(I)/Tl(III) as a function of light exposure and solution properties was studied by quantifying the oxidation states after separation with ion chromatography and on-line detection with ICP-MS. Ultraviolet irradiation of aqueous solutions containing 1 μg l−1 Tl(III) and in equilibrium with the atmosphere increases the reduction rate. In systems with photoreduction of Fe(III)(aq) a quantitative oxidation of Tl(I)(aq) was observed, notably at low pH. The process is reversible, as indicated by formation of Tl(I) when the irradiated systems were kept in the dark. In systems with colloidal silica-stabilised ferrihydrite, UV irradiation also leads to oxidation of Tl(I)(aq), but not quantitatively. It is suggested that adsorption of thallium to the ferrihydrite determines the rate of oxidation. Detectable, but not quantitative, oxidation of Tl(I)(aq) took place when natural water samples with 1 μg l−1 Tl(I)(aq) were exposed to either sunlight or UV-light. For these samples, the reduction was not quantitative when they were kept in the dark for 24 h. The results suggest that the light dependent iron cycle in fresh water systems strongly influences the redox state of thallium.

National Category
Environmental Sciences
Research subject
Chemistry
Identifiers
urn:nbn:se:oru:diva-3057 (URN)10.1039/B516445A (DOI)
Available from: 2006-03-09 Created: 2006-03-09 Last updated: 2011-05-26Bibliographically approved

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