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Separation and quantification of Tl(I) and Tl(III) in fresh water samples
Örebro University, Department of Natural Sciences.
Örebro University, Department of Natural Sciences.
Örebro University, Department of Natural Sciences.
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, p. 1155-1167Article 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.

Place, publisher, year, edition, pages
2006. Vol. 41, no 7, p. 1155-1167
National Category
Chemical Sciences
Research subject
Chemistry
Identifiers
URN: urn:nbn:se:oru:diva-3056DOI: 10.1080/10934520600655747OAI: oai:DiVA.org:oru-3056DiVA, id: diva2:136700
Available from: 2006-03-09 Created: 2006-03-09 Last updated: 2017-12-14Bibliographically approved
In thesis
1. Environmental levels of thallium: influence of redox properties and anthropogenic sources
Open this publication in new window or tab >>Environmental levels of thallium: influence of redox properties and anthropogenic sources
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. p. 44
Series
Örebro Studies in Chemistry, ISSN 1651-4270 ; 5
Keywords
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:nbn:se:oru:diva-356 (URN)91-7668-474-1 (ISBN)
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: 2017-10-18Bibliographically approved

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Karlsson, UlrikaDüker, AndersKarlsson, Stefan

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