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Rapid analysis of actinide isotopes using quadrupole ICP-MS for emergency preparedness and environmental monitoring
Örebro University, Department of Natural Sciences.
2007 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Transuranium elements in the environment are mainly derived from nuclear weapons testing and the nuclear fuel cycle. Of growing concern are illicit nuclear trafficking and the threat of terror acts. The development of rational methods, for environmental monitoring and for tracing sources of nuclear and radioactive materials in the environment, is constantly required.

Traditionally, the actinides have been determined by radiometric techniques. These analyses can be time consuming for elements at low concentrations and with long half-lives. This thesis addresses the determination of actinides, especially plutonium, in environmental samples with ICP-QMS (inductively coupled plasma quadrupole mass spectrometry). The ICP-QMS instrument was equipped with an USN (ultrasonic nebuliser), which proved to be a successful combination for the determination of plutonium at low concentrations in acidified solutions after separation with anion exchange. The detection limit for plutonium was in the range 10-30 pg/l with a RSD of 1-10%. The suitability of chemical separation was evaluated for anion exchange, liquid-liquid-extraction and extraction chromatography.

The outlined procedure, including sample dissolution, chemical separation and analysis, for determination of actinides in environmental matrices proved to be accurate and reliable. Quality assurance of the procedure was performed during an intercomparison exercise and with reference materials. The detection accuracy has also been validated with α-spectrometry and ICP-SFMS. The procedure has been applied to saline sediments and fresh water sediments as well as several fresh water matrices.

Place, publisher, year, edition, pages
Örebro: Örebro universitetsbibliotek , 2007. , p. 67
Series
Örebro Studies in Environmental Science, ISSN 1650-6278 ; 10
Keywords [en]
quadrupole ICP-MS, actinides, plutonium, preparedness
National Category
Natural Sciences Chemical Sciences Environmental Sciences
Research subject
Enviromental Science
Identifiers
URN: urn:nbn:se:oru:diva-947ISBN: 978-91-7668-529-7 (print)OAI: oai:DiVA.org:oru-947DiVA, id: diva2:137480
Public defence
2007-03-06, Hörsal 3, Örebro universitet, Fakultetsgatan 1, Örebro, 10:15
Opponent
Supervisors
Available from: 2007-02-13 Created: 2007-02-13 Last updated: 2017-10-18Bibliographically approved
List of papers
1. Determination of plutonium in environmental samples with quadrupole ICP-MS
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2008 (English)In: Journal of Radioanalytical and Nuclear Chemistry, ISSN 0236-5731, E-ISSN 1588-2780, Vol. 275, no 1, p. 55-70Article in journal (Refereed) Published
Abstract [en]

A method for rapid determination of plutonium isotopes in environmental samples with ultrasonic nebulisation and quadrupole ICP-MS detection was established. Techniques for sample dissolution, pre-concentration and chemical separation were evaluated and the optimal scheme outlined. Comparisons with α-spectrometry and high resolution ICP-MS confirmed the suitability of the method when applied to different environmental matrices within the global fallout concentration range in the northern hemisphere as well as more contaminated sites. Operational detection limits were 0.5–1.5 fg/l for fresh waters and 0.03–0.1 ng/kg for lake sediments and saline marsh sediments.

Place, publisher, year, edition, pages
Berlin: Springer, 2008
National Category
Other Basic Medicine Chemical Sciences
Research subject
Chemistry
Identifiers
urn:nbn:se:oru:diva-3231 (URN)10.1007/s10967-006-7004-z (DOI)000251867200007 ()2-s2.0-37549053953 (Scopus ID)
Available from: 2007-02-13 Created: 2007-02-13 Last updated: 2018-01-13Bibliographically approved
2. Rapid method for ICP-MS analysis of plutonium in sediment samples
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2004 (English)Manuscript (preprint) (Other academic)
National Category
Chemical Sciences Environmental Sciences
Research subject
Enviromental Science
Identifiers
urn:nbn:se:oru:diva-3232 (URN)
Available from: 2007-02-13 Created: 2007-02-13 Last updated: 2017-10-18Bibliographically approved
3. Redistribution pf Pu, Am, Cs and Np in salt marsh sediment - Wigtown Merse, Irish Sea
Open this publication in new window or tab >>Redistribution pf Pu, Am, Cs and Np in salt marsh sediment - Wigtown Merse, Irish Sea
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(English)Manuscript (Other academic)
National Category
Chemical Sciences Environmental Sciences
Research subject
Enviromental Science
Identifiers
urn:nbn:se:oru:diva-3233 (URN)
Available from: 2007-02-13 Created: 2007-02-13 Last updated: 2017-10-18Bibliographically approved
4. Plutonium remobilization in a humic-rich lake
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2007 (English)In: Journal of Radioanalytical and Nuclear Chemistry, ISSN 0236-5731, E-ISSN 1588-2780, Vol. 277, no 1, p. 265-268Article in journal (Refereed) Published
Abstract [en]

Fresh water from Lake Svartsjön, Sweden, was collected and four fractions were prepared: (1) adsorption on DEAE, (2) flocculation with Ca2+, (3) co-precipitation with Fe hydrous oxide and (4) co-precipitation with Mn hydrous oxide. The plutonium level in the lake is 65 fg/l (222 μBq/l), measured by ICP-QMS and ICP-SFMS. Pronounced accumulation in fractions (1) (34%) and (2) (66%), combined with observed levels of organic matter indicate that plutonium is predominantly associated with organic matter. Measurements of isotopic ratios indicate that 77% of the plutonium originates from weapons testing and the remaining appears to originate from the Chernobyl accident.

National Category
Environmental Sciences Chemical Sciences
Research subject
Enviromental Science
Identifiers
urn:nbn:se:oru:diva-3234 (URN)10.1007/s10967-008-0741-4 (DOI)000257318800041 ()2-s2.0-46449100013 (Scopus ID)
Available from: 2007-02-13 Created: 2007-02-13 Last updated: 2017-12-14Bibliographically approved
5. Failure of 137Cs and 239,240Pu dating of lake sediments: fallout from nuclear weapons testing, the Chernobyl accident and redistribution processes?
Open this publication in new window or tab >>Failure of 137Cs and 239,240Pu dating of lake sediments: fallout from nuclear weapons testing, the Chernobyl accident and redistribution processes?
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(English)Manuscript (preprint) (Other academic)
National Category
Environmental Sciences
Research subject
Enviromental Science
Identifiers
urn:nbn:se:oru:diva-3235 (URN)
Available from: 2007-02-13 Created: 2007-02-13 Last updated: 2017-10-18Bibliographically approved

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