Chromatographic separations for fission products and actinides determination by different analytical techniques: mass spectrometry and radiometry

Due to the nuclear testing, reentry and disintegration of nuclear powered satellites, nuclear reactor accidents, uranium nuclear fuel cycle and nuclear weapons production, actinides have been introduced into the environment. Proposed disposal of high-level radioactive waste in mined repositories in...

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Autor: Perna, Lorenzo
Tipo de documento: Tese de doutorado
Data de publicação:2003
País:España
Recursos:Universitat Politècnica de Catalunya (UPC)
Repositório:UPCommons. Portal del coneixement obert de la UPC
Idioma:Inglês
OAI Identifier:oai:upcommons.upc.edu:2117/93744
Acesso em linha:https://hdl.handle.net/2117/93744
https://dx.doi.org/10.5821/dissertation-2117-93744
Nível de acesso:Acesso aberto
Palavra-chave:ICP-MS
UTEVA
cromatography
LSC
speciations
CS5
TEVA
lanthanides
actinides
spectrometry
2305. Química nuclear - 2301. Química analítica
Espectrometria de masses
Radiació -- Mesurament
Cromatografia
Àrees temàtiques de la UPC::Enginyeria química
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author Perna, Lorenzo
author_browse Perna, Lorenzo
author_facet Perna, Lorenzo
author_role author
collection UPCommons. Portal del coneixement obert de la UPC
description Due to the nuclear testing, reentry and disintegration of nuclear powered satellites, nuclear reactor accidents, uranium nuclear fuel cycle and nuclear weapons production, actinides have been introduced into the environment. Proposed disposal of high-level radioactive waste in mined repositories in geologic formation as well as the storage and disposal of uranium and plutonium from weapons dismantlement are further possible sources for actinide releases to the environment. The mobilization of radionuclides in the environment has been studied for many years with the prime objective of tracing the routes by which they accumulate in the food chain and become available for human consumption. Therefore, it is necessary to have available accurate, reliable and precise analytical methods to determine actinides and fission products in environmental samples as well as their isotopic ratio. These procedures should also be as fast as possible in order to give results in radiological emergency cases to take decision for radiation protection of the environment and human beings.<br/><br/>In this Ph.D. thesis, different kinds of phases for liquid chromatography have been tested to achieve the separation of the interfering elements and isotopes before the mass spectrometry and -spectrometry measurements. UTEVA and TEVA extraction resin (Eichrom Industries, USA) have been packed in chromatographic column as stationary phases and used for the separation of tri, tetra and hexavalent actinides and for the separation of trivalent lanthanides (La-Eu) and actinides, respectively. IonPac CS5A and CS10 (Dionex, Sunnyvale, USA) ion chromatography column were used for the simultaneous separation of actinide and lanthanides elements and for the actinides separation. The columns were coupled on-line to an Inductively Coupled Plasma Mass Spectrometer (ICP-MS) to solve isobaric interferences between actinide and lanthanide elements and off-line to a -spectrometer to solve the energy interferences between the analytes. Moreover, an investigation on the use of the UTEVA resin and IonPac Trace Cation Concentrator II column (TCC-II from Dionex, Sunnyvale, USA) as preconcentrator columns for actinide and lanthanide elements has been carried-out.<br/><br/>The analytical measurements have been made by mass spectrometric as well as by radiometric techniques. ICP-MS has been used for the characterization of spent nuclear fuels in terms of actinides and lanthanides content and burn-up calculation as well as for the determination of the long-lived actinides and lanthanides in environmental samples. - and -spectrometry have been used for 241Am determination in sediments and soils samples. -spectrometry and Liquid Scintillation Counting (LSC) have been used to analyze the eluted fractions from on-batch experiments. <br/><br/>The results obtained with the analytical procedures developed, for spent nuclear fuel solutions as well as for environmental samples, were always compared to those obtained by other independent techniques and good agreements have been always achieved.
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publishDate 2003
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publisher Universitat Politècnica de Catalunya
publisherStr Universitat Politècnica de Catalunya
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spelling Chromatographic separations for fission products and actinides determination by different analytical techniques: mass spectrometry and radiometry Perna, Lorenzo ICP-MS UTEVA cromatography LSC speciations CS5 TEVA lanthanides actinides spectrometry 2305. Química nuclear - 2301. Química analítica Espectrometria de masses Radiació -- Mesurament Cromatografia Àrees temàtiques de la UPC::Enginyeria química Due to the nuclear testing, reentry and disintegration of nuclear powered satellites, nuclear reactor accidents, uranium nuclear fuel cycle and nuclear weapons production, actinides have been introduced into the environment. Proposed disposal of high-level radioactive waste in mined repositories in geologic formation as well as the storage and disposal of uranium and plutonium from weapons dismantlement are further possible sources for actinide releases to the environment. The mobilization of radionuclides in the environment has been studied for many years with the prime objective of tracing the routes by which they accumulate in the food chain and become available for human consumption. Therefore, it is necessary to have available accurate, reliable and precise analytical methods to determine actinides and fission products in environmental samples as well as their isotopic ratio. These procedures should also be as fast as possible in order to give results in radiological emergency cases to take decision for radiation protection of the environment and human beings.<br/><br/>In this Ph.D. thesis, different kinds of phases for liquid chromatography have been tested to achieve the separation of the interfering elements and isotopes before the mass spectrometry and -spectrometry measurements. UTEVA and TEVA extraction resin (Eichrom Industries, USA) have been packed in chromatographic column as stationary phases and used for the separation of tri, tetra and hexavalent actinides and for the separation of trivalent lanthanides (La-Eu) and actinides, respectively. IonPac CS5A and CS10 (Dionex, Sunnyvale, USA) ion chromatography column were used for the simultaneous separation of actinide and lanthanides elements and for the actinides separation. The columns were coupled on-line to an Inductively Coupled Plasma Mass Spectrometer (ICP-MS) to solve isobaric interferences between actinide and lanthanide elements and off-line to a -spectrometer to solve the energy interferences between the analytes. Moreover, an investigation on the use of the UTEVA resin and IonPac Trace Cation Concentrator II column (TCC-II from Dionex, Sunnyvale, USA) as preconcentrator columns for actinide and lanthanide elements has been carried-out.<br/><br/>The analytical measurements have been made by mass spectrometric as well as by radiometric techniques. ICP-MS has been used for the characterization of spent nuclear fuels in terms of actinides and lanthanides content and burn-up calculation as well as for the determination of the long-lived actinides and lanthanides in environmental samples. - and -spectrometry have been used for 241Am determination in sediments and soils samples. -spectrometry and Liquid Scintillation Counting (LSC) have been used to analyze the eluted fractions from on-batch experiments. <br/><br/>The results obtained with the analytical procedures developed, for spent nuclear fuel solutions as well as for environmental samples, were always compared to those obtained by other independent techniques and good agreements have been always achieved. Universitat Politècnica de Catalunya https://hdl.handle.net/2117/93744 https://dx.doi.org/10.5821/dissertation-2117-93744
spellingShingle Chromatographic separations for fission products and actinides determination by different analytical techniques: mass spectrometry and radiometry
Perna, Lorenzo
ICP-MS
UTEVA
cromatography
LSC
speciations
CS5
TEVA
lanthanides
actinides
spectrometry
2305. Química nuclear - 2301. Química analítica
Espectrometria de masses
Radiació -- Mesurament
Cromatografia
Àrees temàtiques de la UPC::Enginyeria química
title Chromatographic separations for fission products and actinides determination by different analytical techniques: mass spectrometry and radiometry
title_full Chromatographic separations for fission products and actinides determination by different analytical techniques: mass spectrometry and radiometry
title_fullStr Chromatographic separations for fission products and actinides determination by different analytical techniques: mass spectrometry and radiometry
title_full_unstemmed Chromatographic separations for fission products and actinides determination by different analytical techniques: mass spectrometry and radiometry
title_short Chromatographic separations for fission products and actinides determination by different analytical techniques: mass spectrometry and radiometry
title_sort Chromatographic separations for fission products and actinides determination by different analytical techniques: mass spectrometry and radiometry
topic ICP-MS
UTEVA
cromatography
LSC
speciations
CS5
TEVA
lanthanides
actinides
spectrometry
2305. Química nuclear - 2301. Química analítica
Espectrometria de masses
Radiació -- Mesurament
Cromatografia
Àrees temàtiques de la UPC::Enginyeria química
topic_facet ICP-MS
UTEVA
cromatography
LSC
speciations
CS5
TEVA
lanthanides
actinides
spectrometry
2305. Química nuclear - 2301. Química analítica
Espectrometria de masses
Radiació -- Mesurament
Cromatografia
Àrees temàtiques de la UPC::Enginyeria química
url https://hdl.handle.net/2117/93744
https://dx.doi.org/10.5821/dissertation-2117-93744