Target Development towards First Production of High-Molar- Activity <sup>44g</sup>Sc and <sup>47</sup>Sc by Mass Separation at CERN-MEDICIS

The radionuclides <sup>43</sup>Sc, <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow&g...

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Main Authors: Edgars Mamis, Charlotte Duchemin, Valentina Berlin, Cyril Bernerd, Mathieu Bovigny, Eric Chevallay, Bernard Crepieux, Vadim Maratovich Gadelshin, Reinhard Heinke, Ronaldo Mendez Hernandez, Jake David Johnson, Patrīcija Kalniņa, Alexandros Koliatos, Laura Lambert, Ralf Erik Rossel, Sebastian Rothe, Julien Thiboud, Felix Weber, Klaus Wendt, Rudolfs Jānis Zabolockis, Elīna Pajuste, Thierry Stora
Format: Article
Language:English
Published: MDPI AG 2024-03-01
Series:Pharmaceuticals
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Online Access:https://www.mdpi.com/1424-8247/17/3/390
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author Edgars Mamis
Charlotte Duchemin
Valentina Berlin
Cyril Bernerd
Mathieu Bovigny
Eric Chevallay
Bernard Crepieux
Vadim Maratovich Gadelshin
Reinhard Heinke
Ronaldo Mendez Hernandez
Jake David Johnson
Patrīcija Kalniņa
Alexandros Koliatos
Laura Lambert
Ralf Erik Rossel
Sebastian Rothe
Julien Thiboud
Felix Weber
Klaus Wendt
Rudolfs Jānis Zabolockis
Elīna Pajuste
Thierry Stora
author_facet Edgars Mamis
Charlotte Duchemin
Valentina Berlin
Cyril Bernerd
Mathieu Bovigny
Eric Chevallay
Bernard Crepieux
Vadim Maratovich Gadelshin
Reinhard Heinke
Ronaldo Mendez Hernandez
Jake David Johnson
Patrīcija Kalniņa
Alexandros Koliatos
Laura Lambert
Ralf Erik Rossel
Sebastian Rothe
Julien Thiboud
Felix Weber
Klaus Wendt
Rudolfs Jānis Zabolockis
Elīna Pajuste
Thierry Stora
author_sort Edgars Mamis
collection DOAJ
description The radionuclides <sup>43</sup>Sc, <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mn>44</mn><mi>g</mi><mo>/</mo><mi>m</mi></mrow></msup></semantics></math></inline-formula>Sc, and <sup>47</sup>Sc can be produced cost-effectively in sufficient yield for medical research and applications by irradiating <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>Ti and <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>V target materials with protons. Maximizing the production yield of the therapeutic <sup>47</sup>Sc in the highest cross section energy range of 24–70 MeV results in the co-production of long-lived, high-<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mi>γ</mi></semantics></math></inline-formula>-ray-energy <sup>46</sup>Sc and <sup>48</sup>Sc contaminants if one does not use enriched target materials. Mass separation can be used to obtain high molar activity and isotopically pure Sc radionuclides from natural target materials; however, suitable operational conditions to obtain relevant activity released from irradiated <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>Ti and <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>V have not yet been established at CERN-MEDICIS and ISOLDE. The objective of this work was to develop target units for the production, release, and purification of Sc radionuclides by mass separation as well as to investigate target materials for the mass separation that are compatible with high-yield Sc radionuclide production in the 9–70 MeV proton energy range. In this study, the in-target production yield obtained at MEDICIS with 1.4 GeV protons is compared with the production yield that can be reached with commercially available cyclotrons. The thick-target materials were irradiated at MEDICIS and comprised of metallic <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>Ti, <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>V metallic foils, and <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>TiC pellets. The produced radionuclides were subsequently released, ionized, and extracted from various target and ion source units and mass separated. Mono-atomic Sc laser and molecule ionization with forced-electron-beam-induced arc-discharge ion sources were investigated. Sc radionuclide production in thick <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>Ti and <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>V targets at MEDICIS is equivalent to low- to medium-energy cyclotron-irradiated targets at medically relevant yields, furthermore benefiting from the mass separation possibility. A two-step laser resonance ionization scheme was used to obtain mono-atomic Sc ion beams. Sc radionuclide release from irradiated target units most effectively could be promoted by volatile scandium fluoride formation. Thus, isotopically pure <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mn>44</mn><mi>g</mi><mo>/</mo><mi>m</mi></mrow></msup></semantics></math></inline-formula>Sc, <sup>46</sup>Sc, and <sup>47</sup>Sc were obtained as mono-atomic and molecular ScF<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msubsup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mn>2</mn><mo>+</mo></msubsup></semantics></math></inline-formula> ion beams and collected for the first time at CERN-MEDICIS. Among all the investigated target materials, <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>TiC is the most suitable target material for Sc mass separation as molecular halide beams, due to high possible operating temperatures and sustained release.
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spelling doaj.art-875ce47a032c4caa91e58245a23a67412024-03-27T13:59:28ZengMDPI AGPharmaceuticals1424-82472024-03-0117339010.3390/ph17030390Target Development towards First Production of High-Molar- Activity <sup>44g</sup>Sc and <sup>47</sup>Sc by Mass Separation at CERN-MEDICISEdgars Mamis0Charlotte Duchemin1Valentina Berlin2Cyril Bernerd3Mathieu Bovigny4Eric Chevallay5Bernard Crepieux6Vadim Maratovich Gadelshin7Reinhard Heinke8Ronaldo Mendez Hernandez9Jake David Johnson10Patrīcija Kalniņa11Alexandros Koliatos12Laura Lambert13Ralf Erik Rossel14Sebastian Rothe15Julien Thiboud16Felix Weber17Klaus Wendt18Rudolfs Jānis Zabolockis19Elīna Pajuste20Thierry Stora21European Organization for Nuclear Research (CERN), Esplanade des Particules 1, 1211 Geneva, SwitzerlandEuropean Organization for Nuclear Research (CERN), Esplanade des Particules 1, 1211 Geneva, SwitzerlandEuropean Organization for Nuclear Research (CERN), Esplanade des Particules 1, 1211 Geneva, SwitzerlandEuropean Organization for Nuclear Research (CERN), Esplanade des Particules 1, 1211 Geneva, SwitzerlandEuropean Organization for Nuclear Research (CERN), Esplanade des Particules 1, 1211 Geneva, SwitzerlandEuropean Organization for Nuclear Research (CERN), Esplanade des Particules 1, 1211 Geneva, SwitzerlandEuropean Organization for Nuclear Research (CERN), Esplanade des Particules 1, 1211 Geneva, SwitzerlandInstitut für Physik, Johannes Gutenberg Universität, Staudingerweg 7, 55128 Mainz, GermanyEuropean Organization for Nuclear Research (CERN), Esplanade des Particules 1, 1211 Geneva, SwitzerlandEuropean Organization for Nuclear Research (CERN), Esplanade des Particules 1, 1211 Geneva, SwitzerlandEuropean Organization for Nuclear Research (CERN), Esplanade des Particules 1, 1211 Geneva, SwitzerlandEuropean Organization for Nuclear Research (CERN), Esplanade des Particules 1, 1211 Geneva, SwitzerlandEuropean Organization for Nuclear Research (CERN), Esplanade des Particules 1, 1211 Geneva, SwitzerlandEuropean Organization for Nuclear Research (CERN), Esplanade des Particules 1, 1211 Geneva, SwitzerlandEuropean Organization for Nuclear Research (CERN), Esplanade des Particules 1, 1211 Geneva, SwitzerlandEuropean Organization for Nuclear Research (CERN), Esplanade des Particules 1, 1211 Geneva, SwitzerlandEuropean Organization for Nuclear Research (CERN), Esplanade des Particules 1, 1211 Geneva, SwitzerlandInstitut für Physik, Johannes Gutenberg Universität, Staudingerweg 7, 55128 Mainz, GermanyInstitut für Physik, Johannes Gutenberg Universität, Staudingerweg 7, 55128 Mainz, GermanyInstitute of Chemical Physics (ICP), University of Latvia, Jelgavas Street 1, LV-1004 Riga, LatviaInstitute of Chemical Physics (ICP), University of Latvia, Jelgavas Street 1, LV-1004 Riga, LatviaEuropean Organization for Nuclear Research (CERN), Esplanade des Particules 1, 1211 Geneva, SwitzerlandThe radionuclides <sup>43</sup>Sc, <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mn>44</mn><mi>g</mi><mo>/</mo><mi>m</mi></mrow></msup></semantics></math></inline-formula>Sc, and <sup>47</sup>Sc can be produced cost-effectively in sufficient yield for medical research and applications by irradiating <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>Ti and <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>V target materials with protons. Maximizing the production yield of the therapeutic <sup>47</sup>Sc in the highest cross section energy range of 24–70 MeV results in the co-production of long-lived, high-<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mi>γ</mi></semantics></math></inline-formula>-ray-energy <sup>46</sup>Sc and <sup>48</sup>Sc contaminants if one does not use enriched target materials. Mass separation can be used to obtain high molar activity and isotopically pure Sc radionuclides from natural target materials; however, suitable operational conditions to obtain relevant activity released from irradiated <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>Ti and <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>V have not yet been established at CERN-MEDICIS and ISOLDE. The objective of this work was to develop target units for the production, release, and purification of Sc radionuclides by mass separation as well as to investigate target materials for the mass separation that are compatible with high-yield Sc radionuclide production in the 9–70 MeV proton energy range. In this study, the in-target production yield obtained at MEDICIS with 1.4 GeV protons is compared with the production yield that can be reached with commercially available cyclotrons. The thick-target materials were irradiated at MEDICIS and comprised of metallic <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>Ti, <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>V metallic foils, and <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>TiC pellets. The produced radionuclides were subsequently released, ionized, and extracted from various target and ion source units and mass separated. Mono-atomic Sc laser and molecule ionization with forced-electron-beam-induced arc-discharge ion sources were investigated. Sc radionuclide production in thick <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>Ti and <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>V targets at MEDICIS is equivalent to low- to medium-energy cyclotron-irradiated targets at medically relevant yields, furthermore benefiting from the mass separation possibility. A two-step laser resonance ionization scheme was used to obtain mono-atomic Sc ion beams. Sc radionuclide release from irradiated target units most effectively could be promoted by volatile scandium fluoride formation. Thus, isotopically pure <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mn>44</mn><mi>g</mi><mo>/</mo><mi>m</mi></mrow></msup></semantics></math></inline-formula>Sc, <sup>46</sup>Sc, and <sup>47</sup>Sc were obtained as mono-atomic and molecular ScF<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msubsup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mn>2</mn><mo>+</mo></msubsup></semantics></math></inline-formula> ion beams and collected for the first time at CERN-MEDICIS. Among all the investigated target materials, <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow><mspace width="-2.pt"></mspace><mo> </mo></mrow><mrow><mi>n</mi><mi>a</mi><mi>t</mi></mrow></msup></semantics></math></inline-formula>TiC is the most suitable target material for Sc mass separation as molecular halide beams, due to high possible operating temperatures and sustained release.https://www.mdpi.com/1424-8247/17/3/390scandium radionuclidesmass separationISOL target unitstarget materialslaser resonant ionizationmolecular beams
spellingShingle Edgars Mamis
Charlotte Duchemin
Valentina Berlin
Cyril Bernerd
Mathieu Bovigny
Eric Chevallay
Bernard Crepieux
Vadim Maratovich Gadelshin
Reinhard Heinke
Ronaldo Mendez Hernandez
Jake David Johnson
Patrīcija Kalniņa
Alexandros Koliatos
Laura Lambert
Ralf Erik Rossel
Sebastian Rothe
Julien Thiboud
Felix Weber
Klaus Wendt
Rudolfs Jānis Zabolockis
Elīna Pajuste
Thierry Stora
Target Development towards First Production of High-Molar- Activity <sup>44g</sup>Sc and <sup>47</sup>Sc by Mass Separation at CERN-MEDICIS
Pharmaceuticals
scandium radionuclides
mass separation
ISOL target units
target materials
laser resonant ionization
molecular beams
title Target Development towards First Production of High-Molar- Activity <sup>44g</sup>Sc and <sup>47</sup>Sc by Mass Separation at CERN-MEDICIS
title_full Target Development towards First Production of High-Molar- Activity <sup>44g</sup>Sc and <sup>47</sup>Sc by Mass Separation at CERN-MEDICIS
title_fullStr Target Development towards First Production of High-Molar- Activity <sup>44g</sup>Sc and <sup>47</sup>Sc by Mass Separation at CERN-MEDICIS
title_full_unstemmed Target Development towards First Production of High-Molar- Activity <sup>44g</sup>Sc and <sup>47</sup>Sc by Mass Separation at CERN-MEDICIS
title_short Target Development towards First Production of High-Molar- Activity <sup>44g</sup>Sc and <sup>47</sup>Sc by Mass Separation at CERN-MEDICIS
title_sort target development towards first production of high molar activity sup 44g sup sc and sup 47 sup sc by mass separation at cern medicis
topic scandium radionuclides
mass separation
ISOL target units
target materials
laser resonant ionization
molecular beams
url https://www.mdpi.com/1424-8247/17/3/390
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