Efficient Production of High Specific Activity Thulium-167 at Paul Scherrer Institute and CERN-MEDICIS

Heinke, Reinhard; Chevallay, E.; Chrysalidis, K.; Cocolios, T. E.; Duchemin, Charlotte; Fedosseev, Valentin; Hurier, Sophie; Lambert, Laura; Leenders, Benji; Marsh, B. A.; Meulen, Nicholas P. van der; Sprung, P.; Stora, T.; Tosato, Marianna; Wilkins, S. G.; Zhang, Hui; Talip, Zeynep

doi:10.3389/fmed.2021.712374

Cited by 12 publications

(5 citation statements)

References 49 publications

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“…165 Ho (α, 2n) 15.9-65.8 Mukhrjee et al (1991); Martin and Pilger (1966); Gadkari et al (1997); Tárkányi et al (2010a); Usman et al (2020) nat Er (α, x) CERN-MEDICIS (Heinke et al, 2021). After an 8-h irradiation the highest produced activity was about 250 MBq.…”

Section: Target Reaction Energy Range (Mev) Referencementioning

confidence: 98%

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Study of thulium-167 cyclotron production: a potential medically-relevant radionuclide

Renaldin,

Dellepiane,

Braccini

et al. 2023

Front. Chem.

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Introduction: Targeted Radionuclide Therapy is used for the treatment of tumors in nuclear medicine, while sparing healthy tissues. Its application to cancer treatment is expanding. In particular, Auger-electron emitters potentially exhibit high efficacy in treating either small metastases or single tumor cells due to their short range in tissue. The aim of this paper is to study the feasibility of a large-scale production of thulium-167, an Auger-electron emitter radionuclide, in view of eventual systematic preclinical studies.Methods: Proton-irradiated enriched erbium-167 and erbium-168 oxides were used to measure the production cross sections of thulium-165, thulium-166, thulium-167, and thulium-168 utilizing an 18-MeV medical cyclotron equipped with a Beam Transport Line (BTL) at the Bern medical cyclotron laboratory. The comparison between the experimental and the TENDL 2021 theoretical cross-section results were in good agreement. Additional experiments were performed to assess the production yields of thulium radioisotopes in the BTL. Thulium-167 production yield was also measured irradiating five different target materials (167Er2O3, 168Er2O3, natTm2O3, natYb2O3, 171Yb2O3) with proton beams up to 63 MeV at the Injector II cyclotron of Paul Scherrer Institute.Results and Discussion: Our experiments showed that an 8-h irradiation of enriched ytterbium-171 oxide produced about 420 MBq of thulium-167 with a radionuclidic purity of 99.95% after 5 days of cooling time with a proton beam of about 53 MeV. Larger activities of thulium-167 can be achieved using enriched erbium-168 oxide with a 23-MeV proton beam, obtaining about 1 GBq after 8-h irradiation with a radionuclidic purity of <99.5% 5 days post end of bombardment.

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Section: Target Reaction Energy Range (Mev) Referencementioning

confidence: 98%

“…Their experimental results reported a maximum production yield of 8.3 MBq/ μ Ah. The same material was also irradiated with a 23-MeV proton beam at PSI for offline mass separation experiments at CERN-MEDICIS ( Heinke et al, 2021 ). After an 8-h irradiation the highest produced activity was about 250 MBq.…”

Section: Introductionmentioning

confidence: 99%

Study of thulium-167 cyclotron production: a potential medically-relevant radionuclide

Renaldin,

Dellepiane,

Braccini

et al. 2023

Front. Chem.

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“…The energy range of the detector is 3–10,000 keV, with relative efficiency of >40% and resolution of <1.2 keV (at 122 keV) and <2.0 keV (at 1332 keV) [ 40 ]. These latter measurements were used to quantify the separation efficiency at the end of the collections and any possible sputtering effect [ 41 ].…”

Section: Thick Targets and Mass Separatormentioning

confidence: 99%

“…BeF

and COF

are creating isobaric contamination at mass 47 with relatively high beam intensities. Because of high-beam-current-induced sputtering [ 41 ], the collection of mono-atomic

is not favored using a VADIS ion source if target material is being fluorinated. Chlorine injections in the target units were only available at MEDICIS due to the absence of a specified gas injection and neutralization system at Offline-1.…”

Section: Target Materials Developments and Sc Mass Separation At Medicismentioning

confidence: 99%

Target Development towards First Production of High-Molar- Activity 44gSc and 47Sc by Mass Separation at CERN-MEDICIS

Mamis,

Duchemin,

Berlin

et al. 2024

Pharmaceuticals

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The radionuclides 43Sc, 44g/mSc, and 47Sc can be produced cost-effectively in sufficient yield for medical research and applications by irradiating natTi and natV target materials with protons. Maximizing the production yield of the therapeutic 47Sc in the highest cross section energy range of 24–70 MeV results in the co-production of long-lived, high-γ-ray-energy 46Sc and 48Sc 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 natTi and natV 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 natTi, natV metallic foils, and natTiC 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 natTi and natV 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 44g/mSc, 46Sc, and 47Sc were obtained as mono-atomic and molecular ScF 2+ ion beams and collected for the first time at CERN-MEDICIS. Among all the investigated target materials, natTiC 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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“…Via a laser based multi-step excitation and ionization process, ideally only a single chemical element of interest is selectively ionized by laser photons, which are fine-tuned to resonances of strong transitions between atomic energy levels of the element ( 20 ). Due to the high efficiency of the laser ionization process via transitions into auto-ionizing levels, the ion beam production, and extraction throughput are strongly enhanced, while the product purity against other elements is in parallel improved due to the high selectivity of the resonance ionization technique ( 21 , 22 ). In combination with electromagnetic mass separation, the laser ion source thus provides an output, which is almost entirely free of any kind of isobaric or isotopic contaminations ( 23 ).…”

Section: Introductionmentioning

confidence: 99%

Terbium Medical Radioisotope Production: Laser Resonance Ionization Scheme Development

et al. 2021

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Terbium (Tb) is a promising element for the theranostic approach in nuclear medicine. The new CERN-MEDICIS facility aims for production of its medical radioisotopes to support related R&D projects in biomedicine. The use of laser resonance ionization is essential to provide radioisotopic yields of highest quantity and quality, specifically regarding purity. This paper presents the results of preparation and characterization of a suitable two-step laser resonance ionization process for Tb. By resonance excitation via an auto-ionizing level, the high ionization efficiency of 53% was achieved. To simulate realistic production conditions for Tb radioisotopes, the influence of a surplus of Gd atoms, which is a typical target material for Tb generation, was considered, showing the necessity of radiochemical purification procedures before mass separation. Nevertheless, a 10-fold enhancement of the Tb ion beam using laser resonance ionization was observed even with Gd:Tb atomic ratio of 100:1.

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Efficient Production of High Specific Activity Thulium-167 at Paul Scherrer Institute and CERN-MEDICIS

Cited by 12 publications

References 49 publications

Study of thulium-167 cyclotron production: a potential medically-relevant radionuclide

Study of thulium-167 cyclotron production: a potential medically-relevant radionuclide

Target Development towards First Production of High-Molar- Activity 44gSc and 47Sc by Mass Separation at CERN-MEDICIS

Terbium Medical Radioisotope Production: Laser Resonance Ionization Scheme Development

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