Evaluation of two extraction chromatography resins for scandium and titanium separation for medical isotope production

McLain, Derek R.; Brossard, Thomas; Kruijff, Robin M. de; Kankanamalage, Pavithra H. A.; Rotsch, David A.

doi:10.1007/s10967-023-08783-x

Cited by 5 publications

(5 citation statements)

References 45 publications

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“…In acidic media (>3 M HCl), DGA resin retains Sc, while Ti remains in the aqueous phase, indicating that a high resin loading would be necessary (likely increasing the elution volume). 47 Additionally, DGA resin has been shown to retain Fe 3+ (K d > 10 4 ) at relevant HCl concentrations, thus necessitating alternate strategies to remove Fe 3+ . 48 CA-Def resin was found to remove common contaminants such as Fe 3+ and to give a high separation yield in low volume without organic chelators as eluents, showing its potential use for the purification of 45 Ti.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…Recently, separations of 45 Ti and 45 Sc with DGA resin have been reported, indicating potential feasibility; however, some potential drawbacks are evident. In acidic media (>3 M HCl), DGA resin retains Sc, while Ti remains in the aqueous phase, indicating that a high resin loading would be necessary (likely increasing the elution volume) . Additionally, DGA resin has been shown to retain Fe 3+ ( K d > 10 4 ) at relevant HCl concentrations, thus necessitating alternate strategies to remove Fe 3+ .…”

Section: Resultsmentioning

confidence: 99%

“…Due to their neighboring positions on the periodic table, the production of Sc and Ti isotopes is inexorably linked. A summary of the production of 43 Sc, 44 Sc, and 47 Sc is provided in Table S1; notably several production routes involve the use of isotopically enriched Ti targets. Ti also has several radionuclides of interest for nuclear medicine applications.…”

Section: ■ Introductionmentioning

confidence: 99%

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De Novo Approaches to the Solid-Phase Separation of Titanium(IV) and Scandium(III): Translating Speciation Data to Selective On-Bead Chelation toward Applications in Nuclear Medicine

Koller,

Wang,

Deluca

et al. 2023

Inorg. Chem.

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The solution chemistry of the hydrolytic, early-transition-metal ions Ti4+ and Sc3+ represents a coordination chemistry challenge with important real-world implications, specifically in the context of 44Ti/44Sc and 45Ti/NatSc radiochemical separations. Unclear speciation of the solid and solution phases and tertiary mixtures of mineral acid, organic chelators, and solid supports are common confounds, necessitating tedious screening of multiple variables. Herein we describe how thermodynamic speciation data in solution informs the design of new solid-phase chelation approaches enabling separations of Ti4+ and Sc3+. The ligands catechol (benzene-1,2-diol) and deferiprone [3-hydroxy-1,2-dimethyl-4(1H)-pyridone] bind Ti4+ at significantly more acidic conditions (2–4 pH units) than Sc3+. Four chelating resins were synthesized using either catechol or deferiprone with two different solid supports. Of these, deferiprone appended to carboxylic acid polymer-functionalized silica (CA-Def) resin exhibited excellent binding affinity for Ti4+ across a wide range of HCl concentrations (1.0–0.001 M), whereas Sc3+ was only retained in dilute acidic conditions (0.01–0.001 M HCl). CA-Def resin produced separation factors of >100 (Ti/Sc) in 0.1–0.4 M HCl, and the corresponding K d values (>1000) show strong retention of Ti4+. A model 44Ti/44Sc generator was produced, showing 65 ± 3% yield of 44Sc in 200 μL of 0.2 M HCl with a significant 44Ti breakthrough of 0.1%, precluding use in its current form. Attempts, however, removed natSc in loading fractions and a dilute (0.4 M HCl) wash and recovered 80% of the loaded 45Ti activity in 400 μL of 6 M HCl. The previously validated 45Ti chelator TREN-CAM was used for comparative proof-of-concept reactions with the CA-Def eluent (in HCl) and literature-reported hydroxamate-based resin eluents (in citric acid). CA-Def shows improved radiolabeling efficiency with an apparent molar activity (AMA) of 0.177 mCi nmol–1, exceeding the established methods (0.026 mCi nmol–1) and improving the separation and recovery of 45Ti for positron emission tomography imaging applications.

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Section: ■ Results and Discussionmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

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De Novo Approaches to the Solid-Phase Separation of Titanium(IV) and Scandium(III): Translating Speciation Data to Selective On-Bead Chelation toward Applications in Nuclear Medicine

Koller,

Wang,

Deluca

et al. 2023

Inorg. Chem.

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“…The SPE fritted tube columns were adapted for the use of a syringe pump that allowed for constant flow rates, which reduced flow rate variability. Lastly, the presence of HF in the dissolved target solution would decrease the radioscandium affinity to BDGA resin; thus, the TiO 2 with NH 4 HF 2 was heated for 2 h to ensure complete removal of the HF before addition of concentrated HCl 24 , 27 . These improvements allowed for shorter evaporation time as the collected volume was decreased from 10 to 3 mL for either the 43 Sc or 47 Sc while maintaining an effective separation of the radioscandium from titanium target material and 48 V species 17 .…”

Section: Discussionmentioning

confidence: 99%

Production and purification of 43Sc and 47Sc from enriched [46Ti]TiO2 and [50Ti]TiO2 targets

Cingoranelli,

Bartels,

Kankanamalage

et al. 2023

Sci Rep

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The radioscandium isotopes, 43Sc and 47Sc, compose a promising elementally matched theranostic pair that can be used for the development of imaging and therapeutic radiopharmaceuticals with identical structures. This study aimed to investigate the production of high radionuclidic purity 43Sc from enriched [46Ti]TiO2 targets and 47Sc from enriched [50Ti]TiO2 targets and establish a target recycling technique. Enriched [46Ti]TiO2 targets were irradiated with 18 MeV protons, and enriched [50Ti]TiO2 targets were bombarded with 24 MeV protons. 43Sc and 47Sc were purified using ion chromatography attaining recovery yields of 91.7 ± 7.4% and 89.9 ± 3.9%, respectively. The average radionuclidic purity for 43Sc was 98.8 ± 0.3% and for 47Sc 91.5 ± 0.6%, while the average recovery of enriched titanium target material was 96 ± 4.0%. The highest apparent molar activity for [43Sc]Sc-DOTA was 23.2 GBq/µmol and 3.39 GBq/µmol for [47Sc]Sc-DOTA. This work demonstrates the feasibility of using enriched recycled [46Ti]TiO2 and [50Ti]TiO2 targets to produce high purity 43Sc and 47Sc as an elementally matched theranostic isotope pair.

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“…Despite the extensive studies on vanadium targets, the resulting yields of Sc-47 were relatively low in these cases. A few other methods were also reported, involving different nuclear reactions for the preparation of Sc-47, some with encouraging results [ 111 , 112 , 113 , 114 ].…”

Section: Properties and Effects Of Scandium In The Context Of Nuclear...mentioning

confidence: 99%

Towards Clinical Development of Scandium Radioisotope Complexes for Use in Nuclear Medicine: Encouraging Prospects with the Chelator 1,4,7,10-Tetraazacyclododecane-1,4,7,10-tetraacetic Acid (DOTA) and Its Analogues

Ioannidis,

Lefkaritis,

Georgiades

et al. 2024

IJMS

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Scandium (Sc) isotopes have recently attracted significant attention in the search for new radionuclides with potential uses in personalized medicine, especially in the treatment of specific cancer patient categories. In particular, Sc-43 and Sc-44, as positron emitters with a satisfactory half-life (3.9 and 4.0 h, respectively), are ideal for cancer diagnosis via Positron Emission Tomography (PET). On the other hand, Sc-47, as an emitter of beta particles and low gamma radiation, may be used as a therapeutic radionuclide, which also allows Single-Photon Emission Computed Tomography (SPECT) imaging. As these scandium isotopes follow the same biological pathway and chemical reactivity, they appear to fit perfectly into the “theranostic pair” concept. A step-by-step description, initiating from the moment of scandium isotope production and leading up to their preclinical and clinical trial applications, is presented. Recent developments related to the nuclear reactions selected and employed to produce the radionuclides Sc-43, Sc-44, and Sc-47, the chemical processing of these isotopes and the main target recovery methods are also included. Furthermore, the radiolabeling of the leading chelator, 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid (DOTA), and its structural analogues with scandium is also discussed and the advantages and disadvantages of scandium complexation are evaluated. Finally, a review of the preclinical studies and clinical trials involving scandium, as well as future challenges for its clinical uses and applications, are presented.

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Evaluation of two extraction chromatography resins for scandium and titanium separation for medical isotope production

Abstract: x Important note To cite this publication, please use the final published version (if applicable). Please check the document version above.

Cited by 5 publications

References 45 publications

De Novo Approaches to the Solid-Phase Separation of Titanium(IV) and Scandium(III): Translating Speciation Data to Selective On-Bead Chelation toward Applications in Nuclear Medicine

De Novo Approaches to the Solid-Phase Separation of Titanium(IV) and Scandium(III): Translating Speciation Data to Selective On-Bead Chelation toward Applications in Nuclear Medicine

Production and purification of 43Sc and 47Sc from enriched [46Ti]TiO2 and [50Ti]TiO2 targets

Towards Clinical Development of Scandium Radioisotope Complexes for Use in Nuclear Medicine: Encouraging Prospects with the Chelator 1,4,7,10-Tetraazacyclododecane-1,4,7,10-tetraacetic Acid (DOTA) and Its Analogues

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