• Vol 10, No 2 (2019)
  • Chemical Engineering

Recoiled and Sputtered Radioactive Impurities in 11 MeV Proton-based F-18 Production

Imam Kambali, Hari Suryanto, Parwanto , Kardinah , Nur Huda, Ferdy D. Listiawadi, Herta Astarina, Ratu R. Ismuha

Corresponding email: imamkey@batan.go.id


Cite this article as:
Kambali, I., Suryanto, H., Parwanto., Kardinah., Huda, N., Listiawadi, F.D., Astarina, H., Ismuha, R.R., 2019. Recoiled and Sputtered Radioactive Impurities in 11 MeV Proton-based F-18 Production. International Journal of Technology. Volume 10(2), pp. 300-308
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Imam Kambali Center for Radioisotope and Radiopharmaceutical Technology, National Nuclear Energy Agency (BATAN), Puspiptek Area, Serpong, South Tangerang, Indonesia
Hari Suryanto Center for Radioisotope and Radiopharmaceutical Technology, National Nuclear Energy Agency (BATAN), Puspiptek Area, Serpong, South Tangerang, Indonesia
Parwanto Center for Radioisotope and Radiopharmaceutical Technology, National Nuclear Energy Agency (BATAN), Puspiptek Area, Serpong, South Tangerang, Indonesia
Kardinah Dharmais Cancer Hospital, Jakarta, Indonesia
Nur Huda Dharmais Cancer Hospital, Jakarta, Indonesia
Ferdy D. Listiawadi Dharmais Cancer Hospital, Jakarta, Indonesia
Herta Astarina Dharmais Cancer Hospital, Jakarta, Indonesia
Ratu R. Ismuha Dharmais Cancer Hospital, Jakarta, Indonesia
Email to Corresponding Author

Abstract
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One of the quality control measures in F-18 radionuclide production concerns the impurities which might be present in the proton-irradiated enriched H218O target. In this investigation, proton irradiations of enriched water targets were theoretically simulated by the Stopping and Range of Ions in Matter (SRIM) 2013 codes, followed by experimental measurements. First, the SRIM-calculated data were employed to understand the origins of the recoiled and sputtered species. Using a portable Gamma Ray Spectroscopy System, recoiled and sputtered radioactive impurities were measured in the enriched water target following F-18 production using 11 MeV proton beams. The experimental results indicate that Havar window-originated Co-56 radionuclide and silver body-originated Ag-110m radioisotope were identified in the post-irradiated enriched H218O target. In addition, after passing the 18F solution through a column containing Quaternary Methyl Acetate (QMA) resin, none of the radionuclidic impurities were any longer observed to any great extent in the sample.

Cyclotron; F-18 radionuclide; Gamma ray spectroscopy; Radionuclidic impurity; SRIM

Introduction

Over the past few years, Positron Emission Tomography (PET) has been one of the most applied modalities in nuclear medicine. It requires positron-emitting radionuclides, such as fluorine-18 (F-18) in the form of 18F-Fluorodeoxyglucose (18FDG), 18F-Fluoro-L-dopa (18FDOPA), and 18F-Fluoro-L-tyrosine 18F-FTYR (Xie, 2011; Je et al., 2012; Libert et al., 2014; Lemaire et al., 2015; Jung et al., 2016). Fluorine-18 can be produced via 18O(p,n)18F nuclear reaction, in which an enriched water (H21818O) target is bombarded by relatively low to medium energy protons (Hjelstuen et al., 2011) in a target system. The target system usually consists of a target body made of silver and a Havar window separating the cyclotron chamber from the target (Kambali et al., 2010; Kambali et al., 2016), although a niobium (Nb)-based window has also been used (Köhler et al., 2013).

During proton beam irradiation, the beam has to pass through a Havar window before reaching the enriched water target; therefore, the Havar foil, which consists of cobalt (42.5%), chromium (20%), iron (18.1%), nickel (13%), tungsten (2.8%), molybdenum (2%), manganese (1.6%), carbon (0.2%), beryllium (0.04%) and some other trace elements, could become radioactive

atoms, depending on the proton energy. This occurrence could impact on quality control assessment, and from a broader perspective it could eventually give rise to patient safety concerns.

A previous investigation discovered that during routine production of F-18 radionuclide using 11 MeV proton beams, Co-56 radionuclide was generated via 56Fe(p,n)56Co nuclear reaction as the proton beam passed through the Havar window (Kambali et al., 2016). For higher proton energy (16.5 MeV), Bowden et al. (2009) observed other radionuclides such as V-48, Cr-51, Mn-52, Mn-54, Co-57, Co-58, Tc-95m, Tc-96, Cd-109, Re-183 and Re-184 in the Havar foil. Using Nb foil as the window separating the cyclotron vacuum chamber and enriched water target, Köhler et al. (2013) identified further radionuclides, including Zr-89, Nb-92m, Mo-93m, Tc-95, and Tc-96, when they irradiated the enriched water with 18 MeV protons.

Radionuclides generated during proton bombardment of Havar or Nb windows have previously been found to contaminate the enriched water target (Bowden et al., 2009; Hjelstuen et al., 2011; Köhler et al., 2013;). This work aims to comprehensively identify the recoiled and sputtered radionuclidic impurities during F-18 production using a relatively low (11 MeV) proton accelerating cyclotron. For the first time, the properties of the Havar window- and silver body-originated recoils are discussed in terms of their respective absorbed and kinetic energy after they experience collisions with the incoming proton beams, as well as their collisions with individual H and O atoms in the enriched water. In addition, the recoiled and sputtered yields are also highlighted based on the Stopping and Range of Ions in Matter (SRIM) calculated results.

Conclusion

A theoretical and experimental study of recoiled and sputtered radionuclidic impurities has been conducted. The SRIM codes have been employed to study the recoil distributions, kinetic energy and sputtering yields of individual Havar atoms, a silver body and an enriched H218O target. Based on the SRIM-calculated results, the Co, Cr, Fe and Ni recoil yields increase near the far side of the Havar surface (at a distance of 50 µm), which directly touches the enriched water target. These atoms have the highest probabilities of being recoiled off the Havar surface and then falling into the enriched water target or even hitting the silver body, which could result in further sputtering of the Ag atoms. The experimental data indicate that Havar window-originated 56Co atoms and silver body-originated 110mAg atoms are identified in the post-irradiated water target, although a significant presence in the 18F solution is no longer observed after passing it through a QMA column. The impurities remain detectable in the 18F solution after a 3-day cooling period. Future work will concentrate on the measurement of non-radioactive recoiled and sputtered atoms in the enriched water target, as well as adsorption of the impurities.

Acknowledgement

This research project is supported by The World Academy of Sciences (TWAS) under the Principal Investigator’s Research Grant Number 15-020 RG/PHYS/AS_I – FR3240287075, as well as the Indonesian National Nuclear Energy Agency (BATAN). Moreover, kind support from the Dharmais Cancer Hospital has also greatly contributed to the success of the project. Technical support from the cyclotron technicians and staff at Dharmais Cancer Hospital in Jakarta is also gratefully acknowledged.

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