Activity determination of 18F using liquid scintillation beta-efficiency extrapolation and non-extrapolation methods

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Highlights

  • Absolute standardization of F-18 using beta-efficiency extrapolation and-non extrapolation methods.

  • Liquid scintillation coincidence counting.

  • Double-tube efficiency adapted for threshold above second monopeak for non-extrapolation method.

  • Excellent agreement between the methods.

Abstract

The absolute activity of 18F was determined using 4πβγ liquid scintillation coincidence counting using beta-efficiency extrapolation. An ionization chamber factor was determined for use during a SIRTI comparison, for which results are presented. A non-extrapolation method based on a detection efficiency analysis was also employed using an adaptation of the double-phototube coincidence efficiency for a threshold above the second monopeak. Results and uncertainty budgets for the two methods are presented and discussed.

Introduction

The National Metrology Institute of South Africa (NMISA) performed its first absolute standardization of a18F solution. The method employed 4πβ-γ coincidence counting using liquid scintillation (LS) in the beta-plus channel. The result of the standardization was used to determine a calibration factor for 18F for the NMISA secondary standard ionization chamber. One month later NMISA participated in the BIPM.RI(II)–K4.F-18 International Reference System Transfer Instrument (SIRTI) comparison (Michotte et al., 2017), for which NMISA was only the fourth participant at that time.

Fluorine-18 is the most common positron emission tomography (PET) radiopharmaceutical used for diagnostics. Literature indicates that 18F is a simple radionuclide to standardize (Roteta et al., 2006; Rodrigues et al., 2011; Kim et al., 2012) due to its straightforward decay scheme and high β+ maximum energy of 633.9 keV resulting in a high efficiency in the liquid scintillator. Experimentally, the biggest challenge is measurement logistics due to its short half-life of 1.8 h, which was overcome at NMISA by using a fifteen-channel double- and triple-coincidence unit for simultaneous measurements at various electronic thresholds (Simpson and Meyer, 1988), to allow for activity determination through the liquid scintillation efficiency extrapolation technique.

We present a detection efficiency analysis of the 4πβ-γ coincidence counting method, accounting for both 511 keV annihilation photons, which is more complete than that currently found in the literature (Roteta et al., 2006; Rodrigues et al., 2011) where only one 511 keV photon is considered. The high β+-efficiency leads to a small extrapolation range and corresponding uncertainty.

Additionally, a non-extrapolation method (Simpson and Morris, 2004; van Rooy et al., 2016) was employed to analyse data corresponding to only the first threshold above the second monopeak, advantageous if multi-discrimination data acquisition is not possible. The detection efficiency analysis indicated that the measured liquid scintillation efficiency is a function of the positron- and 511 keV Compton electron efficiency. These efficiencies were determined from the theoretical formulae for the double-phototube coincidence efficiencies, modified for a threshold set above the second monopeak, and using the theoretical positron- and Compton spectra. Subsequently, the activity was determined.

Section snippets

Detection efficiency analysis

18F decays 96.86% via β+-decay and 3.14% via electron-capture (EC) directly to the ground state of 18O (Fig. 1). The threshold in the liquid scintillation channel is set above the second monopeak to eliminate detection of the X-rays and Auger electrons from the EC branch. Considering β+ particles and both counter-propagating 511 keV photons interacting in the liquid scintillator (three-photon annihilation assumed to be negligible), the count rate B is given by:B=Nf[εβ+(1εβ)εβv1+(1εβ)(1εβv1)εβ

Source preparation

A stock solution of 18F Fluorodeoxyglucose (FDG) was used to prepare four liquid scintillation counting sources. Accurately weighed aliquots of the solution were dispensed into 12 mL of scintillation cocktail inside custom made flat-faced cylindrical glass vials. Source masses (buoyancy corrected) ranged between 44 mg and 67 mg. Quicksafe A from Zinsser Analytic was used as the liquid scintillation cocktail, to which 3 mL L−1 of 1 M HCl had been added as a precaution against possible adsorption.

Discussion and conclusions

NMISA successfully participated in its first SIRTI comparison for 18F. Two methods for the primary standardization of 18F were employed using liquid scintillation coincidence counting. The conventional beta-efficiency extrapolation method was used to determine an ionization chamber factor for the SIRTI comparison. The NMISA equivalent activity is 0.34% higher than the KCRV and in agreement within one sigma. A non-extrapolation method was also employed by utilising a formula derived from an

CRediT authorship contribution statement

M.W. van Rooy: Conceptualization, Methodology, Supervision, Software, Formal analysis, Writing - original draft, Writing - review & editing. M.J. van Staden: Conceptualization, Methodology, Supervision, Writing - review & editing. B.R.S. Simpson: Conceptualization, Methodology, Supervision, Writing - review & editing. J. Lubbe: Conceptualization, Writing - review & editing.

Declaration of competing interest

There are no interests to declare.

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