학술논문

Quantification of [99Tc]TcO4- in urine by means of anion-exchange chromatography–aerosol desolvation nebulization–inductively coupled plasma–mass spectrometry
Document Type
Original Paper
Source
Analytical and Bioanalytical Chemistry. 416(11):2849-2858
Subject
Pertechnetate
Elemental speciation
Hyphenated ICP-MS techniques
On-line calibration
Trace analysis
Language
English
ISSN
1618-2642
1618-2650
Abstract
To sensitively determine 99Tc, a new method for internal quantification of its most common and stable species, [99Tc]TcO4-O4-, was developed. Anion-exchange chromatography (IC) was coupled to inductively coupled plasma–mass spectrometry (ICP-MS) and equipped with an aerosol desolvation system to provide enhanced detection power. Due to a lack of commercial Tc standards, an isotope dilution-like approach using a Ru spike and called isobaric dilution analysis (IBDA) was used for internal quantification of 99Tc. This approach required knowledge of the sensitivities of 99Ru and 99Tc in ICP-MS. The latter was determined using an in-house prepared standard manufactured from decayed medical 99mTc-generator eluates. This standard was cleaned and preconcentrated using extraction chromatography with TEVA resin and quantified via total reflection X-ray fluorescence (TXRF) analysis. IC coupled to ICP-MS enabled to separate, detect and quantify [99Tc]TcO4-O4- as most stable Tc species in complex environments, which was demonstrated in a proof of concept. We quantified this species in untreated and undiluted raw urine collected from a patient, who previously underwent scintigraphy with a 99mTc-tracer, and determined a concentration of 19.6 ± 0.5 ng L−1. The developed method has a high utility to characterize a range of Tc-based radiopharmaceuticals, to determine concentrations, purity, and degradation products in complex samples without the need to assess activity parameters of 99(m)Tc.Graphical Abstract: