Determination of precise ¹³⁵Cs/¹³⁷Cs ratio in environmental samples using sector field inductively coupled plasma mass spectrometry.

Abstract

Recent advances in sector field inductively coupled plasma mass spectrometry (ICP-SFMS) have led to significant sensitivity enhancements that expand the range of radionuclides measurable by ICP-MS. The increasing capability and performance of modern ICP-MS now allows analysis of medium-lived radionuclides previously undertaken using radiometric methods. A new generation ICP-SFMS was configured to achieve sensitivities up to 80,000 counts per second for a 1 ng/L (133)Cs solution, providing a detection limit of 1 pg/L. To extend this approach to environmental samples it has been necessary to develop an effective chemical separation scheme using ultrapure reagents. A procedure incorporating digestion, chemical separation and quantification by ICP-SFMS is presented for detection of the significant fission product radionuclides of cesium ((135)Cs and (137)Cs) at concentrations found in environmental and low level nuclear waste samples. This in turn enables measurement of the (135)Cs/(137)Cs ratio, which varies with the source of nuclear contamination, and can therefore provide a powerful dating and forensic tool compared to radiometric detection of (137)Cs alone. A detection limit in sediment samples of 0.05 ng/kg has been achieved for (135)Cs and (137)Cs, corresponding to 2.0 × 10(-3) and 160 mBq/kg, respectively. The critical issue is ensuring removal of barium to eliminate isobaric interferences arising from (135)Ba and (137)Ba. The ability to reliably measure (135)Cs/(137)Cs using a high specification laboratory ICP-SFMS now enables characterization of waste materials destined for nuclear waste repositories as well as extending options in environmental geochemical and nuclear forensics studies.