Abstract
This paper presents a total evaporation method for the analysis of sub-picogram quantities of Pu, utilizing an array of multiple ion counters. Data from three standards are presented to assess the utility of the technique. An external precision of 1.5% RSD (2σ) was achieved on aliquots approaching 100 fg for the minor 240Pu isotope. Accurate analysis of <1 femtogram of 240Pu, is achievable, with an external reproducibility of better than 10% RSD (2σ). This new technique represents a significant advance in the total evaporation method and will allow routine measurement of femtogram sized Pu samples by thermal ionization mass spectrometry.
Similar content being viewed by others
References
Wagner SE, Boone S, Chamberlain JW, Duffy CJ, Efurd DW, Israel KM, Koski NL, Kottmann DL, Lewis D, Lindhal PC, Roensch FR, Steiner RE (2001) Practical application of thermal ionization mass spectrometry for the determination of plutonium for the LANL Bioassay Program. J Radioanal Nucl Chem 248:423–429
LaMont SP, Shick CR, Cable-Dunlap P, Fauth DJ, LaBone TR (2005) Plutonium determination in bioassay samples using radiochemical thermal ionization mass spectrometry. J Radioanal Nucl Chem 263:477–481
Callis EL, Abernathey RM (1991) High-precision isotopic analysis of uranium and plutonium by total sample volatilization and signal integration. Int J Mass Spectrom Ion Process 103:93–105
Burger S, Riciputi LR, Bostick DA, Turgeon S, McBay EH, Lavelle M (2009) Isotope ratio analysis of actinides, fission products, and geolocators by high-efficiency multi-collector thermal ionization mass spectrometry. Int J Mass Spectrom 286:70–82
Park J, Jeong K, Song K (2013) Isotopic analysis of uranium and plutonium at ultra trace levels using thermal ionization mass spectrometry with simultaneous measurements. Asian J Chem 25:7061–7063
Romkowski M, Franzini S, Koch L (1987) Mass-spectrometric analysis of sub-nanocurie samples of uranium and plutonium. 8th Annual ESARDA Symposium, Commission European Comm., London p. 12
Fiedler R (1995) Total evaporation measurements: experience with multi-collector instruments and a thermal ionization quadrapole mass-spectrometer. Int J Mass Spectrom Ion Process 146:91–97
Stanley FE, Byerly BL, Thomas MR, Spencer KJ (2016) Static mixed array total evaporation for improved quantitation of plutonium minor isotopes in small samples. J Am Soc Mass Spectrom 27:1136–1138
Richter S, Goldberg SA (2003) Improved techniques for high accuracy isotope ratio measurments of nuclear materials using thermal ionization mass spectrometry. Int J Mass Spectrom 229:181–197
Mathew K, O’Connor G, Hasozbek A, Kraiem M (2013) Total evaporation method for uranium isotope-amount ratio measurements. J Anal At Spectrom 28:866–876
Mathew K, Hasozbek A (2016) Comparison of mass spectrometric methods (TE, MTE and conventional) for uranium isotope ratio measurements. J Radioanal Nucl Chem 307:1681–1687
Sturm M, Richter S, Aregbe Y, Wellum R, Prohaska T (2016) Optimized chemical separation and measurement by TE TIMS using carburized filaments for uranium isotope ratio measurements applied to plutonium chronometry. Anal Chem 88:6223–6230
Souders KA, Sylvester PJ (2008) In: Sylvester P (ed) Laser ablation ICP-MS in the earth sciences: current practices and outstanding issues
Smith DH, Walker RL, Carter JA (1979) Resin bead mass spectrometry—an analytical technique for safeguarding Pu and U. Nucl Mater Manag 8:66–71
IAEA (1986) Decay data of the transactinium nuclides. Technical Reports Series No. 261
Smith DH, Duckworth DC, Bostick DT, Coleman RM, McPherson RL, McKown HS (1994) Analysis of femtogram-sized plutonium samples by thermal ionization mass spectrometry. Proceedings of the 42nd ASMS Conference on Mass Spectrometry and Allied Topics, Chicago IL, USA, 1994, p. 839
Kelley JM, Bond LA, Beasley TM (1999) Global distribution of Pu isotopes and 237Np. Sci Tot Environ 237(238):483–500
Taylor RN, Warneke T, Milton JA, Croudace IW, Warwick PE, Nesbitt RW (2003) Multiple ion counting determination of plutonium isotope ratios using multi-collector ICP-MS. J Anal At Spectrom 18:480–484
Mialle S, Quemet A, Ponvienne A, Gourgiotis A, Aubert M, Isnard H, Chartier F (2012) The use of total evaporation method using channeltron electronc multipliers by thermal ionization mass spectrometry for europium isotope measurements on picogram sample amounts. Int J Mass Spectrom 309:141–147
Acknowledgements
The authors thank Robert Guest, Isotopx Ltd., for detailed discussions on the optimization of the multiple ion counters used in this study. Andy Nunn & Daniel Gurganus provided useful discussion on total evaporation. Los Alamos National Laboratory is operated by Los Alamos National Security, LLC for the U.S. Department of Energy under Contract number DE-AC52-06NA25396. This publication is LA-UR-17-21703.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Inglis, J.D., Maassen, J., Kara, A. et al. A multiple ion counter total evaporation (MICTE) method for precise analysis of plutonium by thermal ionization mass spectrometry. J Radioanal Nucl Chem 312, 663–673 (2017). https://doi.org/10.1007/s10967-017-5259-1
Received:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10967-017-5259-1