Analytical and Bioanalytical Chemistry

, Volume 411, Issue 5, pp 973–983 | Cite as

Determination of 107Pd in Pd purified by selective precipitation from spent nuclear fuel by laser ablation ICP-MS

  • Shiho AsaiEmail author
  • Masaki Ohata
  • Takumi Yomogida
  • Morihisa Saeki
  • Hironori Ohba
  • Yukiko Hanzawa
  • Takuma Horita
  • Yoshihiro Kitatsuji
Paper in Forefront


Determination of radiopalladium 107Pd is required to ensure radiation safety of the Pd extracted from spent nuclear fuel for recycling or disposal. We employed nanosecond laser ablation inductively coupled plasma quadrupole mass spectrometry (ns-LA-ICP-QMS) to simplify the analytical procedure of 107Pd. Pd was separated through a selective Pd precipitation reaction induced by pulsed laser irradiation that reduces Pd(II) ions to metal Pd(0). Laser ablation facilitates direct measurement of the Pd precipitates, skipping the dissolution and dilution procedure with aqua regia and HCl, which causes serious corrosion damage to the introduction system of the ICP. In the present study, 102Pd in natural Pd standard solution was used as an internal standard owing to its absence in spent nuclear fuel. Pd precipitates with diameters ranging from 0.2 to 0.5 μm, obtained by pulsed laser irradiation, were embedded uniformly on the surface of the centrifugal filter to form a microscopically thin and flat Pd surface. The resulting homogeneous Pd layer is suitable for obtaining a stable signal ratio of 107Pd/102Pd (< 4%, 2RSD). The mass bias-corrected ratio of 107Pd/102Pd and the amount of 107Pd were 0.163 ± 0.004 and 17.8 ± 0.6 ng, respectively, which correspond to the values obtained by solution nebulization measurement after the dissolution of identical Pd precipitates.

Graphical abstract


107Pd Spent nuclear fuel Laser ablation ICP-MS Laser-induced photoreduction Precipitation Nanoparticles 



The authors are grateful to Mr. Nobuaki Kohno of Radiation Application Development Association (RADA) for insightful comments on this work.

Compliance with ethical standards

Conflict of interest

The authors declare that they have no conflict of interest.

Supplementary material

216_2018_1527_MOESM1_ESM.pdf (108 kb)
ESM 1 (PDF 107 kb)


  1. 1.
    Okumura K, Okamoto T. Nuclides inventories of spent fuels form light water reactors. JAEA-Data/Code 2011-020, 2012/2.Google Scholar
  2. 2.
    Qi L, Gregoire DC, Zhou MF, Malpas J. Determination of Pt, Pd, Ru and Ir in geological samples by ID-ICP-MS using sodium peroxide fusion and Te co-precipitation. Geochem J. 2003;37(5):557–65. Scholar
  3. 3.
    Gómez MB, Gómez MM, Palacios MA. ICP-MS determination of Pt, Pd and Rh in airborne and road dust after tellurium coprecipitation. J Anal At Spectrom. 2003;18(1):80–3. Scholar
  4. 4.
    Rudolph E, Limbeck A, Hann S. Novel matrix separation—on-line pre-concentration procedure for accurate quantification of palladium in environmental samples by isotope dilution inductively coupled plasma sector field mass spectrometry. J Anal At Spectrom. 2006;21(11):1287–93. Scholar
  5. 5.
    Nischkauer W, Neouze MA, Vanhaecke F, Limbeck A. Extraction and pre-concentration of platinum and palladium from microwave-digested road dust via ion exchanging mesoporous silica microparticles prior to their quantification by quadrupole ICP-MS. Microchim Acta. 2015;182(15–16):2369–76. Scholar
  6. 6.
    Ek M, Hunt AC, Schonbachler M. A new method for high-precision palladium isotope analyses of iron meteorites and other metal samples. J Anal At Spectrom. 2017;32(3):647–56. Scholar
  7. 7.
    Rehkämper M, Halliday AN. Development and application of new ion-exchange techniques for the separation of the platinum group and other siderophile elements from geological samples. Talanta. 1997;44(4):663–72. Scholar
  8. 8.
    Song K, Cha H, Lee J, Choi JS, Lee YI, Choi K. Extraction of palladium metal from aqueous solution of palladium chloride by laser-induced photochemistry. Microchem J. 2001;68(2–3):121–6. Scholar
  9. 9.
    Saeki M, Taguchi T, Nakashima N, Ohba H. Wet separation between palladium(II) and molybdenum(IV) ions by using laser-induced particle formation: enhancement of recovery efficiency of palladium by laser condition. J Photochem Photobiol A. 2015;299:189–93. Scholar
  10. 10.
    Saeki M, Esaka F, Taguchi T, Ohba H. Study on separation of platinum-group metals by using laser-induced particle formation. JAEA-Research 2012-030, 2012/11.Google Scholar
  11. 11.
    Yomogida T, Esaka F, Saeki M, Taguchi T, Asai S, Kitatsuji Y, Hanzawa Y. Non-contact Pd separation based on laser-induced particle formation for determination of Pd with ICP-MS. 2016 Pittcon, Atlanta, GA, March 6–10, 2016.Google Scholar
  12. 12.
    Asai S, Yomogida T, Saeki M, Ohba H, Hanzawa Y, Horita T, et al. Determination of 107Pd in Pd recovered by laser-induced photoreduction with inductively coupled plasma mass spectrometry. Anal Chem. 2016;88(24):12227–33. Scholar
  13. 13.
    Russo RE, Mao X, Gonzalez JJ, Zorba V, Yoo J. Laser ablation in analytical chemistry. Anal Chem. 2013;85(13):6162–77. Scholar
  14. 14.
    Poitrasson F, Abzac FX. Femtosecond laser ablation inductively coupled plasma source mass spectrometry for elemental and isotopic analysis: are ultrafast lasers worthwhile? J Anal At Spectrom. 2017;32(6):1075–91. Scholar
  15. 15.
    Jackson SE, Günther D. The nature and sources of laser induced isotopic fractionation in laser ablation-multicollector-inductively coupled plasma-mass spectrometry. J Anal At Spectrom. 2003;18(3):205–12. Scholar
  16. 16.
    Asai S, Hanzawa Y, Okumura K, Shinohara N, Hotoku S, Kaneko S, et al. Determination of Se-79 and Cs-135 in spent nuclear fuel for inventory estimation of high-level radioactive wastes. J Nucl Sci Technol. 2011;48(5):851–4. Scholar
  17. 17.
    Asai S, Toshimitsu M, Hanzawa Y, Suzuki H, Shinohara N, Inagawa J, et al. Isotope dilution inductively coupled plasma mass spectrometry for determination of Sn-126 content in spent nuclear fuel sample. J Nucl Sci Technol. 2013;50(6):556–62. Scholar
  18. 18.
    Asai S, Hanzawa Y, Konda M, Suzuki D, Magara M, Kimura T, et al. Preparation of microvolume anion-exchange cartridge for inductively coupled plasma mass spectrometry-based determination of Np-237 content in spent nuclear fuel. Anal Chem. 2016;88(6):3149–55. Scholar
  19. 19.
    Asai S, Hanzawa Y, Konda M, Suzuki D, Magara M, Kimura T, et al. Rapid separation of zirconium using microvolume anion-exchange cartridge for 93Zr determination with isotope dilution ICP-MS. Talanta. 2018;185(1):98–106. Scholar
  20. 20.
    Asai S, Magara M, Shinohara N, Yamada S, Nagai M, Miyoshi K, et al. Separation of U and Pu in spent nuclear fuel sample using anion-exchange-group-introduced porous polymer sheet for ICP-MS determination. Talanta. 2008;77(2):695700. Scholar
  21. 21.
    Meija J, Coplen TB, Berglund M, Brand WA, Bièvre PD, Gröning M, et al. Isotopic compositions of the elements 2013 (IUPAC Technical Report). Pure Appl Chem. 2016;88(3):293–306. Scholar
  22. 22.
    Košler J, Pedersen RB, Kruber C, Sylvester PJ. Analysis of Fe isotopes in sulfides and iron meteorites by laser ablation high-mass resolution multi-collector ICP mass spectrometry. J Anal At Spectrom. 2005;20(3):192–9. Scholar
  23. 23.
    Graham S, Pearson N, Jackson S, Griffin W, O'Reilly SY. Tracing Cu and Fe from source to porphyry: in situ determination of Cu and Fe isotope ratios in sulfides from the Grasberg Cu–Au deposit. Chem Geol. 2004;207(3_4):147–69. Scholar

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2018

Authors and Affiliations

  1. 1.Nuclear Science and Engineering CenterJapan Atomic Energy Agency (JAEA)Naka-gunJapan
  2. 2.National Metrology Institute of Japan (NMIJ)National Institute of Advanced Industrial Science and Technology (AIST)TsukubaJapan
  3. 3.Quantum Beam Science Research DirectorateNational Institutes for Quantum and Radiological Science and Technology (QST)ChibaJapan

Personalised recommendations