Skip to main content

A simple acid digestion using HCl–HNO3−NH4HF2 for rapid SF-ICP-MS determination of 237Np and Pu isotopes in steel and concrete samples


A rapid method was developed to analyze 237Np and Pu isotopes in steel and concrete samples using HCl–HNO3–NH4HF2 digestion, CaF2/LaF3 co-precipitation, AG MP-1 M resin column separation and SF-ICP-MS measurement. Compared to acid digestion using HCl–HNO3–HF, the whole procedure not only avoids the use of toxic HF, but can be completed within 1 day. The decontamination factor of U was estimated to be 1.1 × 106. The limits of detection of 237Np, 239Pu, and 240Pu were 0.25, 0.16, and 0.14 fg g−1, respectively, allowing method users to sufficiently detect low level Pu and Np in steel and concrete samples.

This is a preview of subscription content, access via your institution.

Fig. 1
Fig. 2


  1. 1.

    Chu S, Majumdar A (2012) Opportunities and challenges for a sustainable energy future. Nature 488(7411):294–303

    CAS  Article  Google Scholar 

  2. 2.

    Alam F, Sarkar R, Chowdhury H (2019) Nuclear power plants in emerging economies and human resource development: a review. Energy Procedia 160:3–10

    Article  Google Scholar 

  3. 3.

    Samseth J, Banford A W, Batandjieva-Metcalf B, Cantone MC, Lietava P, Peimani H, Szilagyi A (2012) Closing and decommissioning nuclear power reactors: another look following the Fukushima accident. UNEP Year Book. 35–49.

  4. 4.

    Zhu LC, Hou XL, Qiao JX (2021) Determination of 135Cs concentration and 135Cs/137Cs ratio in waste samples from nuclear decommissioning by chemical separation and ICP-MS/MS. Talanta 221:121637

    CAS  Article  Google Scholar 

  5. 5.

    Weinreich R, Bajo S, Eikenberg J, Atchison F (2004) Determination of uranium and plutonium in shielding concrete. J Radioanal Nucl Chem 261(2):319–325

    CAS  Article  Google Scholar 

  6. 6.

    Thakur P, Mulholland GP (2012) Determination of 237Np in environmental and nuclear samples: a review of the analytical method. Appl Radiat Isot 70(8):1747–1778

    CAS  Article  Google Scholar 

  7. 7.

    De Andrade JC, Cuelbas CJ, Paula Eiras DE, S, (1998) Spectrophotometric determination of Mo(VI) in steel using a homogeneous ternary solvent system after single-phase extraction. Talanta 47(3):719–727

    Article  Google Scholar 

  8. 8.

    Tamba MGDM, Falciani R, López TD, Ceodo AG (1994) One-step microwave digestion procedure for the determination of aluminum in steels and iron ores by inductively coupled plasma atomic emission spectrometry. Analyst 119(9):2081–2085

    Article  Google Scholar 

  9. 9.

    Wang ZT, Yang GS, Zheng J, Cao LG, Yu HJ, Zhu YB, Tagami K, Uchida S (2015) Effect of ashing temperature on accurate determination of plutonium in soil samples. Anal Chem 87(11):5511–5515

    CAS  Article  Google Scholar 

  10. 10.

    Maxwell SL, Culligan B, Hutchison JB, Sudowe R, McAlister DR (2017) Rapid method to determine plutonium isotopes in steel samples. J Radioanal Nucl Chem 314(2):1103–1111

    CAS  Article  Google Scholar 

  11. 11.

    Qiao JX, Hou XL, Roos P, Miró M (2010) Rapid and simultaneous determination of neptunium and plutonium isotopes in environment samples by extraction chromatography using sequential injection analysis and ICP-MS. J Anal At Spectrom 25(11):1769–1779

    CAS  Article  Google Scholar 

  12. 12.

    Huang ZY, Ni YY, Wang H, Zheng J, Yamazaki S, Sakaguchi A, Long XG, Uchida S (2019) Simultaneous determination of ultra-trace level 237Np and Pu isotopes in soil and sediment samples by SF-ICP-MS with a single column chromatographic separation. Microchem J 148:597–604

    CAS  Article  Google Scholar 

  13. 13.

    Yang GS, Zheng J, Kim E, Zhang S, Seno H, Kowatari M, Aono T, Kowatari O (2021) Rapid analysis of 237Np and Pu isotopes in urine by single chromatographic column coupled to SF-ICP-MS or ICP-MS/MS. Anal Chim Acta 1158:338431

    CAS  Article  Google Scholar 

  14. 14.

    Matteson BS, Hanson SK, Miller JL, Oldham WJ Jr (2015) Concurrent determination of 237Np and Pu isotopes using ICP-MS: analysis of NIST environmental matrix standard reference materials 4357, 1646a, and 2702. J Environ Radioact 142:62–67

    CAS  Article  Google Scholar 

  15. 15.

    Chen Q, Dahlgaard H, Nielsen SP, Aarkrog A (2002) 242Pu as tracer for simultaneous determination of 237Np and 239, 240Pu in environment samples. J Radioanal Nucl Chem 253(3):451–458

    CAS  Article  Google Scholar 

  16. 16.

    Qiao JX, Hou XL, Roos P, Miró M (2011) High-throughput sequential injection method for simultaneous determination of plutonium and neptunium in environmental solids using macroporous anion-exchange chromatography, followed by inductively coupled plasma mass spectrometric detection. Anal Chem 83(1):374–381

    CAS  Article  Google Scholar 

  17. 17.

    Wang ZT, Wen W, Quan W, Du L, Wang P, Lin JX, Xie Y, Tan ZY (2018) Rapid determination of Pu isotopes for decommission concrete samples by inductively coupled plasma mass spectrometry. J Radioanal Nucl Chem 316(1):411–417

    CAS  Article  Google Scholar 

  18. 18.

    Maxwell SL, Culligan BK, Kelsey-Wall A, Shaw PJ (2011) Rapid determination method for determination of actinides in emergency concrete and brick samples. Anal Chim Acta 701(1):112–118

    CAS  Article  Google Scholar 

  19. 19.

    O’Hara MJ, Kellogg CM, Parker M, Morrison SS, Corbey JF, Grate JW (2017) Decomposition of diverse solid inorganic matrices with molten ammonium bifluoride salt for constituent elemental analysis. Chem Geol 466:341–351

    Article  Google Scholar 

  20. 20.

    Wang H, Ni Y, Zheng J, Huang Z, Xiao D (2019) Low-temperature fusion using HN4HSO4 and NH4HF2 for rapid determination of Pu in soil and sediment samples. Anal Chim Acta 1050:71–79

    CAS  Article  Google Scholar 

  21. 21.

    Zhang W, Hu ZC, Liu YS, Chen HH, Gao S, Gaschnig RM (2012) Total rock dissolution using ammonium bifluoride (NH4HF2) in screw-top Teflon vials: a new development in open-vessel digestion. Anal Chem 84(24):10686–10693

    CAS  Article  Google Scholar 

  22. 22.

    Zheng J (2015) Evaluation of a new sector-field ICP-MS with Jet Interface for ultra-trace determination of Pu isotopes: from femtogram to attogram levels. J Nucl Radiochem Sci 15(1):7–13

    CAS  Article  Google Scholar 

  23. 23.

    Wang ZT, Zheng J, Ni YY, Men W, Tagami K, Uchida S (2017) High-performance method for determination of Pu isotopes in soil and sediment samples by sector field-inductively coupled plasma mass spectrometry. Anal Chem 89(4):2221–2226

    CAS  Article  Google Scholar 

  24. 24.

    Kim CS, Kim CK, Martin P, Sansone U (2007) Determination of Pu isotope concentrations and isotope ratio by inductively coupled plasma mass spectrometry: a review of analytical methodology. J Anal At Spectrom 22(7):827–841

    CAS  Article  Google Scholar 

  25. 25.

    Haynes WM (2015) CRC Handbook of Chemistry and Physics, 96th edn. CRC Press, Boca Raton, FL

    Google Scholar 

  26. 26.

    Tian ZH, Song LJ, Fang KW, Lin GX, Zhou HL (2019) Corrosion behavior of 304L stainless steel in a B-Li coolant for a nuclear power plant. Mater Tehnol 53(5):643–647

    CAS  Article  Google Scholar 

  27. 27.

    Baddoo NR (2008) Stainless steel in construction: A review of research, applications, challenges and opportunities. J Constr Steel Res 64(11):1199–1206

    Article  Google Scholar 

  28. 28.

    Sun C, Tan Y, He K, Zhang SH, Liang KX, Lu Q (2020) Galvanic corrosion behaviors of A508-III/304L couples in boric acid solution. Int J Electrochem Sci 15:3298–3314

    CAS  Article  Google Scholar 

  29. 29.

    Maxwell SL, Culligan B, Hutchison JB, Utsey RC, Sudowe R, McAlister DR (2017) Rapid method to determine 89/90Sr in steel samples. J Radioanal Nucl Chem 314(1):439–450

    CAS  Article  Google Scholar 

  30. 30.

    Kerry T, Banford AW, Bower W, Thompson OR, Carey T, Mosselmans JFW, Ignatyev K, Sharred CA (2018) Uranium contamination of stainless steel in nuclear processing plants. Ind Eng Chem Res 57(11):3957–3962

    CAS  Article  Google Scholar 

  31. 31.

    Vajda N, Kim CK (2011) Determination of transuranium isotopes (Pu, Np, Am) by radiometric techniques: A review of analytical methodology. Anal Chem 83(12):4688–4719

    CAS  Article  Google Scholar 

  32. 32.

    Epov VN, Benkhedda K, Evans D (2005) Determination of Pu isotopes in vegetation using a new on-line FI-ICP-DRC-MS protocol after microwave digestion. J Anal At Spectrom 20(9):990–992

    CAS  Article  Google Scholar 

  33. 33.

    Huff EA, Bowers DL (1989) The determination of impurities in plutonium metal by anion exchange and ICP/AES. Appl Spectrosc 43(2):223–226

    CAS  Article  Google Scholar 

  34. 34.

    Wang ZT, Lin JX, Li SX, Guo QJ, Huang WN, Dan GP, Tan ZY (2018) Rapid method for accurate determination of actinides (U, Th, Pu and Am) in water samples for emergency response. J Radioanal Nucl Chem 315(1):103–110

    CAS  Article  Google Scholar 

Download references


This study was supported by the JSPS KAKENHI (JP 17K00537 and JP 21H03609), the Grant of Fukushima Prefecture related to research and development in radiological sciences, and ERAN I-21-24. Shuai Zhang thanks the China Scholarship Council for offering a scholarship (201906190116) to support his Ph. D. study

Author information




All authors contributed to the study conception and design. Material preparation, data collection and analysis were performed by [Shuai Zhang], [Guosheng Yang], [Jian Zheng]. The draft of the manuscript was written by [Shuai Zhang] and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.

Corresponding author

Correspondence to Jian Zheng.

Additional information

Publisher's Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Rights and permissions

Reprints and Permissions

About this article

Verify currency and authenticity via CrossMark

Cite this article

Zhang, S., Yang, G., Zheng, J. et al. A simple acid digestion using HCl–HNO3−NH4HF2 for rapid SF-ICP-MS determination of 237Np and Pu isotopes in steel and concrete samples. J Radioanal Nucl Chem 329, 1083–1090 (2021).

Download citation


  • Steel
  • Concrete
  • Plutonium
  • Neptunium