Skip to main content
SpringerLink
Log in

Denitration of simulated high-level liquid waste by formic acid for the connection of PUREX process with TRPO process

  • Published:
Journal of Radioanalytical and Nuclear Chemistry Aims and scope Submit manuscript

Abstract

Denitration of simulated high level liquid waste (HLLW) by formic acid was performed for the connection of Plutonium Uranium Recovery by EXtraction (PUREX) process with trialkyl phosphine oxide (TRPO) process. The concentration of acid, anions and metal ions in solution were monitored under different mole ratios of formic acid to nitric acid and denitration time. Precipitates formed were characterized by Scanning electron microscope, energy dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy and X-ray absorption near edge structure. This work presents a promising strategy for the connection of PUREX process with TRPO process and also provides some new information on the precipitation behavior in denitration of HLLW.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8
Fig. 9

Similar content being viewed by others

References

  1. Salvatores M, Palmiotti G (2011) Radioactive waste partitioning and transmutation within advanced fuel cycles: achievements and challenges. Prog Part Nucl Phys 66:144–166

    Article  CAS  Google Scholar 

  2. Jiao RZ, Wang SZ, Fan SG, Liu BR, Zhu YJ, Zheng HL, Zhou SL, Chen SM (1985) Trialkyl (C6–C8) phosphine oxide for the extraction of actinides and lanthanides from high active waste. J Nucl Radiochem 7(66–71):77

    Google Scholar 

  3. Wang JC, Song CL (2001) Hot test of trialkyl phosphine oxide (TRPO) for removing actinides from highly saline high-level liquid waste (HLLW). Solvent Extr Ion Exch 19:231–242

    Article  Google Scholar 

  4. Chen J, Wang JC (2011) Overview of 30 years research on TRPO process for actinides partitioning from high level liquid waste. Prog Chem 23:1366–1371

    CAS  Google Scholar 

  5. Bush RP, Mills AI, Stearn MI (1995) Comparison of the plant requirements, process performance and waste arisings for potential processes for the partitioning of high level waste. Global 1995

  6. Nakamura H, Yamaguchi I, Kubota M (1978) Effect of platinum group elements on denitration of high-level liquid waste with formic-acid. J Nucl Sci Technol 15:760–764

    Article  CAS  Google Scholar 

  7. Kubota M, Yamaguchi I, Nakamura H (1979) Eeffects of nitrite on denitration of nuclear-fuel reprocessing waste with organic reductants. J Nucl Sci Technol 16:426–433

    Article  CAS  Google Scholar 

  8. Kondo Y, Matsumura M, Kubota M (1994) Solid formation behavior during the conditioning of simulated high level liquid waste for transuranic elements extraction. J Radioanal Nucl Chem 177:311–320

    Article  CAS  Google Scholar 

  9. Kondo Y, Matsumura M, Kubota M (1994) Solid formation in simulated high level liquid waste of relatively low nitric acid concentration. J Radioanal Nucl Chem 177:301–309

    Article  CAS  Google Scholar 

  10. Kondo Y, Kubota M (1997) Formation and filtration characteristics of solids generated in a high level liquid waste treatment process. 1. Solids formation behavior from simulated high level liquid waste. J Radioanal Nucl Chem 221:45–52

    Article  CAS  Google Scholar 

  11. Kondo Y, Kubota M (1997) Formation and filtration characteristics of solids generated in a high level liquid waste treatment process. 2. Filtration characteristics of solids formed in simulated high level liquid waste. J Radioanal Nucl Chem 221:53–61

    Article  CAS  Google Scholar 

  12. Kondo Y (1999) Development of a safety denitration method to remove nitric acid from mixtures. J Radioanal Nucl Chem 240:123–136

    Article  CAS  Google Scholar 

  13. Kondo Y (1999) Influence of urea on initiation and termination of reaction between nitric acid and formic acid. J Radioanal Nucl Chem 242:515–526

    Article  CAS  Google Scholar 

  14. Kondo Y (1999) Removal of nitric acid from a simulated high level liquid waste by a safe chemical denitration. J Radioanal Nucl Chem 242:505–513

    Article  CAS  Google Scholar 

  15. Hwang DS, Lee EH, Kim KW, Lee KI, Park JH, Yoo JH, Park SJ (1999) Denitration of simulated high-level liquid waste by formic acid. J Ind Eng Chem 5:45–51

    CAS  Google Scholar 

  16. Mishra S, Lawrence F, Sreenivasan R, Pandey NK, Mallika C, Koganti SB, Mudali UK (2010) Development of a continuous homogeneous process for denitration by treatment with formaldehyde. J Radioanal Nucl Chem 285:687–695

    Article  CAS  Google Scholar 

  17. Liu X, Chen J, Zhang Y, Wang J (2012) Precipitation of zirconium and molybdenum in simulated high-level liquid waste concentration and denitration process. Atalante 2012 International Conference on Nuclear Chemistry for Sustainable Fuel Cycles, 7: 575–580

  18. Lloyd MH (1976) Instabilities and solids formation in LWR reprocessing solutions. Trans Am Nucl Soc 24:233–234

    Google Scholar 

  19. Kubota M, Fukase T (1980) Formation of precipitate in high-level liquid waste from nuclear-fuel reprocessing. J Nucl Sci Technol 17:783–790

    Article  CAS  Google Scholar 

  20. Gonda K, Oka K, Nemoto T (1982) Characteristics and behavior of emulsion at nuclear-fuel reprocessing. Nucl Technol 57:192–202

    Article  CAS  Google Scholar 

  21. Rao BSM, Gantner E, Muller HG, Reinhardt J, Steinert D, Ache HJ (1986) Solids formation from synthetic fuel-reprocessing solutions-characterization of zirconium molybdate by ICP, XRF, and Raman microprobe spectroscopy. Appl Spectrosc 40:330–336

    Article  CAS  Google Scholar 

  22. Izumida T, Kawamura F (1990) Precipitates formation behavior in simulated high-level liquid waste of fuel-reprocessing. J Nucl Sci Technol 27:267–274

    Article  CAS  Google Scholar 

  23. Rao BSM, Gantner E, Reinhardt J, Steinert D, Ache HJ (1990) Characterization of the solids formed from simulated nuclear-fuel reprocessing solutions. J Nucl Mater 170:39–49

    Article  CAS  Google Scholar 

  24. Paul N, Hammond RB, Hunter TN, Edmondson M, Maxwell L, Biggs S (2015) Synthesis of nuclear waste simulants by reaction precipitation: formation of caesium phosphomolybdate, zirconium molybdate and morphology modification with citratomolybdate complex. Polyhedron 89:129–141

    Article  CAS  Google Scholar 

  25. Doucet FJ, Goddard DT, Taylor CM, Denniss IS, Hutchison SM, Bryan ND (2002) The formation of hydrated zirconium molybdate in simulated spent nuclear fuel reprocessing solutions. Phys Chem Chem Phys 4:3491–3499

    Article  CAS  Google Scholar 

  26. Magnaldo A, Masson M, Champion R (2007) Nucleation and crystal growth of zirconium molybdate hydrate in nitric acid. Chem Eng Sci 62:766–774

    Article  CAS  Google Scholar 

  27. Zhang L, Takeuchi M, Koizumi T, Hirasawa I (2013) Evaluation of precipitation behavior of zirconium molybdate hydrate. Front Chem Sci Eng 7:65–71

    Article  CAS  Google Scholar 

  28. International Atomic Energy Agency (Vienna), Design and operation of high level waste vitrification and storage facilities, Technical Reports Series No. 339 (IAEA, Vienna, 1992)

  29. Healy TV (1958) The reaction of nitric acid with formaldehyde and with formic acid and its application to the removal of nitric acid from mixtures. J Chem Technol Biotechnol 8:553–561

    CAS  Google Scholar 

  30. Ravel B, Newville M (2005) Athena, Artemis, Hephaestus: data analysis for X-ray absorption spectroscopy using IFEFFIT. J Synchrot Radiat 12:537–541

    Article  CAS  Google Scholar 

  31. Orebaugh (1976) Denitration of Savannah River Plant waste streams

  32. Biesinger MC, Lau LWM, Gerson AR, Smart RSC (2010) Resolving surface chemical states in XPS analysis of first row transition metals, oxides and hydroxides: Sc, Ti, V, Cu and Zn. Appl Surf Sci 257:887–898

    Article  CAS  Google Scholar 

  33. Biesinger MC, Payne BP, Grosvenor AP, Lau LWM, Gerson AR, Smart RSC (2011) Resolving surface chemical states in XPS analysis of first row transition metals, oxides and hydroxides: Cr, Mn, Fe, Co and Ni. Appl Surf Sci 257:2717–2730

    Article  CAS  Google Scholar 

  34. Rehr JJ, Ankudinov AL (2005) Progress in the theory and interpretation of XANES. Coordin Chem Rev 249:131–140

    Article  CAS  Google Scholar 

  35. Henderson GS, De Groot FM, Moulton BJ (2014) X-ray absorption near-edge structure (XANES) spectroscopy. Rev Mineral Geochem 78(1):75–138

    Article  CAS  Google Scholar 

  36. Wong J, Lytle FW, Messmer RP, Maylotte DH (1984) K-edge absorption-spectra of selected vanadium compounds. Phys Rev B 30:5596–5610

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This study was supported by National Natural Science Foundation of China (21401115, 51425403), and Program for Changjiang Scholars and Innovative Research Team in University (IRT13026).

Author information

Authors and Affiliations

  1. Collaborative Innovation Center of Advanced Nuclear Energy Technology, Institute of Nuclear and New Energy Technology (INET), Tsinghua University, Beijing, 100084, China

    Wenbing Li, Wuhua Duan, Taoxiang Sun, Jianchen Wang & Jing Chen

  2. Faculty of Chemical Science and Engineering, China University of Petroleum, Beijing, 102249, China

    Wenbing Li & Changjian Liu

Authors
  1. Wenbing Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Wuhua Duan
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Taoxiang Sun
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Changjian Liu
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Jianchen Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Jing Chen
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Taoxiang Sun.

Electronic supplementary material

Below is the link to the electronic supplementary material.

Supplementary material 1 (DOCX 1193 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Li, W., Duan, W., Sun, T. et al. Denitration of simulated high-level liquid waste by formic acid for the connection of PUREX process with TRPO process. J Radioanal Nucl Chem 314, 221–229 (2017). https://doi.org/10.1007/s10967-017-5357-0

Download citation

  • Received:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10967-017-5357-0

Keywords

Search

Navigation