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Removal of entrained organic phase from raffinate in spent fuel reprocessing with graphene-based composites

  • Yiyun Geng
  • Zheng LiEmail author
  • Haogui Zhao
  • Mumei Chen
  • Lan ZhangEmail author
Article
  • 16 Downloads

Abstract

In spent fuel reprocessing, the phase entrainment in the solvent extraction process would result in solvent loss, low efficiency and other adverse effects. As a superhydrophobic material with low density and large specific surface area, graphene aerogel may have potential applications in spent fuel reprocessing for the removal of entrained organic phase from raffinate. In this paper, the phase entrainment in the solvent extraction process was investigated by using centrifugal extractor as the extraction equipment. It was found the operation conditions, such as rotor speed, flow rates and phase ratio, have a significant effect on the phase entrainment. Afterwards, a kind of graphene-based superhydrophobic composite was synthesized and used to treat the entrained organic phase in raffinate by a simple adsorption process. The results showed that the proposed method can quickly reduce the content of the organic phase in raffinate to less than 0.1%, showing potential applications in spent fuel reprocessing.

Keywords

Centrifugal contactor Phase entrainment Spent fuel reprocessing Graphene aerogel 

Notes

Acknowledgements

This work was financially supported by National Natural Science Foundation of China (Nos. 11305244, U1867203) and “Strategic Priority Research Program” of the Chinese Academy of Science (Grant No. XDA02030000).

Compliance with ethical standards

Conflict of interest

No conflict of interest exists in the submission of this manuscript and manuscript is approved by all authors for publication. I would like to declare on behalf of my co-authors that the work described is original research that has not been published previously, and not under consideration for publication elsewhere, in whole or in part. All the authors listed have approved the manuscript that is enclosed.

References

  1. 1.
    Kusaka R, Watanabe M (2018) Mechanism of phase transfer of uranyl ions: a vibrational sum frequency generation spectroscopy study on solvent extraction in nuclear reprocessing. Phys Chem Chem Phys 20(47):29588–29590.  https://doi.org/10.1039/c8cp04558e CrossRefPubMedGoogle Scholar
  2. 2.
    Paiva AP, Malik P (2004) Recent advances on the chemistry of solvent extraction applied to the reprocessing of spent nuclear fuels and radioactive wastes. J Radioanal Nucl Chem 261(2):485–496CrossRefGoogle Scholar
  3. 3.
    Spasic AM, Djokovic NN, Babic MD, Marinko MM, Jovanovic GN (1997) Performance of demulsions: entrainment problems in solvent extraction. Chem Eng Sci 52(5):657–675CrossRefGoogle Scholar
  4. 4.
    Leonard RA, Bernstein GJ, Ziegler AA, Pelto RH (2006) Annular centrifugal contactors for solvent extraction. Sep Sci Technol 15(4):925–943.  https://doi.org/10.1080/01496398008076278 CrossRefGoogle Scholar
  5. 5.
    Wang S, Zhang T, Zhao Q, Liu Y, Wu Q (2013) Experimental study on aqueous phase entrainment in a mixer-settler with double stirring mode. China Pet Process Petrochem Technol 15(2):59–62Google Scholar
  6. 6.
    Mandal K, Kumar S, Vijayakumar V, Mudali UK, Ravisankar A, Natarajan R (2015) Hydrodynamic and mass transfer studies of 125 mm centrifugal extractor with 30% TBP/nitric acid system. Prog Nucl Energy 85:1–10.  https://doi.org/10.1016/j.pnucene.2015.05.005 CrossRefGoogle Scholar
  7. 7.
    Liu X, Li H, Liu Y, Su C, Sand W (2015) Impact of entrained and dissolved organic chemicals associated with copper solvent extraction on Acidithiobacillus ferrooxidans. Hydrometallurgy 157:207–213.  https://doi.org/10.1016/j.hydromet.2015.08.010 CrossRefGoogle Scholar
  8. 8.
    Morgan J, Cashwell W, Doole S, Steeples J (2011) Entrainment reduction at freeport-mcmoran copper & gold morenci operations. Solv Extr Ion Exchange 29(5–6):854–867.  https://doi.org/10.1080/07366299.2011.595642 CrossRefGoogle Scholar
  9. 9.
    Hu H, Zhao Z, Wan W, Gogotsi Y, Qiu J (2013) Ultralight and highly compressible graphene aerogels. Adv Mater 25(15):2219–2223.  https://doi.org/10.1002/adma.201204530 CrossRefPubMedGoogle Scholar
  10. 10.
    Zhang X, Zhang T, Wang Z, Ren Z, Yan S, Duan Y, Zhang J (2019) Ultralight, superelastic and fatigue resistant graphene aerogel templated by graphene oxide liquid crystal stabilized air bubbles. ACS Appl Mater Interfaces 11(1):1303–1310.  https://doi.org/10.1021/acsami.8b18606 CrossRefPubMedGoogle Scholar
  11. 11.
    Chen L, Han Q, Li W, Zhou Z, Fang Z, Xu Z, Wang Z, Qian X (2018) Three-dimensional graphene-based adsorbents in sewage disposal: a review. Environ Sci Pollut Res Int 25(26):25840–25861.  https://doi.org/10.1007/s11356-018-2767-7 CrossRefPubMedGoogle Scholar
  12. 12.
    Chen M, Li Z, Geng Y, Zhao H, He S, Chen A, Li Q, Zhang L (2018) A modular process for the treatment of high level liquid waste (HLLW) using solvent-impregnated graphene aerogel. Hydrometallurgy 179:167–174.  https://doi.org/10.1016/j.hydromet.2018.06.005 CrossRefGoogle Scholar
  13. 13.
    Chen T, Zhang J, Li M, Ge H, Li Y, Duan T, Zhu W (2019) Biomass-derived composite aerogels with novel structure for removal/recovery of uranium from simulated radioactive wastewater. Nanotechnology.  https://doi.org/10.1088/1361-6528/ab3991 CrossRefPubMedGoogle Scholar
  14. 14.
    Zhang Y, Zhang L, Zhang G, Li H (2018) Naturally dried graphene-based nanocomposite aerogels with exceptional elasticity and high electrical conductivity. ACS Appl Mater Interfaces 10(25):21565–21572.  https://doi.org/10.1021/acsami.8b04689 CrossRefPubMedGoogle Scholar
  15. 15.
    Ren R-P, Wang Z, Ren J, Lv Y-K (2018) Highly compressible polyimide/graphene aerogel for efficient oil/water separation. J Mater Sci 54(7):5918–5926.  https://doi.org/10.1007/s10853-018-03238-1 CrossRefGoogle Scholar
  16. 16.
    Zhao D, Yu L, Liu D (2018) Ultralight graphene/carbon nanotubes aerogels with compressibility and oil absorption properties. Mater (Basel) 11(4):641.  https://doi.org/10.3390/ma11040641 CrossRefGoogle Scholar
  17. 17.
    Geng Y, Li J, Li Z, Chen M, Zhao H, Zhang L (2019) Facile preparation of 3D graphene-based/polyvinylidene fluoride composite for organic solvents capture in spent fuel reprocessing. J Porous Mater 26(6):1619–1629.  https://doi.org/10.1007/s10934-019-00760-8 CrossRefGoogle Scholar
  18. 18.
    Sun H, Xu Z, Gao C (2013) Multifunctional, ultra-flyweight, synergistically assembled carbon aerogels. Adv Mater 25(18):2554–2560.  https://doi.org/10.1002/adma.201204576 CrossRefPubMedGoogle Scholar
  19. 19.
    Chen M, Li Z, Geng Y, Zhao H, He S, Li Q, Zhang L (2018) Adsorption behavior of thorium on N, N, N’, N’-tetraoctyldiglycolamide (TODGA) impregnated graphene aerogel. Talanta 181:311–317.  https://doi.org/10.1016/j.talanta.2018.01.020 CrossRefPubMedGoogle Scholar
  20. 20.
    Zhou J, Zhou X, Yu W, Zhang C, He X (1997) Miniature centrifugal contactor for radiochemical separation. J Tsinghua Univ 37:46–49Google Scholar
  21. 21.
    Alcock K, Grimley SS, Healy TV, Kennedy J, Mckay HAC (1956) The extraction of nitrates by tri-n-butyl phosphate (TBP): part 1. - The system TBP + diluent + H2O + HNO3. Trans Faraday Soc 52:39–47CrossRefGoogle Scholar
  22. 22.
    Sovilj M, Lukešová S, Rod V (1985) Extraction of nitric acid by TBP solutions in kerosene. Collect Czech Chem Commun 50(3):738–744CrossRefGoogle Scholar
  23. 23.
    Peng M, Li H, Wu L, Zheng Q, Chen Y, Gu W (2005) Porous poly(vinylidene fluoride) membrane with highly hydrophobic surface. J Appl Polym Sci 98(3):1358–1363.  https://doi.org/10.1002/app.22303 CrossRefGoogle Scholar
  24. 24.
    Ma Q, Cheng H, Fane AG, Wang R, Zhang H (2016) Recent development of advanced materials with special wettability for selective oil/water separation. Small 12(16):2186–2202.  https://doi.org/10.1002/smll.201503685 CrossRefPubMedGoogle Scholar
  25. 25.
    Gillens AR, Powell BA (2012) Rapid quantification of TBP and TBP degradation product ratios by FTIR-ATR. J Radioanal Nucl Chem 296(2):859–868.  https://doi.org/10.1007/s10967-012-2147-6 CrossRefGoogle Scholar
  26. 26.
    Jing X, Ning P, Cao H, Wang J, Sun Z (2018) A review of application of annular centrifugal contactors in aspects of mass transfer and operational security. Hydrometallurgy 177:41–48.  https://doi.org/10.1016/j.hydromet.2018.02.005 CrossRefGoogle Scholar

Copyright information

© Akadémiai Kiadó, Budapest, Hungary 2020

Authors and Affiliations

  1. 1.Shanghai Institute of Applied PhysicsChinese Academy of SciencesShanghaiChina
  2. 2.University of Chinese Academy of SciencesBeijingChina

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