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Theoretical insights into the reduction mechanism of neptunyl nitrate by hydrazine derivatives

  • Zhong-Ping Cheng , Xiao-Bo Li , Qun-Yan Wu EMAIL logo , Zhi-Fang Chai and Wei-Qun Shi EMAIL logo
Published/Copyright: April 21, 2022
Radiochimica Acta
From the journal Radiochimica Acta Volume 110 Issue 6-9

Abstract

In the advanced spent fuel cycle, the control and adjustment of neptunium valence state is greatly important for the highly efficient separation of neptunium. Hydrazine and its derivatives as salt-free reagents can selectively reduce Np(VI) to Np(V), but their reduction mechanisms are still unclear. We explored the reduction of [NpVIO2(H2O)2(NO3)2] by N2H4 and its two derivatives HOC2H4N2H3 and CHON2H3 using scalar relativistic density functional theory. The thermodynamic energy of the reactions [NpVIO2(H2O)2(NO3)2] with three reductants are sensitive to the substitution group, HOC2H4N2H3 enhances thermodynamic ability of the reaction and CHON2H3 shows contrary result. Both HOC2H4N2H3 and CHON2H3 have lower energy barrier compared to N2H4 based on the potential energy profiles (PEPs), which probably attributes to the intramolecular hydrogen bond of hydrazine derivatives. The nature of these redox reactions is that the hydrogen atom of reductants is gradually transferred to the axis oxygen atom of neptunyl, which accompanies the N–H bond dissociation and Oax–H bond formation. The reduction of Np(VI) with HOC2H4N2H3 is the most favorable reaction based on the thermodynamic and kinetic results. This work provides theoretical perspective into the reduction of Np(VI) to Np(V), which is beneficial to the development of more effective free-salt reductants for the separation of neptunium from uranium and plutonium in spent fuel reprocessing.

Keywords: hydrazine derivatives; neptunium; reduction mechanism; scalar relativistic density functional theory; spent fuel reprocessing
Corresponding authors: Qun-Yan Wu and Wei-Qun Shi, Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, China, E-mail: (Q.-Y. Wu), (W.-Q. Shi)

Funding source: National Natural Science Foundation of China

Award Identifier / Grant number: U1867205

Award Identifier / Grant number: 22076188

Award Identifier / Grant number: 11875058

Funding source: National Science Fund for Distinguished Young Scholars

Award Identifier / Grant number: 21925603

  1. Author contributions: All the authors have accepted responsibility for the entire content of this submitted manuscript and approved submission.

  2. Research funding: This work was supported by the National Natural Science Foundation of China (Grants U1867205, 22076188, 11875058), the National Science Fund for Distinguished Young Scholars (21925603).

  3. Conflict of interest statement: The authors declare no conflicts of interest regarding this article.

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Supplementary Material

Electronic supplementary information: Optimized structures, two dimensioned ELF diagrams and Mayer bond orders of the neptunyl nitrate with HOC2H4N2H3 and CHON2H3.

The online version of this article offers supplementary material (https://doi.org/10.1515/ract-2021-1120).

Received: 2021-11-03
Accepted: 2021-11-27
Published Online: 2022-04-21
Published in Print: 2022-06-27

© 2021 Walter de Gruyter GmbH, Berlin/Boston

Articles in the same Issue

  1. Frontmatter
  2. Editorial: Diamond Jubilee Issue
  3. Sixty years of Radiochimica Acta: a brief overview with emphasis on the last 10 years
  4. A. Chemistry of Radioelements
  5. Five decades of GSI superheavy element discoveries and chemical investigation
  6. Chemistry of the elements at the end of the actinide series using their low-energy ion-beams
  7. Sonochemistry of actinides: from ions to nanoparticles and beyond
  8. Theoretical insights into the reduction mechanism of neptunyl nitrate by hydrazine derivatives
  9. The speciation of protactinium since its discovery: a nightmare or a path of resilience
  10. On the volatility of protactinium in chlorinating and brominating gas media
  11. The aqueous chemistry of radium
  12. B. Energy Related Radiochemistry
  13. Selective actinide(III) separation using 2,6-bis[1-(propan-1-ol)-1,2,3-triazol-4-yl]pyridine (PyTri-Diol) in the innovative-SANEX process: laboratory scale counter current centrifugal contactor demonstration
  14. Fate of Neptunium in nuclear fuel cycle streams: state-of-the art on separation strategies
  15. Uranium adsorption – a review of progress from qualitative understanding to advanced model development
  16. Targeted synthesis of carbon-supported titanate nanofibers as host structure for nuclear waste immobilization
  17. Progress of energy-related radiochemistry and radionuclide production in the Republic of Korea
  18. C. Nuclear Data
  19. How accurate are half-life data of long-lived radionuclides?
  20. Status of the decay data for medical radionuclides: existing and potential diagnostic γ emitters, diagnostic β+ emitters and therapeutic radioisotopes
  21. An overview of nuclear data standardisation work for accelerator-based production of medical radionuclides in Pakistan
  22. An overview of activation cross-section measurements of some neutron and charged-particle induced reactions in Bangladesh
  23. Nuclear reaction data for medical and industrial applications: recent contributions by Egyptian cyclotron group
  24. Nuclear data for light charged particle induced production of emerging medical radionuclides
  25. D. Radionuclides and Radiopharmaceuticals
  26. The role of chemistry in accelerator-based production and separation of radionuclides as basis for radiolabelled compounds for medical applications
  27. Production of neutron deficient rare earth radionuclides by heavy ion activation
  28. Evaluation of 186WS2 target material for production of high specific activity 186Re via proton irradiation: separation, radiolabeling and recovery/recycling
  29. Special radionuclide production activities – recent developments at QST and throughout Japan
  30. China’s radiopharmaceuticals on expressway: 2014–2021
  31. E. Environmental Radioactivity
  32. A summary of environmental radioactivity research studies by members of the Japan Society of Nuclear and Radiochemical Sciences
https://doi.org/10.1515/ract-2021-1120
Keywords for this article
hydrazine derivatives; neptunium; reduction mechanism; scalar relativistic density functional theory; spent fuel reprocessing

Articles in the same Issue

  1. Frontmatter
  2. Editorial: Diamond Jubilee Issue
  3. Sixty years of Radiochimica Acta: a brief overview with emphasis on the last 10 years
  4. A. Chemistry of Radioelements
  5. Five decades of GSI superheavy element discoveries and chemical investigation
  6. Chemistry of the elements at the end of the actinide series using their low-energy ion-beams
  7. Sonochemistry of actinides: from ions to nanoparticles and beyond
  8. Theoretical insights into the reduction mechanism of neptunyl nitrate by hydrazine derivatives
  9. The speciation of protactinium since its discovery: a nightmare or a path of resilience
  10. On the volatility of protactinium in chlorinating and brominating gas media
  11. The aqueous chemistry of radium
  12. B. Energy Related Radiochemistry
  13. Selective actinide(III) separation using 2,6-bis[1-(propan-1-ol)-1,2,3-triazol-4-yl]pyridine (PyTri-Diol) in the innovative-SANEX process: laboratory scale counter current centrifugal contactor demonstration
  14. Fate of Neptunium in nuclear fuel cycle streams: state-of-the art on separation strategies
  15. Uranium adsorption – a review of progress from qualitative understanding to advanced model development
  16. Targeted synthesis of carbon-supported titanate nanofibers as host structure for nuclear waste immobilization
  17. Progress of energy-related radiochemistry and radionuclide production in the Republic of Korea
  18. C. Nuclear Data
  19. How accurate are half-life data of long-lived radionuclides?
  20. Status of the decay data for medical radionuclides: existing and potential diagnostic γ emitters, diagnostic β+ emitters and therapeutic radioisotopes
  21. An overview of nuclear data standardisation work for accelerator-based production of medical radionuclides in Pakistan
  22. An overview of activation cross-section measurements of some neutron and charged-particle induced reactions in Bangladesh
  23. Nuclear reaction data for medical and industrial applications: recent contributions by Egyptian cyclotron group
  24. Nuclear data for light charged particle induced production of emerging medical radionuclides
  25. D. Radionuclides and Radiopharmaceuticals
  26. The role of chemistry in accelerator-based production and separation of radionuclides as basis for radiolabelled compounds for medical applications
  27. Production of neutron deficient rare earth radionuclides by heavy ion activation
  28. Evaluation of 186WS2 target material for production of high specific activity 186Re via proton irradiation: separation, radiolabeling and recovery/recycling
  29. Special radionuclide production activities – recent developments at QST and throughout Japan
  30. China’s radiopharmaceuticals on expressway: 2014–2021
  31. E. Environmental Radioactivity
  32. A summary of environmental radioactivity research studies by members of the Japan Society of Nuclear and Radiochemical Sciences
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