Abstract
The reaction mechanisms and rate constants of N, N-diethylhydroxylamine (DEHA) with ·OH, CO3−·, eaq− and ·H were studied. Results show that ·OH radicals oxidize DEHA by hydrogen abstraction from DEHA’s hydroxyl group to form transient (C2H5)2NO·, which has an absorption maximum at 395 nm. The transient intermediates for the reactions of DEHA with CO3−· and eaq−, as well as protonated DEHA with ·H, show no absorption peak between 300 and 800 nm. The rate constants for the reactions of DEHA with ·OH, CO3−· and eaq−, also protonated DEHA with ·H, were measured.
Similar content being viewed by others
References
Choppin GR, Morgenstern A (2000) Radionuclide separations in radioactive waste disposal. J Radioanal Nucl Chem 243(1):45–51. https://doi.org/10.1023/A:1006754927614
Wang FR, Horne GP, Pernot P et al (2018) Picosecond pulse radiolysis study on the radiation induced reactions in neat tributyl phosphate. J Phys Chem B 122(28):7134–7142. https://doi.org/10.1021/acs.jpcb.8b03715
Natarajan R (2017) Reprocessing of spent nuclear fuel in India: Present challenges and future programme. Prog Nucl Energ 101:118–132. https://doi.org/10.1016/j.pnucene.2017.03.001
Mincher BJ, Mezyk SP, Martin LRA (2008) A pulse radiolysis investigation of the reactions of tributyl phosphate with the radical products of aqueous nitric acid irradiation. J Phys Chem A 112(28):6275–6280. https://doi.org/10.1021/jp802169v
Ochsenfeld W, Petrich G (1983) Neptunium decontamination in a uranium purification cycle of a spent fuel reprocessing plant. Sep Sci Technol 18(14 & 15):1685–1698. https://doi.org/10.1080/01496398308056121
Zhang AY, Liu Y (2000) Hydroxylamine derivative in Purex Process III The kinetics of oxidation-reduction reaction between N, N-diethylhydroxylamine and neptunium (VI). J Radioanal Nucl Chem 245(2):357–361. https://doi.org/10.1023/A:1006726925123
Zhang AY, Hu JX, Zhang XY et al (2002) Hydroxylamine derivative in Purex Process-Part IV. A study on the kinetics of the oxidation-reduction reaction between N, N-diethylhydroxylamine and plutonium (IV). J Radioanal Nucl Chem 252(3):565–571
Zhang AY, Hu JX, Zhang XY et al (2002) Hydroxylamine derivative in the Purex Process - Part V. The single-stage reduction extraction and back extraction of neptunium with N, N-diethylhydroxylamine. J Radioanal Nucl Chem 253(1):107–113
Zhang AY, Hu JX, Zhang XY et al (2001) Hydroxylamine derivative in purex process VI. Study on the partition of uranium/neptunium and uranium/plutonium with N, N-diethylhydroxylamine in the purification cycle of uranium contactor. Solvent Extr Ion Exc 19(6):965–979. https://doi.org/10.1081/SEI-100107613
Sze K, Gosselin JA (1983) Oxidation of Pu (III) by nitric acid in tri-n-butyl phosphate solutions. Part II. Chemical methods for the suppression of oxidation to improve plutonium separation in contactor operation. Nucl Technol 63(3): 431–441. https://doi.org/10.13182/NT83-A33270
Wang JH, Wang CC, Wang ShX et al (2016) γ-rays damage of N, N-Diethyl-hydroxylamine in water and its radiolytic products at lower dose. J Radioanal Nucl Chem 309(2):503–510. https://doi.org/10.1007/s10967-015-4641-0
Wang JH, Wang ShX, Bao BR et al (2008) Gaseous products generated by radiation degradation of N,N-diethylhydroxylamine aqueous solution. Nucl Sci Tech 19(2):79–82. https://doi.org/10.1016/S1001-8042(08)60027-5
Spinks JWT, Woods RJ (1976) An Introduction to Radiation Chemistry, 2nd. ed. A Wiley-Interscience Publication, John Wiley & Sons., New York
Wu JL, Ch QS (1993) Radiation Chemistry. Atomic Energy Publisher, Beijing
Simic M, Hayon E (1971) Intermediates produced from the one-electron oxidation and reduction of hydroxylamines. Acid-base properties of the amino, hydroxyamino, and methoxyamino radicals. J Am Chem Soc 93(23):5982–5986. https://doi.org/10.1021/ja00752a005
Saunders BB, Gorse RA (1979) Reactions of diethylhydroxylamine with radiolytically produced radicals in aqueous solutions. J Phys Chem 83(13):1696–1701. https://doi.org/10.1021/j100476a004
Yao SD, Sheng SG, Cai JH et al (1995) Nanosecond pulse radiolysis studies in China. Radiat Phys Chem 46(1):105–109
Zhang P, Yao SD, Li HX et al (2011) Pulse radiolysis study on several fluoroquinolones. Radiat Phys Chem 80(4):548–553. https://doi.org/10.1016/j.radphyschem.2010.12.003
Adamic K, Bowman DF, Gillan T et al (1971) Kinetic applications of electron paramagnetic resonance spectroscopy I self-reactions of diethyl nitroxide radicals. J Am Chem Soc 93(4):902–908
Forrester AR, Hay JM, Thomson RH (1968) Organlc chemistry of stable free radicals. Academic Press, New York
Wang JH, Wan Y, Wu MH et al (2008) Analyses of organics in irradiated aqueous N,N-diethylhydroxylamine solution. Nucl Sci Tech 19(6):343–346
Wang JH, Zhang J, Wu MH et al (2011) Radiolytic organics in gamma-ray irradiated aqueous solution of N,N-diethylhydroxylamine. Nucl Sci Tech 22(2):95–98
Wu MH, Liu N, Xu G et al (2011) Kinetics and mechanisms studies on dimethyl phthalate degradation in aqueous solutions by pulse radiolysis and electron beam radiolysis. Radiat Phys Chem 80(3): 420–424. https://doi.org/10.1016/j.radphyschem.2010.10.008
Pagsberg PB (1969) Pulse radiolysis of ammonia in aqueous solutions in the presence of nitrous oxide. Radiat Res 39(2):531–532
Land EJ, Ebert M (1967) Pulse radiolysis studies of aqueous phenol. Trans Faraday Soc 63:1181–1190
Acknowledgements
The authors wish to extend warm acknowledgement for the financial assistance of the National Natural Science Foundation of China (No. 20771074).
Author information
Authors and Affiliations
Corresponding author
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
Wang, J.H., Zhao, X.Y., Shi, Y. et al. Nanosecond pulse radiolysis of aqueous N, N-diethylhydroxylamine solution. J Radioanal Nucl Chem 331, 241–247 (2022). https://doi.org/10.1007/s10967-021-08031-0
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10967-021-08031-0