Abstract
It was confirmed that the pH of NaOH solution (pH 12) could be lowered to pH 6 or less, where I2 was chemically stable, by radiolysis products of air and water. It was also confirmed that acetic acid (CH3COOH) or formic acid (HCOOH) can act as a source material for CH3I formation if these organic acids and I− have specific concentration ratios and the solution pH is maintained within a specific range under gamma irradiation conditions. In the case of CH3COOH mixed solutions, a high concentration of CH3I was formed at a pH lower than the pKa (= 4.76), where the radiolysis rate of CH3COOH was relatively low. In the case of HCOOH mixed solutions, the formation of CH3I was confirmed under the conditions of satisfying a pH of 3 or more, where radiolysis of HCOOH is inhibited, and a pH of 6 or less, where I2 is stably present.
Similar content being viewed by others
References
Paquette J, Torgerson DF, Wren JC, Wren DJ (1985) Volatility of fission products during reactor accidents. J Nucl Mater 130:129–138
Ishigure K, Shiraishi H, Okuda H, Fujita N (1986) Effect of radiation on chemical forms of iodine species in relation to nuclear reactor accidents. Radiat Phys Chem 28:601–610
Lucas M (1988) Radiolysis of cesium iodide solutions in conditions prevailing in a pressurized water reactor severe accident. Nucl Technol 82:157–161
Evans GJ, Kupferschmidt WCH, Portman R, Palson A, Sanipelli GG (1994) Radiochemical analysis of iodine behaviour in the radioiodine test facility. J Radioanal Nucl Chem 180:225–235
Wren JC, Ball JM, Glowa GA (2000) The chemistry of iodine in containment. Nucl Technol 129:297–325
Taghipour F, Evans GJ (2002) Iodine behavior under conditions relating to nuclear reactor accidents. Nucl Technol 137:181–193
Jung S-H, Yeon J-W, Hong SY, Kang Y, Song K (2015) The oxidation behavior of iodide ion under gamma irradiation conditions. Nucl Sci Eng 181:191–203
Kim M, Kim T, Yeon J-W (2018) Formation of CH3I in a NaI and methyl alkyl ketone solution under gamma irradiation conditions. J Radioanal Nucl Chem 316:1329–1335
Wu G, Tong J, Gao Y, Zhang L, Zhao Y (2018) Uncertainty analysis of containment dose rate for core damage assessment in nuclear power plants. Nucl Eng Technol 50:673–682
Bosland L, Funke F, Girault N, Langrock G (2008) Paris Project: Radiolytic oxidation of molecular iodine in containment during a nuclear reactor severe accident. Part 1. Formation and destruction of air radiolysis products. Experimental results and modeling. Nucl Eng Des. 238:3542–3550
Kim M, Hong SY, Kim T, Jung S-H, Yeon J-W (2020) Change in the pH of NaI and methyl alkyl ketone solutions under gamma irradiation. J Radioanal Nucl Chem 326:121–127
Ashmore CB, Gwyther JR, Sims HE (1996) Some effects of pH on inorganic iodine volatility in containment. Nucl Eng Des 166:347–355
Driver P, Glowa G, Wren JC (2000) Steady-state γ-radiolysis of aqueous methyl ethyl ketone (2-butanone) under postulated nuclear reactor accident conditions. Radiat Phys Chem 57:37–51
Glowa G, Driver P, Wren JC (2000) Irradiation of MEK-II: a detailed kinetic model for the degradation of 2-butanone in aerated aqueous solutions under steady-state γ-radiolysis conditions. Radiat Phys Chem 58:49–68
Beahm EC, Wang YM, Wisbey SJ, Shockley WE (1987) Organic iodide formation during severe accidents in light water nuclear reactors. Nucl Technol 78:34–42
Tietze S, Foreman MRS, Ekberg CH (2013) Formation of organic iodides from containment paint ingredients caused by gamma irradiation. J Nucl Sci Technol 50:689–694
Funke F, Langrock G, Kanzleiter T, Poss G, Fischer K, Kühnel A, Weber G, Allelein H-J (2012) Iodine oxides in large-scale THAI tests. Nucl Eng Des 245:206–222
Bosland L, Dickinson S, Glowa GA, Herranz LE, Kim HC, Powers DA, Salay M, Tietze S (2014) Iodine-paint interactions during nuclear reactor severe accidents. Ann Nucl Energ 74:184–199
Wren JC, Ball JM, Glowa GA (1999) The interaction of iodine with organic material in containment. Nucl Technol 125:337–362
Hong SY, Jung S-H, Yeon J-W (2016) Effect of aluminum metal surface on oxidation of iodide under gamma irradiation conditions. J Radioanal Nucl Chem 308:459–468
Kim M, Kim J, Yeon J-W (2021) Concentration determination of I2 and I− formed by thermal and radiolytic decomposition of NaIO3. J Radioanal Nucl Chem 330:475–480
Kim M, Yeon J-W (2021) Accuracy analysis on concentration determination of molecular iodine in gamma irradiated solutions. J Radioanal Nucl Chem 330:469–473
Kim T, Kim M, Kim D, Jung S-H, Yeon J-W (2018) Concentration determination of volatile molecular iodine and methyl iodide. Bull Korean Chem Soc 39:824–828
Lin CC (1980) Chemical effects of gamma radiation on iodine in aqueous solutions. J Inorg Nucl Chem 42:1101–1107
Bosland L, Colombani J (2020) Review of the potential sources of organic iodides in a NPP containment during a severe accident and remaining uncertainties. Ann Nucl Energy 140:107127
Criquet J, Leitner NKV (2011) Radiolysis of acetic acid aqueous solutions—effect of pH and persulfate addition. Chem Eng J 174:504–509
Buxton GV, Greenstock CL, Helman WP, Ross AB (1988) Critical Review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (⋅OH/⋅O−) in Aqueous Solution. J Phys Chem Ref Data 17:513–886
Hart EJ (1954) γ-ray-induced oxidation of aqueous formic acid-oxygen solutions. Effect of pH. J Am Chem Soc 76:4198–4201
Acknowledgements
This work was supported by the National Research Foundation of Korea (NRF) Grant funded by the Korean government (MSIT) (NRF-2017M2A8A4015281, 2021M2E3A3040092, RS-2022-00144202, RS-2023-00261146).
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Minsik Kim is currently affiliated with Inhalation Toxicity Research Group at Korea Institute of Toxicology.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Kim, M., Yeon, JW. Formation of methyl iodide in sodium iodide solutions in the presence of acetic acid and formic acid under gamma irradiation conditions. J Radioanal Nucl Chem 332, 5225–5231 (2023). https://doi.org/10.1007/s10967-023-09148-0
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10967-023-09148-0