Kinetics of reaction of oxygen with uranium(IV) chloride in alkali chloride melts

V. A. Volkovich; A. B. Ivanov; A. A. Ryzhov; D. S. Maltsev; T. R. Griffiths

doi:10.1149/09810.0365ecst

Kinetics of reaction of oxygen with uranium(IV) chloride in alkali chloride melts

V. A. Volkovich, A. B. Ivanov, A. A. Ryzhov, D. S. Maltsev, T. R. Griffiths

Research output: Chapter in Book/Report/Conference proceeding › Conference contribution › peer-review

2 Scopus citations

Abstract

The reaction of oxygen with solutions of uranium tetrachloride in molten alkali chlorides was studied. The experiments were performed in LiCl-KCl, NaCl-KCl-CsCl, and NaCl-CsCl eutectic based melts at 450-750 ^oC. Pure oxygen and argon-oxygen mixtures (containing ca. 1 and 10 % O₂) were used. Amount of oxygen passed through the melt varied from less than one to over 100 moles per mole of uranium present. In addition the reaction of oxygen with the melts containing a mixture of uranium(IV) and neodymium chlorides was investigated. The course of the reactions was followed by in situ electronic absorption spectroscopy measurements with the spectra recorded at the certain time intervals. Depending on temperature, cationic melt composition and oxygen-to-uranium molar ratio, the reaction resulted in oxidation of uranium(IV) to soluble uranyl chloride and/or precipitation of uranium oxide. Analysis of the spectra provided the information on kinetics of U(IV) concentration change and the reaction rates were determined. Increasing temperature, O₂: U(IV) molar ratio or decreasing mean radius of alkali cations of the solvent melt resulted in faster decrease of U(IV) concentration in the melt.

Original language	English
Title of host publication	PRiME 2020
Subtitle of host publication	Molten Salts and Ionic Liquids 22
Editors	D. P. Durkin, P. C. Trulove, A. Bund, A. Ispas, V. Di Noto, W. M. Reichert, R. A. Mantz, H. C. De Long, M. Mizuhata, M. Ueda
Publisher	IOP Publishing Ltd
Pages	365-372
Number of pages	8
Edition	10
ISBN (Electronic)	9781607689058
DOIs	https://doi.org/10.1149/09810.0365ecst
State	Published - 2020
Externally published	Yes
Event	Pacific Rim Meeting on Electrochemical and Solid State Science 2020, PRiME 200 - Honolulu, United States Duration: Oct 4 2020 → Oct 9 2020

Publication series

Name	ECS Transactions
Number	10
Volume	98
ISSN (Print)	1938-6737
ISSN (Electronic)	1938-5862

Conference

Conference	Pacific Rim Meeting on Electrochemical and Solid State Science 2020, PRiME 200
Country/Territory	United States
City	Honolulu
Period	10/4/20 → 10/9/20

Access to Document

10.1149/09810.0365ecst

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Volkovich, V. A., Ivanov, A. B., Ryzhov, A. A., Maltsev, D. S., & Griffiths, T. R. (2020). Kinetics of reaction of oxygen with uranium(IV) chloride in alkali chloride melts. In D. P. Durkin, P. C. Trulove, A. Bund, A. Ispas, V. Di Noto, W. M. Reichert, R. A. Mantz, H. C. De Long, M. Mizuhata, & M. Ueda (Eds.), PRiME 2020: Molten Salts and Ionic Liquids 22 (10 ed., pp. 365-372). (ECS Transactions; Vol. 98, No. 10). IOP Publishing Ltd. https://doi.org/10.1149/09810.0365ecst

Volkovich, V. A. ; Ivanov, A. B. ; Ryzhov, A. A. et al. / Kinetics of reaction of oxygen with uranium(IV) chloride in alkali chloride melts. PRiME 2020: Molten Salts and Ionic Liquids 22. editor / D. P. Durkin ; P. C. Trulove ; A. Bund ; A. Ispas ; V. Di Noto ; W. M. Reichert ; R. A. Mantz ; H. C. De Long ; M. Mizuhata ; M. Ueda. 10. ed. IOP Publishing Ltd, 2020. pp. 365-372 (ECS Transactions; 10).

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title = "Kinetics of reaction of oxygen with uranium(IV) chloride in alkali chloride melts",

abstract = "The reaction of oxygen with solutions of uranium tetrachloride in molten alkali chlorides was studied. The experiments were performed in LiCl-KCl, NaCl-KCl-CsCl, and NaCl-CsCl eutectic based melts at 450-750 oC. Pure oxygen and argon-oxygen mixtures (containing ca. 1 and 10 % O2) were used. Amount of oxygen passed through the melt varied from less than one to over 100 moles per mole of uranium present. In addition the reaction of oxygen with the melts containing a mixture of uranium(IV) and neodymium chlorides was investigated. The course of the reactions was followed by in situ electronic absorption spectroscopy measurements with the spectra recorded at the certain time intervals. Depending on temperature, cationic melt composition and oxygen-to-uranium molar ratio, the reaction resulted in oxidation of uranium(IV) to soluble uranyl chloride and/or precipitation of uranium oxide. Analysis of the spectra provided the information on kinetics of U(IV) concentration change and the reaction rates were determined. Increasing temperature, O2: U(IV) molar ratio or decreasing mean radius of alkali cations of the solvent melt resulted in faster decrease of U(IV) concentration in the melt.",

author = "Volkovich, {V. A.} and Ivanov, {A. B.} and Ryzhov, {A. A.} and Maltsev, {D. S.} and Griffiths, {T. R.}",

note = "Publisher Copyright: {\textcopyright} The Electrochemical Society; Pacific Rim Meeting on Electrochemical and Solid State Science 2020, PRiME 200 ; Conference date: 04-10-2020 Through 09-10-2020",

year = "2020",

doi = "10.1149/09810.0365ecst",

language = "English",

series = "ECS Transactions",

publisher = "IOP Publishing Ltd",

number = "10",

pages = "365--372",

editor = "Durkin, {D. P.} and Trulove, {P. C.} and A. Bund and A. Ispas and {Di Noto}, V. and Reichert, {W. M.} and Mantz, {R. A.} and {De Long}, {H. C.} and M. Mizuhata and M. Ueda",

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Volkovich, VA, Ivanov, AB, Ryzhov, AA, Maltsev, DS & Griffiths, TR 2020, Kinetics of reaction of oxygen with uranium(IV) chloride in alkali chloride melts. in DP Durkin, PC Trulove, A Bund, A Ispas, V Di Noto, WM Reichert, RA Mantz, HC De Long, M Mizuhata & M Ueda (eds), PRiME 2020: Molten Salts and Ionic Liquids 22. 10 edn, ECS Transactions, no. 10, vol. 98, IOP Publishing Ltd, pp. 365-372, Pacific Rim Meeting on Electrochemical and Solid State Science 2020, PRiME 200, Honolulu, United States, 10/4/20. https://doi.org/10.1149/09810.0365ecst

Kinetics of reaction of oxygen with uranium(IV) chloride in alkali chloride melts. / Volkovich, V. A.; Ivanov, A. B.; Ryzhov, A. A. et al.
PRiME 2020: Molten Salts and Ionic Liquids 22. ed. / D. P. Durkin; P. C. Trulove; A. Bund; A. Ispas; V. Di Noto; W. M. Reichert; R. A. Mantz; H. C. De Long; M. Mizuhata; M. Ueda. 10. ed. IOP Publishing Ltd, 2020. p. 365-372 (ECS Transactions; Vol. 98, No. 10).

Research output: Chapter in Book/Report/Conference proceeding › Conference contribution › peer-review

TY - GEN

T1 - Kinetics of reaction of oxygen with uranium(IV) chloride in alkali chloride melts

AU - Volkovich, V. A.

AU - Ivanov, A. B.

AU - Ryzhov, A. A.

AU - Maltsev, D. S.

AU - Griffiths, T. R.

N1 - Publisher Copyright: © The Electrochemical Society

PY - 2020

Y1 - 2020

N2 - The reaction of oxygen with solutions of uranium tetrachloride in molten alkali chlorides was studied. The experiments were performed in LiCl-KCl, NaCl-KCl-CsCl, and NaCl-CsCl eutectic based melts at 450-750 oC. Pure oxygen and argon-oxygen mixtures (containing ca. 1 and 10 % O2) were used. Amount of oxygen passed through the melt varied from less than one to over 100 moles per mole of uranium present. In addition the reaction of oxygen with the melts containing a mixture of uranium(IV) and neodymium chlorides was investigated. The course of the reactions was followed by in situ electronic absorption spectroscopy measurements with the spectra recorded at the certain time intervals. Depending on temperature, cationic melt composition and oxygen-to-uranium molar ratio, the reaction resulted in oxidation of uranium(IV) to soluble uranyl chloride and/or precipitation of uranium oxide. Analysis of the spectra provided the information on kinetics of U(IV) concentration change and the reaction rates were determined. Increasing temperature, O2: U(IV) molar ratio or decreasing mean radius of alkali cations of the solvent melt resulted in faster decrease of U(IV) concentration in the melt.

AB - The reaction of oxygen with solutions of uranium tetrachloride in molten alkali chlorides was studied. The experiments were performed in LiCl-KCl, NaCl-KCl-CsCl, and NaCl-CsCl eutectic based melts at 450-750 oC. Pure oxygen and argon-oxygen mixtures (containing ca. 1 and 10 % O2) were used. Amount of oxygen passed through the melt varied from less than one to over 100 moles per mole of uranium present. In addition the reaction of oxygen with the melts containing a mixture of uranium(IV) and neodymium chlorides was investigated. The course of the reactions was followed by in situ electronic absorption spectroscopy measurements with the spectra recorded at the certain time intervals. Depending on temperature, cationic melt composition and oxygen-to-uranium molar ratio, the reaction resulted in oxidation of uranium(IV) to soluble uranyl chloride and/or precipitation of uranium oxide. Analysis of the spectra provided the information on kinetics of U(IV) concentration change and the reaction rates were determined. Increasing temperature, O2: U(IV) molar ratio or decreasing mean radius of alkali cations of the solvent melt resulted in faster decrease of U(IV) concentration in the melt.

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M3 - Conference contribution

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EP - 372

BT - PRiME 2020

A2 - Durkin, D. P.

A2 - Trulove, P. C.

A2 - Bund, A.

A2 - Ispas, A.

A2 - Di Noto, V.

A2 - Reichert, W. M.

A2 - Mantz, R. A.

A2 - De Long, H. C.

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PB - IOP Publishing Ltd

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Volkovich VA, Ivanov AB, Ryzhov AA, Maltsev DS, Griffiths TR. Kinetics of reaction of oxygen with uranium(IV) chloride in alkali chloride melts. In Durkin DP, Trulove PC, Bund A, Ispas A, Di Noto V, Reichert WM, Mantz RA, De Long HC, Mizuhata M, Ueda M, editors, PRiME 2020: Molten Salts and Ionic Liquids 22. 10 ed. IOP Publishing Ltd. 2020. p. 365-372. (ECS Transactions; 10). doi: 10.1149/09810.0365ecst

Kinetics of reaction of oxygen with uranium(IV) chloride in alkali chloride melts

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