Uranium-series ages of secondary uranium minerals with applications to the long-term evolution of spent nuclear fuel

Robert Finch; Juhani Suksi; Kari Rasilainen; Rodney Ewing

doi:10.1557/PROC-412-823

Uranium-series ages of secondary uranium minerals with applications to the long-term evolution of spent nuclear fuel

Robert Finch, Juhani Suksi, Kari Rasilainen, Rodney Ewing

Research output: Chapter in Book/Report/Conference proceeding › Conference article in proceedings › Scientific › peer-review

25 Citations (Scopus)

Abstract

Uranium-series activity ratios for U(VI) minerals from the Shinkolobwe mine in southern Zaire indicate that these minerals have not experienced significant preferential loss of uranium since their formation more than 100,000 years ago. The minerals examined include rutherfordine, UO₂CO₃, schoepite, [(UO₂)₈O₂(OH)₁₂]·12H₂O, becquerelite, Ca[(UO₂)₆O₄(OH)₆]·8H₂O, and uranophane, Ca[(UO₂)₂(SiO₃OH)₂]·5H₂O. No correlation between mineral species and mineral age was evident. The oxidative dissolution of primary uraninite (UO_2+x) has maintained ground waters supersaturated with respect to all of the secondary U(VI) minerals, providing an inexhaustible source of dissolved U⁶⁺ for mineral formation and growth. As long as uraninite persists in an oxidizing environment, the assemblage of secondary U(VI) phases is determined by local ground water chemistry (including transitory changes), but not necessarily a unidirectional reaction path towards equilibrium with U(VI) minerals of lower solubility. Thus the Shinkolobwe mine displays a complex assemblage of U(VI) minerals that reflects variations in the availability of dissolved elements besides U. Similarly, for a geologic repository exposed to oxidizing waters, the assemblage of corrosion products that will form during the corrosion of spent UO₂ fuel is likely to be as complex as mineral assemblages found in natural uranium deposits under similar conditions.

Original language	English
Title of host publication	Scientific Basis for Nuclear Waste Management XIX
Editors	William M. Murphy, Dieter A. Knecht
Place of Publication	Pittsburgh
Publisher	Materials Research Society
Pages	823-830
ISBN (Print)	978-1-55899-315-0
DOIs	https://doi.org/10.1557/PROC-412-823
Publication status	Published - 1996
MoE publication type	A4 Article in a conference publication
Event	XIX International Symposium on the Scientific Basis for Nuclear Waste Management - Boston, United States Duration: 27 Nov 1995 → 1 Dec 1995

Publication series

Series	Materials Research Society Symposia Proceedings
Volume	412
ISSN	0272-9172

Conference

Conference	XIX International Symposium on the Scientific Basis for Nuclear Waste Management
Country/Territory	United States
City	Boston
Period	27/11/95 → 1/12/95

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10.1557/PROC-412-823

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Finch, Robert ; Suksi, Juhani ; Rasilainen, Kari et al. / Uranium-series ages of secondary uranium minerals with applications to the long-term evolution of spent nuclear fuel. Scientific Basis for Nuclear Waste Management XIX. editor / William M. Murphy ; Dieter A. Knecht. Pittsburgh : Materials Research Society, 1996. pp. 823-830 (Materials Research Society Symposia Proceedings, Vol. 412).

@inproceedings{4432c5009a3d40aeae4172c1b564c105,

title = "Uranium-series ages of secondary uranium minerals with applications to the long-term evolution of spent nuclear fuel",

abstract = "Uranium-series activity ratios for U(VI) minerals from the Shinkolobwe mine in southern Zaire indicate that these minerals have not experienced significant preferential loss of uranium since their formation more than 100,000 years ago. The minerals examined include rutherfordine, UO2CO3, schoepite, [(UO2)8O2(OH)12]·12H2O, becquerelite, Ca[(UO2)6O4(OH)6]·8H2O, and uranophane, Ca[(UO2)2(SiO3OH)2]·5H2O. No correlation between mineral species and mineral age was evident. The oxidative dissolution of primary uraninite (UO2+x) has maintained ground waters supersaturated with respect to all of the secondary U(VI) minerals, providing an inexhaustible source of dissolved U6+ for mineral formation and growth. As long as uraninite persists in an oxidizing environment, the assemblage of secondary U(VI) phases is determined by local ground water chemistry (including transitory changes), but not necessarily a unidirectional reaction path towards equilibrium with U(VI) minerals of lower solubility. Thus the Shinkolobwe mine displays a complex assemblage of U(VI) minerals that reflects variations in the availability of dissolved elements besides U. Similarly, for a geologic repository exposed to oxidizing waters, the assemblage of corrosion products that will form during the corrosion of spent UO2 fuel is likely to be as complex as mineral assemblages found in natural uranium deposits under similar conditions.",

author = "Robert Finch and Juhani Suksi and Kari Rasilainen and Rodney Ewing",

year = "1996",

doi = "10.1557/PROC-412-823",

language = "English",

isbn = "978-1-55899-315-0",

series = "Materials Research Society Symposia Proceedings",

publisher = "Materials Research Society",

pages = "823--830",

editor = "Murphy, {William M.} and Knecht, {Dieter A.}",

booktitle = "Scientific Basis for Nuclear Waste Management XIX",

address = "United States",

note = "XIX International Symposium on the Scientific Basis for Nuclear Waste Management ; Conference date: 27-11-1995 Through 01-12-1995",

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Finch, R, Suksi, J, Rasilainen, K & Ewing, R 1996, Uranium-series ages of secondary uranium minerals with applications to the long-term evolution of spent nuclear fuel. in WM Murphy & DA Knecht (eds), Scientific Basis for Nuclear Waste Management XIX. Materials Research Society, Pittsburgh, Materials Research Society Symposia Proceedings, vol. 412, pp. 823-830, XIX International Symposium on the Scientific Basis for Nuclear Waste Management, Boston, United States, 27/11/95. https://doi.org/10.1557/PROC-412-823

Uranium-series ages of secondary uranium minerals with applications to the long-term evolution of spent nuclear fuel. / Finch, Robert; Suksi, Juhani; Rasilainen, Kari et al.
Scientific Basis for Nuclear Waste Management XIX. ed. / William M. Murphy; Dieter A. Knecht. Pittsburgh: Materials Research Society, 1996. p. 823-830 (Materials Research Society Symposia Proceedings, Vol. 412).

Research output: Chapter in Book/Report/Conference proceeding › Conference article in proceedings › Scientific › peer-review

TY - GEN

T1 - Uranium-series ages of secondary uranium minerals with applications to the long-term evolution of spent nuclear fuel

AU - Finch, Robert

AU - Suksi, Juhani

AU - Rasilainen, Kari

AU - Ewing, Rodney

PY - 1996

Y1 - 1996

N2 - Uranium-series activity ratios for U(VI) minerals from the Shinkolobwe mine in southern Zaire indicate that these minerals have not experienced significant preferential loss of uranium since their formation more than 100,000 years ago. The minerals examined include rutherfordine, UO2CO3, schoepite, [(UO2)8O2(OH)12]·12H2O, becquerelite, Ca[(UO2)6O4(OH)6]·8H2O, and uranophane, Ca[(UO2)2(SiO3OH)2]·5H2O. No correlation between mineral species and mineral age was evident. The oxidative dissolution of primary uraninite (UO2+x) has maintained ground waters supersaturated with respect to all of the secondary U(VI) minerals, providing an inexhaustible source of dissolved U6+ for mineral formation and growth. As long as uraninite persists in an oxidizing environment, the assemblage of secondary U(VI) phases is determined by local ground water chemistry (including transitory changes), but not necessarily a unidirectional reaction path towards equilibrium with U(VI) minerals of lower solubility. Thus the Shinkolobwe mine displays a complex assemblage of U(VI) minerals that reflects variations in the availability of dissolved elements besides U. Similarly, for a geologic repository exposed to oxidizing waters, the assemblage of corrosion products that will form during the corrosion of spent UO2 fuel is likely to be as complex as mineral assemblages found in natural uranium deposits under similar conditions.

AB - Uranium-series activity ratios for U(VI) minerals from the Shinkolobwe mine in southern Zaire indicate that these minerals have not experienced significant preferential loss of uranium since their formation more than 100,000 years ago. The minerals examined include rutherfordine, UO2CO3, schoepite, [(UO2)8O2(OH)12]·12H2O, becquerelite, Ca[(UO2)6O4(OH)6]·8H2O, and uranophane, Ca[(UO2)2(SiO3OH)2]·5H2O. No correlation between mineral species and mineral age was evident. The oxidative dissolution of primary uraninite (UO2+x) has maintained ground waters supersaturated with respect to all of the secondary U(VI) minerals, providing an inexhaustible source of dissolved U6+ for mineral formation and growth. As long as uraninite persists in an oxidizing environment, the assemblage of secondary U(VI) phases is determined by local ground water chemistry (including transitory changes), but not necessarily a unidirectional reaction path towards equilibrium with U(VI) minerals of lower solubility. Thus the Shinkolobwe mine displays a complex assemblage of U(VI) minerals that reflects variations in the availability of dissolved elements besides U. Similarly, for a geologic repository exposed to oxidizing waters, the assemblage of corrosion products that will form during the corrosion of spent UO2 fuel is likely to be as complex as mineral assemblages found in natural uranium deposits under similar conditions.

U2 - 10.1557/PROC-412-823

DO - 10.1557/PROC-412-823

M3 - Conference article in proceedings

SN - 978-1-55899-315-0

T3 - Materials Research Society Symposia Proceedings

SP - 823

EP - 830

BT - Scientific Basis for Nuclear Waste Management XIX

A2 - Murphy, William M.

A2 - Knecht, Dieter A.

PB - Materials Research Society

CY - Pittsburgh

T2 - XIX International Symposium on the Scientific Basis for Nuclear Waste Management

Y2 - 27 November 1995 through 1 December 1995

ER -

Finch R, Suksi J, Rasilainen K, Ewing R. Uranium-series ages of secondary uranium minerals with applications to the long-term evolution of spent nuclear fuel. In Murphy WM, Knecht DA, editors, Scientific Basis for Nuclear Waste Management XIX. Pittsburgh: Materials Research Society. 1996. p. 823-830. (Materials Research Society Symposia Proceedings, Vol. 412). doi: 10.1557/PROC-412-823

Uranium-series ages of secondary uranium minerals with applications to the long-term evolution of spent nuclear fuel

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