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Title: Chemical speciation of U, Fe, and Pu in melt glass from nuclear weapons testing

Abstract

Nuclear weapons testing generates large volumes of glassy materials that influence the transport of dispersed actinides in the environment and may carry information on the composition of the detonated device. We determine the oxidation state of U and Fe (which is known to buffer the oxidation state of actinide elements and to affect the redox state of groundwater) in samples of melt glass collected from three U.S. nuclear weapons tests. For selected samples, we also determine the coordination geometry of U and Fe, and we report the oxidation state of Pu from one melt glass sample. We find significant variations among the melt glass samples and, in particular, find a clear deviation in one sample from the expected buffering effect of Fe(II)/Fe(III) on the oxidation state of uranium. In the first direct measurement of Pu oxidation state in a nuclear test melt glass, we obtain a result consistent with existing literature that proposes Pu is primarily present as Pu(IV) in post-detonation material. In addition, our measurements imply that highly mobile U(VI) may be produced in significant quantities when melt glass is quenched rapidly following a nuclear detonation, though these products may remain immobile in the vitrified matrices. The observed differencesmore » in chemical state among the three samples show that redox conditions can vary dramatically across different nuclear test conditions. The local soil composition, associated device materials, and the rate of quenching are all likely to affect the final redox state of the glass. The resulting variations in glass chemistry are significant for understanding and interpreting debris chemistry and the later environmental mobility of dispersed material.« less

Authors:
; ; ;  [1]; ;  [2];  [3]
  1. Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States)
  2. Nuclear and Chemical Sciences Division, Lawrence Livermore National Laboratory, Livermore, California 94550 (United States)
  3. Materials Science Division, Lawrence Livermore National Laboratory, Livermore, California 94550 (United States)
Publication Date:
OSTI Identifier:
22596995
Resource Type:
Journal Article
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 119; Journal Issue: 19; Other Information: (c) 2016 Author(s); Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-8979
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; BUFFERS; CHEMICAL STATE; CHEMISTRY; EQUIPMENT; GEOMETRY; GLASS; GROUND WATER; IRON; NUCLEAR EXPLOSIONS; NUCLEAR WEAPONS; OXIDATION; PLUTONIUM; QUENCHING; SOILS; TESTING; URANIUM; VALENCE

Citation Formats

Pacold, J. I., Lukens, W. W., Booth, C. H., Shuh, D. K., Knight, K. B., Eppich, G. R., and Holliday, K. S. Chemical speciation of U, Fe, and Pu in melt glass from nuclear weapons testing. United States: N. p., 2016. Web. doi:10.1063/1.4948942.
Pacold, J. I., Lukens, W. W., Booth, C. H., Shuh, D. K., Knight, K. B., Eppich, G. R., & Holliday, K. S. Chemical speciation of U, Fe, and Pu in melt glass from nuclear weapons testing. United States. doi:10.1063/1.4948942.
Pacold, J. I., Lukens, W. W., Booth, C. H., Shuh, D. K., Knight, K. B., Eppich, G. R., and Holliday, K. S. Sat . "Chemical speciation of U, Fe, and Pu in melt glass from nuclear weapons testing". United States. doi:10.1063/1.4948942.
@article{osti_22596995,
title = {Chemical speciation of U, Fe, and Pu in melt glass from nuclear weapons testing},
author = {Pacold, J. I. and Lukens, W. W. and Booth, C. H. and Shuh, D. K. and Knight, K. B. and Eppich, G. R. and Holliday, K. S.},
abstractNote = {Nuclear weapons testing generates large volumes of glassy materials that influence the transport of dispersed actinides in the environment and may carry information on the composition of the detonated device. We determine the oxidation state of U and Fe (which is known to buffer the oxidation state of actinide elements and to affect the redox state of groundwater) in samples of melt glass collected from three U.S. nuclear weapons tests. For selected samples, we also determine the coordination geometry of U and Fe, and we report the oxidation state of Pu from one melt glass sample. We find significant variations among the melt glass samples and, in particular, find a clear deviation in one sample from the expected buffering effect of Fe(II)/Fe(III) on the oxidation state of uranium. In the first direct measurement of Pu oxidation state in a nuclear test melt glass, we obtain a result consistent with existing literature that proposes Pu is primarily present as Pu(IV) in post-detonation material. In addition, our measurements imply that highly mobile U(VI) may be produced in significant quantities when melt glass is quenched rapidly following a nuclear detonation, though these products may remain immobile in the vitrified matrices. The observed differences in chemical state among the three samples show that redox conditions can vary dramatically across different nuclear test conditions. The local soil composition, associated device materials, and the rate of quenching are all likely to affect the final redox state of the glass. The resulting variations in glass chemistry are significant for understanding and interpreting debris chemistry and the later environmental mobility of dispersed material.},
doi = {10.1063/1.4948942},
journal = {Journal of Applied Physics},
issn = {0021-8979},
number = 19,
volume = 119,
place = {United States},
year = {2016},
month = {5}
}

Works referencing / citing this record:

Development of small particle speciation for nuclear forensics by soft X-ray scanning transmission spectromicroscopy
journal, January 2018

  • Pacold, J. I.; Altman, A. B.; Knight, K. B.
  • The Analyst, Vol. 143, Issue 6
  • DOI: 10.1039/c7an01838j