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Title: Laser ablation of silicate glasses doped with transuranic actinides

Abstract

Direct sampling laser ablation plasma mass spectrometry was applied to silica glasses doped with {sup 237}Np, {sup 242}Pu, or {sup 241}Am using an instrument installed in a transuranic glove box. The primary goal was to assess the utility of mass spectrometry of directly ablated ions for facile evaluation of actinide (An) constituents of silicate glass immobilization matrices used for encapsulation of radionuclides. The instrument and general procedures have been described elsewhere. The key finding was that actinides and other easily ionized elements such as Ba and Al (ionization energy {le} 6 eV) produced abundant M{sup +} and/or MO{sup +}, whereas positive ions of elements with relatively large ionization energies, such as Si and B (IE {ge} 8 eV), were essentially absent. Laser ablation mass spectrometry is accordingly well-suited to detecting An and fission products such as {sup 90}Sr and {sup 137}Cs in glasses. Detection limits of <0.1 at.% should be readily achievable, and improvement of the ion collection geometry would enhance detection. This exploratory study demonstrated direct sampling laser ablation mass spectrometry as a viable tool for analyzing glass immobilization matrices. The technique would be of greatest value for detecting and determining spatial variations of actinides and fission products. Themore » use of chemical separation of ablated ions should discriminate isobaric actinides.« less

Authors:
;  [1]
  1. Oak Ridge National Lab., TN (United States)
Publication Date:
OSTI Identifier:
298266
Report Number(s):
CONF-981106-
Journal ID: TANSAO; ISSN 0003-018X; TRN: 99:001898
Resource Type:
Journal Article
Journal Name:
Transactions of the American Nuclear Society
Additional Journal Information:
Journal Volume: 79; Conference: American Nuclear Society winter meeting, Washington, DC (United States), 15-19 Nov 1998; Other Information: PBD: 1998
Country of Publication:
United States
Language:
English
Subject:
05 NUCLEAR FUELS; 40 CHEMISTRY; WASTE FORMS; MASS SPECTROSCOPY; DOPED MATERIALS; NEPTUNIUM 237; PLUTONIUM 242; AMERICIUM 241; GLASS; LASER RADIATION; PERFORMANCE

Citation Formats

Gibson, J K, and Haire, R G. Laser ablation of silicate glasses doped with transuranic actinides. United States: N. p., 1998. Web.
Gibson, J K, & Haire, R G. Laser ablation of silicate glasses doped with transuranic actinides. United States.
Gibson, J K, and Haire, R G. 1998. "Laser ablation of silicate glasses doped with transuranic actinides". United States.
@article{osti_298266,
title = {Laser ablation of silicate glasses doped with transuranic actinides},
author = {Gibson, J K and Haire, R G},
abstractNote = {Direct sampling laser ablation plasma mass spectrometry was applied to silica glasses doped with {sup 237}Np, {sup 242}Pu, or {sup 241}Am using an instrument installed in a transuranic glove box. The primary goal was to assess the utility of mass spectrometry of directly ablated ions for facile evaluation of actinide (An) constituents of silicate glass immobilization matrices used for encapsulation of radionuclides. The instrument and general procedures have been described elsewhere. The key finding was that actinides and other easily ionized elements such as Ba and Al (ionization energy {le} 6 eV) produced abundant M{sup +} and/or MO{sup +}, whereas positive ions of elements with relatively large ionization energies, such as Si and B (IE {ge} 8 eV), were essentially absent. Laser ablation mass spectrometry is accordingly well-suited to detecting An and fission products such as {sup 90}Sr and {sup 137}Cs in glasses. Detection limits of <0.1 at.% should be readily achievable, and improvement of the ion collection geometry would enhance detection. This exploratory study demonstrated direct sampling laser ablation mass spectrometry as a viable tool for analyzing glass immobilization matrices. The technique would be of greatest value for detecting and determining spatial variations of actinides and fission products. The use of chemical separation of ablated ions should discriminate isobaric actinides.},
doi = {},
url = {https://www.osti.gov/biblio/298266}, journal = {Transactions of the American Nuclear Society},
number = ,
volume = 79,
place = {United States},
year = {Thu Dec 31 00:00:00 EST 1998},
month = {Thu Dec 31 00:00:00 EST 1998}
}