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On-line gas chromatographic studies of chlorides of rutherfordium and homologs Zr and Hf

Abstract

Gas-phase isothermal chromatography is a method by which volatile compounds of different chemical elements can be separated. The technique, coupled with theoretical modeling of the processes occurring in the chromatography column, provides information about thermodynamic properties (e.g., adsorption enthalpies) for compounds of elements, such as the transactinides, which can only be produced on an atom-at-a-time basis. In addition, the chemical selectivity of the isothermal chromatography technique provides the decontamination from interfering activities necessary for determination of the nuclear decay properties of the isotopes of these elements. The Zr and Hf isotopes, 30.7-s {sup 98}Zr and 38-s {sup 162}Hf were produced via the {sup 235}U(n,f) and {sup 147}Sm({sup 20}Ne,5n) reactions, respectively. The 65-s {sup 261}Rf was produced via the {sup 248}Cm({sup 18}O,5n) reaction. A new and more accurate half-life for {sup 261}Rf of 78{sup +11}{sub -6}-s has been measured. Measurements were performed on chloride species of Rf and its group 4 homologs, Zr and Hf and on Zr-bromides using the Heavy Element Volatility Instrument (HEVI). Adsorption enthalpies were calculated for all species using a Monte Carlo code simulation based on a microscopic model for gas thermochromatography in open columns with laminar flow of the carrier gas and the following adsorption enthalpies  More>>
Authors:
Kadkhodayen, B; [1]  Tuerler, A; [2]  Gregorich, K E; [3]  Baisden, P A; [1]  Czerwinski, K R; [3]  Eichler, B; [2]  Gaeggeler, H W; [2]  Hamilton, T M; [3]  Jost, D T; [2]  Kacher, C D; [3]  Kovacs, A; [2]  Kreek, S A; [3]  Lane, M R; [3]  Mohar, M F; [3]  Neu, M P; [3]  Stoyer, N J; [3]  Sylwester, E R; [3]  Lee, D M; [3]  Nurmia, M J; [3]  Seaborg, G T; [3]  Hoffman, D C [3] 
  1. Seaborg (Glenn T.) Inst. for Transactinium Science, Livermore, CA (United States)
  2. Paul Scherrer Inst., Villigen (Switzerland)
  3. Lawrence Berkeley Lab., CA (United States)
Publication Date:
Aug 01, 1996
Product Type:
Journal Article
Reference Number:
SCA: 400702; 400105; PA: DEN-96:0FB440; EDB-96:114106; SN: 96001625709
Resource Relation:
Journal Name: Radiochimica Acta; Journal Volume: 72; Journal Issue: 4; Other Information: PBD: 1996
Subject:
40 CHEMISTRY; ELEMENT 104; GAS CHROMATOGRAPHY; THERMODYNAMIC PROPERTIES; ENTHALPY; HAFNIUM 162; VOLATILITY; MONTE CARLO METHOD; ZIRCONIUM 98; CHLORIDES; TEMPERATURE DEPENDENCE
OSTI ID:
257926
Country of Origin:
Germany
Language:
English
Other Identifying Numbers:
Journal ID: RAACAP; ISSN 0033-8230; TRN: DE96FB440
Submitting Site:
DEN
Size:
pp. 169-178
Announcement Date:
Aug 05, 1996

Citation Formats

Kadkhodayen, B, Tuerler, A, Gregorich, K E, Baisden, P A, Czerwinski, K R, Eichler, B, Gaeggeler, H W, Hamilton, T M, Jost, D T, Kacher, C D, Kovacs, A, Kreek, S A, Lane, M R, Mohar, M F, Neu, M P, Stoyer, N J, Sylwester, E R, Lee, D M, Nurmia, M J, Seaborg, G T, and Hoffman, D C. On-line gas chromatographic studies of chlorides of rutherfordium and homologs Zr and Hf. Germany: N. p., 1996. Web.
Kadkhodayen, B, Tuerler, A, Gregorich, K E, Baisden, P A, Czerwinski, K R, Eichler, B, Gaeggeler, H W, Hamilton, T M, Jost, D T, Kacher, C D, Kovacs, A, Kreek, S A, Lane, M R, Mohar, M F, Neu, M P, Stoyer, N J, Sylwester, E R, Lee, D M, Nurmia, M J, Seaborg, G T, & Hoffman, D C. On-line gas chromatographic studies of chlorides of rutherfordium and homologs Zr and Hf. Germany.
Kadkhodayen, B, Tuerler, A, Gregorich, K E, Baisden, P A, Czerwinski, K R, Eichler, B, Gaeggeler, H W, Hamilton, T M, Jost, D T, Kacher, C D, Kovacs, A, Kreek, S A, Lane, M R, Mohar, M F, Neu, M P, Stoyer, N J, Sylwester, E R, Lee, D M, Nurmia, M J, Seaborg, G T, and Hoffman, D C. 1996. "On-line gas chromatographic studies of chlorides of rutherfordium and homologs Zr and Hf." Germany.
@misc{etde_257926,
title = {On-line gas chromatographic studies of chlorides of rutherfordium and homologs Zr and Hf}
author = {Kadkhodayen, B, Tuerler, A, Gregorich, K E, Baisden, P A, Czerwinski, K R, Eichler, B, Gaeggeler, H W, Hamilton, T M, Jost, D T, Kacher, C D, Kovacs, A, Kreek, S A, Lane, M R, Mohar, M F, Neu, M P, Stoyer, N J, Sylwester, E R, Lee, D M, Nurmia, M J, Seaborg, G T, and Hoffman, D C}
abstractNote = {Gas-phase isothermal chromatography is a method by which volatile compounds of different chemical elements can be separated. The technique, coupled with theoretical modeling of the processes occurring in the chromatography column, provides information about thermodynamic properties (e.g., adsorption enthalpies) for compounds of elements, such as the transactinides, which can only be produced on an atom-at-a-time basis. In addition, the chemical selectivity of the isothermal chromatography technique provides the decontamination from interfering activities necessary for determination of the nuclear decay properties of the isotopes of these elements. The Zr and Hf isotopes, 30.7-s {sup 98}Zr and 38-s {sup 162}Hf were produced via the {sup 235}U(n,f) and {sup 147}Sm({sup 20}Ne,5n) reactions, respectively. The 65-s {sup 261}Rf was produced via the {sup 248}Cm({sup 18}O,5n) reaction. A new and more accurate half-life for {sup 261}Rf of 78{sup +11}{sub -6}-s has been measured. Measurements were performed on chloride species of Rf and its group 4 homologs, Zr and Hf and on Zr-bromides using the Heavy Element Volatility Instrument (HEVI). Adsorption enthalpies were calculated for all species using a Monte Carlo code simulation based on a microscopic model for gas thermochromatography in open columns with laminar flow of the carrier gas and the following adsorption enthalpies for the group 4 chlorides were obtained for quartz surfaces: Zr(-74{+-}5 kJ/mol), Hf(-96{+-}5 kJ/mol) and Rf (-77{+-}6 kJ/mol). These results indicate that Rf deviates from the trend expected based on extrapolation of the Zr and Hf values. Further calculations are needed to assess whether this is due to relativistic effects in the transactinide region. (orig.)}
journal = []
issue = {4}
volume = {72}
journal type = {AC}
place = {Germany}
year = {1996}
month = {Aug}
}