Effects of ionizing radiation on the hollandite structure-type: Ba0.85 Cs0.26 Al1.35 Fe0.77 Ti5.90O16

Abdesselam Abdelouas, Satoshi Utsunomiya, Tomo Suzuki, Bernd Grambow, Thierry Advocat, Florence Bart, Rodney C. Ewing

Research output: Contribution to journalArticle

19 Citations (Scopus)

Abstract

The hollandite structure-type has received considerable attention as a nuclear waste form for the incorporation of radioactive 135Cs and 137Cs, both of which are important fission product radionuclides in the high-level nuclear waste generated by the reprocessing of used nuclear fuel. A critical concern has been the effects of high doses of ionizing radiation from incorporated Cs on the long-term structural stability of the hollandite structure. Optimization of the synthesis conditions has resulted in the hollandite stoichiometry of Ba0.85 Cs0.26 Al1.35 Fe0.77 Ti5.90 O16. To evaluate the effect of Cs-beta-decay on this stoichiometry, we have simulated the ionizing radiation using 200 kV electron beam using transmission electron microscopy (TEM) at 298 and 573 K. Complete amorphization was achieved at doses of 1.1 × 1014 and 1.8 × 1014 Gy at temperatures of 298 and 573 K, respectively. Electron energy-loss spectroscopy (EELS) of the Cs M-edge revealed the selective loss of Cs at the maximum doses. Hollandite irradiated using gamma rays, ∼106 Gy, which has defects associated with the formation of Ti3+ and O2- had a dissolution rate similar to that of the pristine hollandite, suggesting that the initial stage of defect formation does not influence chemical durability. Because the accumulated dose in the hollandite with 5 wt% of radioactive 137Cs2O is estimated to be ∼2.0 × 1010 Gy after 500 years, the hollandite structure should be stable under the conditions anticipated for geologic disposal.

Original languageEnglish
Pages (from-to)241-247
Number of pages7
JournalAmerican Mineralogist
Volume93
Issue number1
DOIs
Publication statusPublished - Jan 1 2008

Fingerprint

Radioactive Waste
Ionizing radiation
Stoichiometry
ionizing radiation
Dosimetry
dosage
Defects
Amorphization
Fission products
Electron energy loss spectroscopy
radioactive wastes
Nuclear fuels
stoichiometry
Radioisotopes
Gamma rays
radioactive waste
defect
Electron beams
Dissolution
Durability

All Science Journal Classification (ASJC) codes

  • Geophysics
  • Geochemistry and Petrology

Cite this

Effects of ionizing radiation on the hollandite structure-type : Ba0.85 Cs0.26 Al1.35 Fe0.77 Ti5.90O16. / Abdelouas, Abdesselam; Utsunomiya, Satoshi; Suzuki, Tomo; Grambow, Bernd; Advocat, Thierry; Bart, Florence; Ewing, Rodney C.

In: American Mineralogist, Vol. 93, No. 1, 01.01.2008, p. 241-247.

Research output: Contribution to journalArticle

Abdelouas, Abdesselam ; Utsunomiya, Satoshi ; Suzuki, Tomo ; Grambow, Bernd ; Advocat, Thierry ; Bart, Florence ; Ewing, Rodney C. / Effects of ionizing radiation on the hollandite structure-type : Ba0.85 Cs0.26 Al1.35 Fe0.77 Ti5.90O16. In: American Mineralogist. 2008 ; Vol. 93, No. 1. pp. 241-247.
@article{b56f9a5d775a4f4b81a559acc70efb7f,
title = "Effects of ionizing radiation on the hollandite structure-type: Ba0.85 Cs0.26 Al1.35 Fe0.77 Ti5.90O16",
abstract = "The hollandite structure-type has received considerable attention as a nuclear waste form for the incorporation of radioactive 135Cs and 137Cs, both of which are important fission product radionuclides in the high-level nuclear waste generated by the reprocessing of used nuclear fuel. A critical concern has been the effects of high doses of ionizing radiation from incorporated Cs on the long-term structural stability of the hollandite structure. Optimization of the synthesis conditions has resulted in the hollandite stoichiometry of Ba0.85 Cs0.26 Al1.35 Fe0.77 Ti5.90 O16. To evaluate the effect of Cs-beta-decay on this stoichiometry, we have simulated the ionizing radiation using 200 kV electron beam using transmission electron microscopy (TEM) at 298 and 573 K. Complete amorphization was achieved at doses of 1.1 × 1014 and 1.8 × 1014 Gy at temperatures of 298 and 573 K, respectively. Electron energy-loss spectroscopy (EELS) of the Cs M-edge revealed the selective loss of Cs at the maximum doses. Hollandite irradiated using gamma rays, ∼106 Gy, which has defects associated with the formation of Ti3+ and O2- had a dissolution rate similar to that of the pristine hollandite, suggesting that the initial stage of defect formation does not influence chemical durability. Because the accumulated dose in the hollandite with 5 wt{\%} of radioactive 137Cs2O is estimated to be ∼2.0 × 1010 Gy after 500 years, the hollandite structure should be stable under the conditions anticipated for geologic disposal.",
author = "Abdesselam Abdelouas and Satoshi Utsunomiya and Tomo Suzuki and Bernd Grambow and Thierry Advocat and Florence Bart and Ewing, {Rodney C.}",
year = "2008",
month = "1",
day = "1",
doi = "10.2138/am.2008.2563",
language = "English",
volume = "93",
pages = "241--247",
journal = "American Mineralogist",
issn = "0003-004X",
publisher = "Mineralogical Society of America",
number = "1",

}

TY - JOUR

T1 - Effects of ionizing radiation on the hollandite structure-type

T2 - Ba0.85 Cs0.26 Al1.35 Fe0.77 Ti5.90O16

AU - Abdelouas, Abdesselam

AU - Utsunomiya, Satoshi

AU - Suzuki, Tomo

AU - Grambow, Bernd

AU - Advocat, Thierry

AU - Bart, Florence

AU - Ewing, Rodney C.

PY - 2008/1/1

Y1 - 2008/1/1

N2 - The hollandite structure-type has received considerable attention as a nuclear waste form for the incorporation of radioactive 135Cs and 137Cs, both of which are important fission product radionuclides in the high-level nuclear waste generated by the reprocessing of used nuclear fuel. A critical concern has been the effects of high doses of ionizing radiation from incorporated Cs on the long-term structural stability of the hollandite structure. Optimization of the synthesis conditions has resulted in the hollandite stoichiometry of Ba0.85 Cs0.26 Al1.35 Fe0.77 Ti5.90 O16. To evaluate the effect of Cs-beta-decay on this stoichiometry, we have simulated the ionizing radiation using 200 kV electron beam using transmission electron microscopy (TEM) at 298 and 573 K. Complete amorphization was achieved at doses of 1.1 × 1014 and 1.8 × 1014 Gy at temperatures of 298 and 573 K, respectively. Electron energy-loss spectroscopy (EELS) of the Cs M-edge revealed the selective loss of Cs at the maximum doses. Hollandite irradiated using gamma rays, ∼106 Gy, which has defects associated with the formation of Ti3+ and O2- had a dissolution rate similar to that of the pristine hollandite, suggesting that the initial stage of defect formation does not influence chemical durability. Because the accumulated dose in the hollandite with 5 wt% of radioactive 137Cs2O is estimated to be ∼2.0 × 1010 Gy after 500 years, the hollandite structure should be stable under the conditions anticipated for geologic disposal.

AB - The hollandite structure-type has received considerable attention as a nuclear waste form for the incorporation of radioactive 135Cs and 137Cs, both of which are important fission product radionuclides in the high-level nuclear waste generated by the reprocessing of used nuclear fuel. A critical concern has been the effects of high doses of ionizing radiation from incorporated Cs on the long-term structural stability of the hollandite structure. Optimization of the synthesis conditions has resulted in the hollandite stoichiometry of Ba0.85 Cs0.26 Al1.35 Fe0.77 Ti5.90 O16. To evaluate the effect of Cs-beta-decay on this stoichiometry, we have simulated the ionizing radiation using 200 kV electron beam using transmission electron microscopy (TEM) at 298 and 573 K. Complete amorphization was achieved at doses of 1.1 × 1014 and 1.8 × 1014 Gy at temperatures of 298 and 573 K, respectively. Electron energy-loss spectroscopy (EELS) of the Cs M-edge revealed the selective loss of Cs at the maximum doses. Hollandite irradiated using gamma rays, ∼106 Gy, which has defects associated with the formation of Ti3+ and O2- had a dissolution rate similar to that of the pristine hollandite, suggesting that the initial stage of defect formation does not influence chemical durability. Because the accumulated dose in the hollandite with 5 wt% of radioactive 137Cs2O is estimated to be ∼2.0 × 1010 Gy after 500 years, the hollandite structure should be stable under the conditions anticipated for geologic disposal.

UR - http://www.scopus.com/inward/record.url?scp=38649102469&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=38649102469&partnerID=8YFLogxK

U2 - 10.2138/am.2008.2563

DO - 10.2138/am.2008.2563

M3 - Article

AN - SCOPUS:38649102469

VL - 93

SP - 241

EP - 247

JO - American Mineralogist

JF - American Mineralogist

SN - 0003-004X

IS - 1

ER -