Incorporation of Technetium into Spinel Ferrites
Abstract
Technetium (99Tc) is a problematic fission product for the long-term disposal of nuclear waste due to its long half-life, high fission yield, and to the environmental mobility of pertechnetate, the stable species in aerobic environments. One approach to preventing 99Tc contamination is using sufficiently durable waste forms. We report the incorporation of technetium into a family of synthetic spinel ferrites that have environmentally durable natural analogs. A combination of X-ray diffraction, X-ray absorption fine structure spectroscopy, and chemical analysis reveals that Tc(IV) replaces Fe(III) in octahedral sites and illustrates how the resulting charge mismatch is balanced. When a large excess of divalent metal ions is present, the charge is predominantly balanced by substitution of Fe(III) by M(II). When a large excess of divalent metal ions is absent, the charge is largely balanced by creation of vacancies among the Fe(III) sites (maghemitization). In most samples, Tc is present in Tc-rich regions rather than being homogeneously distributed.
- Authors:
-
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; European Commission, Karlsruhe (Germany). Joint Research Centre, Inst. for Transuranium Elements
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Geosciences Group
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1482510
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Environmental Science and Technology
- Additional Journal Information:
- Journal Volume: 50; Journal Issue: 23; Journal ID: ISSN 0013-936X
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Lukens, Wayne W., Magnani, Nicola, Tyliszczak, Tolek, Pearce, Carolyn I., and Shuh, David K. Incorporation of Technetium into Spinel Ferrites. United States: N. p., 2016.
Web. doi:10.1021/acs.est.6b04209.
Lukens, Wayne W., Magnani, Nicola, Tyliszczak, Tolek, Pearce, Carolyn I., & Shuh, David K. Incorporation of Technetium into Spinel Ferrites. United States. https://doi.org/10.1021/acs.est.6b04209
Lukens, Wayne W., Magnani, Nicola, Tyliszczak, Tolek, Pearce, Carolyn I., and Shuh, David K. Mon .
"Incorporation of Technetium into Spinel Ferrites". United States. https://doi.org/10.1021/acs.est.6b04209. https://www.osti.gov/servlets/purl/1482510.
@article{osti_1482510,
title = {Incorporation of Technetium into Spinel Ferrites},
author = {Lukens, Wayne W. and Magnani, Nicola and Tyliszczak, Tolek and Pearce, Carolyn I. and Shuh, David K.},
abstractNote = {Technetium (99Tc) is a problematic fission product for the long-term disposal of nuclear waste due to its long half-life, high fission yield, and to the environmental mobility of pertechnetate, the stable species in aerobic environments. One approach to preventing 99Tc contamination is using sufficiently durable waste forms. We report the incorporation of technetium into a family of synthetic spinel ferrites that have environmentally durable natural analogs. A combination of X-ray diffraction, X-ray absorption fine structure spectroscopy, and chemical analysis reveals that Tc(IV) replaces Fe(III) in octahedral sites and illustrates how the resulting charge mismatch is balanced. When a large excess of divalent metal ions is present, the charge is predominantly balanced by substitution of Fe(III) by M(II). When a large excess of divalent metal ions is absent, the charge is largely balanced by creation of vacancies among the Fe(III) sites (maghemitization). In most samples, Tc is present in Tc-rich regions rather than being homogeneously distributed.},
doi = {10.1021/acs.est.6b04209},
journal = {Environmental Science and Technology},
number = 23,
volume = 50,
place = {United States},
year = {Mon Nov 21 00:00:00 EST 2016},
month = {Mon Nov 21 00:00:00 EST 2016}
}
Web of Science
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