Incorporation of Technetium into Spinel Ferrites

Lukens, Wayne W.; Magnani, Nicola; Tyliszczak, Tolek; Pearce, Carolyn I.; Shuh, David K.

doi:10.1021/acs.est.6b04209

Incorporation of Technetium into Spinel Ferrites

Journal Article · Mon Nov 21 00:00:00 EST 2016 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.6b04209· OSTI ID:1482510

Lukens, Wayne W. ^[1]; Magnani, Nicola ^[2]; Tyliszczak, Tolek ^[3]; Pearce, Carolyn I. ^[4]; Shuh, David K. ^[1]

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

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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1482510

Alternate ID(s):: OSTI ID: 1406815

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 23 Vol. 50; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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