Synthesis and Characterization of Non-Aqueous [TcXM-PW11O39]n– with M = O, N: Comparing TcV and TcVI in Metal Oxide Matrices

Burton‐Pye, Benjamin P.; Dembowski, Mateusz; Lukens, Wayne W.; Cruz, Anthony; Althour, Alrasheed; Lopez, Gustavo E.; Salcedo, Ramsey; Gallagher, Colleen B.; McGregor, Donna; Francesconi, Lynn C.

doi:10.1002/ejic.201900864

Title: Synthesis and Characterization of Non-Aqueous [Tc^XM-PW11O39]ⁿ^– with M = O, N: Comparing Tc^V and Tc^VI in Metal Oxide Matrices

Journal Article · Tue Nov 26 00:00:00 EST 2019 · European Journal of Inorganic Chemistry

DOI:https://doi.org/10.1002/ejic.201900864· OSTI ID:1782133

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^[3]; Cruz, Anthony ^[1]; Althour, Alrasheed ^[4];

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^[5]; Gallagher, Colleen B. ^[6];

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City Univ. of New York (CUNY), NY (United States). Lehman College; City Univ. of New York (CUNY), NY (United States). Ph.D. Program in Chemistry Graduate Center
City Univ. of New York (CUNY), NY (United States). Hunter College
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Div., The Glenn T. Seaborg Center
City Univ. of New York (CUNY), NY (United States). Lehman College
City Univ. of New York (CUNY), NY (United States). Lehman College; City Univ. of New York (CUNY), NY (United States). Ph.D. Program in Chemistry Graduate Center; City Univ. of New York (CUNY), NY (United States). Hunter College
City Univ. of New York (CUNY), NY (United States). Ph.D. Program in Chemistry Graduate Center; City Univ. of New York (CUNY), NY (United States). Hunter College

Technetium‐99, a prevalent by‐product of the nuclear fuel cycle, is a transition metal with 9 accessible oxidation states and a half‐life of 2.1 × 10 ⁵ years. ⁹⁹ Tc ^VII has been found in the environment surrounding National Lab sites and fuel reprocessing centers, and its separation and long‐term storage is complicated by its extensive redox chemistry. In our prior work we have reported the synthesis and reduction of Tc ^V O to Tc ^IV O in α ₁ ‐ and α ₂ ‐Wells–Dawson P ₂ W ₁₇ O ₆₁ ^10– polyoxometalates and reported on the polyoxometalate features that promote reduction and stabilization. In this work we report on the oxidation state stabilization of Tc ^V O, Tc ^VI O and Tc ^VI N within the α‐Keggin PW ₁₁ O ₃₉ ^7– polyoxometalate. Both Density Functional Theory and experimental results show that Tc in TBA ₄ [Tc ^VI N‐PW ₁₁ O ₃₉ ] can be reduced to Tc ^V , but any subsequent electrons reduce the tungsten framework of the polyoxometalate. TBA ₄ [Tc ^V O‐PW ₁₁ O ₃₉ ] however, can be theoretically reduced down to Tc ^I before reduction of the polyoxometalate occurs.

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

Sponsoring Organization:: USDOE Office of Science (SC); National Science Foundation (NSF)

Grant/Contract Number:: AC02-05CH11231; HRD-1547830; DGE-0965983; CHE-0750118; FG‐09ER16097

OSTI ID:: 1782133

Alternate ID(s):: OSTI ID: 1575837

Journal Information:: European Journal of Inorganic Chemistry, Vol. 2019, Issue 45; ISSN 1434-1948

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 2 works

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Title: Synthesis and Characterization of Non-Aqueous [Tc^XM-PW11O39]ⁿ^– with M = O, N: Comparing Tc^V and Tc^VI in Metal Oxide Matrices