Technetium-99 (99Tc) is a high yield (~6%) product of Uranium-235 fission and is a weak beta emitter (bmax energy of 0.29 MeV) with a half-life of 2.1x105 years. When exposed to air, 99Tc is most prevalent in its oxidized (Tc(VII)) form, which exists predominantly as pertechnetate (TcO4-). The immobilization of 99Tc in the environment has usually been achieved via reduction of the prevalent TcO4- anion to relatively insoluble TcO2, Tc(IV) species. We have been studying the use of small metal-oxide clusters called Keggin polyoxometalates (POMs), XM12O40n- (X= P, Si, Al, n=3, 4, 5) to act as both reducing agent and chelator for 99Tc to lower valent species. The reduction potentials of Keggin POMs are a function of the central heteroatom that dictates the overall charge of the ion and its reduction potential. Under UV and visible light in acidic conditions they promote reduction of TcO4- to Tc(IV) in the form of TcO2●2H2O and Tc2(μ-O)2 4+ species. The examination of Keggin POMs to photocatalytically reduce TcO4- will lead to investigation of solid-state materials for photocatalytic reduction of TcO4-.

Strategies for the photoreduction of Tc-99 pertechnetate to low valent Tc by Keggin polyoxometalates

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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