4.7 Article

Photocatalytic Conversion of Am(III) to Am(VI) Using a TiO2 Electrode

Journal

ACS APPLIED ENERGY MATERIALS
Volume 4, Issue 10, Pages 11854-11857

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsaem.1c02635

Keywords

photoelectrocatalysis; actinides; oxides; semiconductors; americium; electrochemistry; redox reactions

Funding

  1. U.S. Department of Energy (US-DOE), Office of Nuclear Energy through the Nuclear Energy University Program (NEUP) [DE-NE0008539]
  2. Center for Actinide Science and Technology (CAST) and Energy Frontier Research Center (EFRC) - US-DOE, Office of Science, Basic Energy Sciences [DE-SC0016568]
  3. U.S. Nuclear Regulatory Commission [NRC-HQ-84-14-G-0038]

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Titanium-titania nanostructured electrodes were used to photoelectrochemically oxidize Am(III) to Am(VI) in 0.1 M HNO3 solutions under UV-light illumination. The oxidation process occurred through the generation of adsorbed hydroxyl radicals or direct electron transfer. The one-electron Am(VI/V) couple at 1.60 V vs SCE can be applied in nuclear fuel reprocessing, with Am being the main challenge.
Titanium-titania (Ti vertical bar TiO2) nanostructured electrodes in 0.1 M HNO3 solutions under UV-light illumination using a 375 nm LED and a 1.55 V vs SCE bias photoelectrochemically oxidize Am(III) to Am(VI) ((AmO22+)-O-VI). Oxidation occurs through photoelectrochemically generated adsorbed hydroxyl radicals (2.81 V vs SCE) and/or direct electron transfer between the excited-state electrode (E(TiO2VB*) = ca. 2.95 V vs SCE) and Am(III) (E(Am-IV/III) = 2.62 V). An electrochemically irreversible but chemically reversible electrochemical process at 1.60 V vs SCE is assigned to the one-electron Am(VI/V) couple. This system may be applied to used nuclear fuel reprocessing to separate actinides of concern (U, Np, Pu, and Am), where Am is the most significant challenge.

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