TY - JOUR
T1 - Photocatalytic Conversion of Am(III) to Am(VI) Using a TiO2Electrode
AU - Sheridan, Matthew V.
AU - Gonzalez-Moya, Johan R.
AU - McLachlan, Jeffrey R.
AU - Grimes, Travis S.
AU - Dares, Christopher J.
N1 - Funding Information:
This research was supported by the U.S. Department of Energy (US-DOE), Office of Nuclear Energy through the Nuclear Energy University Program (NEUP) under award number DE-NE0008539, and the Center for Actinide Science and Technology (CAST) and Energy Frontier Research Center (EFRC) funded by the US-DOE, Office of Science, Basic Energy Sciences, under Award Number DE-SC0016568. J.R.M was supported by a U.S. Nuclear Regulatory Commission for a Graduate Student Fellowship (NRC-HQ-84-14-G-0038).
Publisher Copyright:
© 2021 American Chemical Society.
PY - 2021/10/25
Y1 - 2021/10/25
N2 - Titanium-titania (Ti|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) (AmVIO22+). 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(AmIV/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.
AB - Titanium-titania (Ti|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) (AmVIO22+). 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(AmIV/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.
KW - actinides
KW - americium
KW - electrochemistry
KW - oxides
KW - photoelectrocatalysis
KW - redox reactions
KW - semiconductors
UR - https://www.scopus.com/pages/publications/85117282286
UR - https://www.mendeley.com/catalogue/a59dc455-9bfd-3682-8ada-8b76611f015c/
U2 - 10.1021/acsaem.1c02635
DO - 10.1021/acsaem.1c02635
M3 - Article
AN - SCOPUS:85117282286
SN - 2574-0962
VL - 4
SP - 11854
EP - 11857
JO - ACS Applied Energy Materials
JF - ACS Applied Energy Materials
IS - 10
ER -