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Research output: Contribution to Journal/Magazine › Journal article › peer-review
Research output: Contribution to Journal/Magazine › Journal article › peer-review
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TY - JOUR
T1 - Ruthenium volatilisation from reprocessed spent nuclear fuel - Studying the baseline thermodynamics of Ru(III)
AU - Johal, Sukhraaj K.
AU - Boxall, Colin
AU - Gregson, Colin
AU - Steele, Carl J.
N1 - © 2015 ECS - The Electrochemical Society
PY - 2015
Y1 - 2015
N2 - Ruthenium is a fission product possessed of two relatively long lived isotopes, Ru and Ru, both of which form part of the Highly Active (HA) waste raffinate during spent nuclear fuel reprocessing. During reprocessing ruthenium, which may be in the form of the RuNO+ complex, encounters temperatures conducive to volatilization. Due rutheium's high specific radioactivity it is important to understand the mechanism by which volatilisation occurs. Here we use combined CV, RDE and electrochemical microgravimetry experiments in a study of the the RuCl3 system for the first time. We do this in the interest of establishing NO-free Ru(III) baseline behaviour so as to support future studies on NO complexed ruthenium. Using wide aqueous solvent window carbon electrodes we have observed discrete oxidations to a solution phase Ru(III)-Ru(IV)-Ru(III) trimer, to solid RuO2 and volatile RuO4. We have also observed and assigned discrete reductions of solid RuO2 back to Ru(III) and Ru(III) reduction to ruthenium metal.
AB - Ruthenium is a fission product possessed of two relatively long lived isotopes, Ru and Ru, both of which form part of the Highly Active (HA) waste raffinate during spent nuclear fuel reprocessing. During reprocessing ruthenium, which may be in the form of the RuNO+ complex, encounters temperatures conducive to volatilization. Due rutheium's high specific radioactivity it is important to understand the mechanism by which volatilisation occurs. Here we use combined CV, RDE and electrochemical microgravimetry experiments in a study of the the RuCl3 system for the first time. We do this in the interest of establishing NO-free Ru(III) baseline behaviour so as to support future studies on NO complexed ruthenium. Using wide aqueous solvent window carbon electrodes we have observed discrete oxidations to a solution phase Ru(III)-Ru(IV)-Ru(III) trimer, to solid RuO2 and volatile RuO4. We have also observed and assigned discrete reductions of solid RuO2 back to Ru(III) and Ru(III) reduction to ruthenium metal.
U2 - 10.1149/06621.0031ecst
DO - 10.1149/06621.0031ecst
M3 - Journal article
AN - SCOPUS:84940397501
VL - 66
SP - 31
EP - 42
JO - ECS Transactions
JF - ECS Transactions
SN - 1938-6737
T2 - Symposium on Electrochemical Engineering General Session - 227th ECS Meeting
Y2 - 24 May 2015 through 28 May 2015
ER -