Kinetics of oxidation and dissolution of uranium dioxide in aqueous acid solutions

被引：4

作者：

Gaulard-Balandret, Coralie ^{[1
,2
,3
]}

Larabi-Gruet, Nathalie ^{[4
]}

Miserque, Frederic ^{[5
]}

Radwan, Jean ^{[1
]}

Ferry, Cecile ^{[1
]}

Chausse, Annie ^{[3
]}

机构：

[1] CEA, DEN, DPC, Lab Mesures & Modelisat Migrat Radionucleides,SEC, F-91191 Gif Sur Yvette, France

[2] ANDRA, F-92298 Chatenay Malabry, France

[3] Univ Evry Val Essonne, Lab Anal & Modelisat Biol & Environm, CNRS, CEA,Univ Evry,UMR 8587, F-91025 Evry, France

[4] CEA, DEN, DPC, Lab Etud Corros Non Aqueuse,SCCME, F-91191 Gif Sur Yvette, France

[5] CEA, DEN, DPC, Lab Etud Corros Aqueuse,SCCME, F-91191 Gif Sur Yvette, France

来源：

ELECTROCHIMICA ACTA | 2012年 / 83卷

关键词：

Uranium dioxide; Oxidation mechanism; Triflate ions; Perchlorate ions; Rotating disc electrode; NUCLEAR-FUEL UO2; WASTE-DISPOSAL CONDITIONS; TRIFLUOROMETHANESULFONIC ACID; ANODIC-DISSOLUTION; PERCHLORATE SOLUTIONS; OXYGENATED SOLUTIONS; HYDROGEN-PEROXIDE; SIMFUEL UO2; CORROSION; PH;

D O I：

10.1016/j.electacta.2012.04.022

中图分类号：

O646 [电化学、电解、磁化学];

学科分类号：

081704 ;

摘要：

The oxidation and dissolution of UO2 has been studied using electrochemical methods with an UO2 rotating disc electrode in acidic (pH 3) and non-complexing (trifluoromethanesulfonate: 0.1 mol L-1 NaCF3SO3) media. The effect of the experimental parameters such as scan rate (nu) and rotation rate (omega) on the electrochemical signal has been studied. The rotation rate of the electrode does not influence the resulting signal, which indicates that only a charge transfer is involved in the UO2 oxidation kinetic. However, scan rate variations show different reactions involved in the UO2 oxidation. Linear sweep voltammetry and cyclic voltammetry coupled to X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma mass spectrometry (ICP-MS) measurements suggest two successive electrochemical reactions with an exchange of one electron for each of them and the formation of one intermediate species of U(V). (C) 2012 Published by Elsevier Ltd.

引用

页码：471 / 477

页数：7

共 26 条

[1]

[Anonymous], 1993, ELECTROCHIMIE ANAL R

[2] CYCLIC VOLTAMMETRY IN TRIFLUOROMETHANESULFONIC ACID - FACILE ELECTROCHEMISTRY UP TO +3 V [J].

BERNHARD, P ;

DIAB, H ;

LUDI, A .

INORGANICA CHIMICA ACTA, 1990, 173 (01) :65-68

[3]

CASAS I, 1994, RADIOCHIM ACTA, V66-7, P23

[4] REAGENTS FOR HIGH-TEMPERATURE AQUEOUS CHEMISTRY - TRIFLUOROMETHANESULFONIC ACID AND ITS SALTS [J].

FABES, L ;

SWADDLE, TW .

CANADIAN JOURNAL OF CHEMISTRY-REVUE CANADIENNE DE CHIMIE, 1975, 53 (20) :3053-3059

[5]

Gaulard C., 2012, THESIS U EVRY VAL DE

[6]

Guillaumont R., 2003, UPDATE CHEM THERMODY

[7] Mica surfaces stabilize pentavalent uranium [J].

Ilton, ES ;

Haiduc, A ;

Cahill, CL ;

Felmy, AR .

INORGANIC CHEMISTRY, 2005, 44 (09) :2986-2988

[8] The electrochemical reduction of hydrogen peroxide on uranium dioxide under intermediate pH to acidic conditions [J].

Keech, P. G. ;

Noel, J. J. ;

Shoesmith, D. W. .

ELECTROCHIMICA ACTA, 2008, 53 (18) :5675-5683

[9] On the reduction of ClO4- ions in the course of metal dissolution in HClO4 solutions [J].

Láng, G ;

Ujvári, M ;

Horányi, G .

CORROSION SCIENCE, 2003, 45 (01) :1-5

[10]

Larabi N., 2005, THESIS U P M CURIE P

← 1 2 3 →