On the change in UO2 redox reactivity as a function of H2O2 exposure

被引:18
|
作者
Maier, Annika Carolin [1 ]
Kegler, Philip [2 ]
Klinkenberg, Martina [2 ]
Baena, Angela [2 ]
Finkeldei, Sarah [2 ]
Brandt, Felix [2 ]
Jonsson, Mats [1 ]
机构
[1] KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth, Dept Chem, S-10044 Stockholm, Sweden
[2] Forschungszentrum Julich, Inst Energy & Climate Res Nucl Waste Management &, D-52425 Julich, Germany
关键词
RADIATION-INDUCED DISSOLUTION; SPENT NUCLEAR-FUEL; OXIDATIVE DISSOLUTION; RADIOLYSIS PRODUCTS; RELATIVE IMPACT; HYDROGEN; RAMAN; DIOXIDE; SIMFUEL; STORAGE;
D O I
10.1039/c9dt04395k
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
To assess the long-term leaching behaviour of UO2, the main constituent of spent nuclear fuel, the oxidative dissolution of UO2 pellets was studied at high H2O2 exposures ranging from 0.33 mol m(-2) to 1.36 mol m(-2). The experiments were performed in aqueous media containing 10 mM HCO3- where the pellets were exposed to H2O2 three consecutive times. The results indicate that the dissolution yield (amount of dissolved uranium per consumed H2O2) at high H2O2 exposures is significantly lower compared to previous studies of both pellets and powders and decreases for each H2O2 addition for a given pellet. This implies a change in redox reactivity, which is attributed to irreversible alteration of the pellet surface. Surface characterization after the exposure to H2O2, by SEM, XRD and Raman spectroscopy shows, that the surface of all pellets is significantly oxidized.
引用
收藏
页码:1241 / 1248
页数:8
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