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Kinetics of dissolution of simulated (U–Ce) MOX fuel pellet in nitric acid

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Abstract

In the present study, the dissolution kinetics of simulated urania, ceria MOX fuel pellets in nitric acid under PUREX process condition has been investigated. Influence of various parameters like initial concentration of nitric acid, temperature and Ce composition on rate of dissolution of MOX fuel pellet was studied. Rate expression was developed by considering Langmuir–Hinshelwood mechanism to describe the dissolution of MOX fuel pellet in nitric acid. The estimated value of activation energy of about 40–50 kJ mol−1 confirms the intrinsic nature of dissolution kinetics.

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Abbreviations

HNO3 :

Nitric acid

UO2 :

Uranium dioxide

CeO2 :

Cerium oxide

MOX:

Mixed oxide

U:

Uranium

Pu:

Plutonium

Ce:

Cerium

v B :

Stoichiometric coefficient of UO2

v AB :

Stoichiometric coefficient of HNO3 for UO2 dissolution

v E :

Stoichiometric coefficient of CeO2

v AE :

Stoichiometric coefficient of HNO3 for CeO2 dissolution

C:

Cocentration, kmol m−3

kLA :

Mass transfer coefficient between the reaction surface and the bulk liquid phase, m/s

nA :

Number of mols of nitric acid in reaction mixture

nBL :

Number of mols of uranium in reaction mixture

nEL :

Number of mols of cerium in reaction mixture

kB :

Rate constant for UO2 dissolution, kmol m−5 s−1

kE :

Rate constant for CeO2 dissolution, kmol m−5 s−1

rsB :

Rate of surface reaction for UO2 dissolution, kmol m−5 s−1

rsE :

Rate of surface reaction for CeO2 dissolution, kmol m−5 s−1

AtB :

Reactive surface area for UO2 dissolution at any time, m2

AtE :

Reactive surface area for CeO2 dissolution at any time, m2

θ AU :

The surface coverage of HNO3 on solid phase by adsorption for UO2 dissolution (fractional coverage)

θ AE :

The surface coverage of HNO3 on solid phase by adsorption for CeO2 dissolution (fractional coverage)

T:

Temperature, K

θ A :

Surface coverage of HNO3 on solid phase by adsorption

Kad :

Adsorption constant, m3 kmol−1

a:

Shape factor

Ap :

Reactive surface area of particle, m2

Vp :

Volume of particle, m3

R:

Radius of particle, m

n:

Amount of unreacted solid at any time, t

n0 :

Amount of solid material at time, t = 0

M:

Molecular wt of MOX pellet, gmmol−1

mP :

Mass of solid particle, kg

x0B :

Mole fraction of UO2

n0B :

Amount of UO2 in solid partcile at time, t = 0

nB :

Unreacted amount of UO2 in solid particle at any time, t

x0E :

Mole fraction of CeO2

n0E :

Amount of CeO2 in solid particle at time, t = 0

nE :

Unreacted amount of CeO2 in solid particle at any time, t

VL :

Volume of the reaction mixture, m3

L:

Liquid phase/Reaction mixture

B:

UO2/Uranium

A:

Nitric acid

E:

CeO2/Cerium

S:

Concentration at solid surface

b:

Bulk liquid phase

t:

Time

0/t = 0:

Initial condition, at t = 0

f:

Final condition

p:

Solid particle

Calc:

Calculated

Exp:

Experimental

ρp :

Density of solid particle, kg m−3

σ:

Specific surface area of solid particle, m2 kg−1

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Authors and Affiliations

  1. Reprocessing R&D Division, Reprocessing Group, IGCAR, Kalpakkam, 603 102, India

    Elizabeth Augustine, N. Desigan, R. Rajeev & N. K. Pandey

  2. Institute of Chemical Technology, Mumbai, 400 019, India

    J. B. Joshi

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  1. Elizabeth Augustine
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Augustine, E., Desigan, N., Rajeev, R. et al. Kinetics of dissolution of simulated (U–Ce) MOX fuel pellet in nitric acid. J Radioanal Nucl Chem 331, 4529–4539 (2022). https://doi.org/10.1007/s10967-022-08582-w

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