Influence of hydrogen reduction temperature in a fluidized bed on AUC derived UO₂ powder properties
Abstract
The production of uranium dioxide (UO₂) powders by calcination–reduction of ammonium uranyl carbonate (AUC, (NH₄)₄UO₂(CO₃)₃) is an important step in the UO₂ fuel pellet fabrication process. The nature and quality of the resulting UO₂ depend closely on the initial characteristics of AUC as well as on the applied thermal treatment conditions. The UO₂ powders obtained must meet specific requirements, particularly those related to specific surface area (4.5–7 m²/g) and particle size distribution. The objective of this work is to analyze the effect of the hydrogen reduction temperature on the properties of AUC-derived UO₂ powders using a fluidized-bed furnace. In this study, the reduction temperature of AUC was varied from 400 to 550 °C, and the resulting UO₂ powders were characterized. The O/U ratio, specific surface area, and particle size distribution of the UO₂ powders were determined respectively by spectrophotometry, nitrogen adsorption–desorption (BET method), and laser granulometry. During tests on stabilization of the AUC powder bed, it was observed that the minimum fluidization flow rate ranged between 20 and 30 L/min. Within this range, a proportional relationship was observed between the pressure drop and the fluidization velocity. Beyond 30 L/min, the fluidized bed became stable. As the reduction temperature increased from 400 to 550 °C, the specific surface area decreased from 10.2 to about 7 m²/g (±0.2 m²/g). However, the particle size distribution of the UO₂ powders varied only slightly with temperature. A reduction temperature of 550 °C under hydrogen in a fluidized bed was selected as the optimal condition for the conversion of AUC into UO₂ powder exhibiting good sintering properties for nuclear fuel pellet production (7 m²/g).
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Kim EH, Park JJ, Chang JH, Choi CS, Kim SD. Thermal decomposition kinetics of ammonium uranyl carbonate. J Nucl Mater. 1994;209:294–300. https://doi.org/10.1016/0022-3115(94)90266-6
Bachmann HG, Seibold K, Dokuzoguz HZ, Müller HM. X-ray powder diffraction and some thermodynamic data for (NH₄)₄[UO₂(CO₃)₃]. J Inorg Nucl Chem. 1975;37:735–737.
Hälldahl L. Study of the composition of the amorphous phase formed during decomposition of ammonium uranyl carbonate in various atmospheres. Thermochim Acta. 1985;95:389–394. https://doi.org/10.1016/0040-6031(85)85300-4
Hälldahl L. In situ studies of the decomposition of ammonium uranyl carbonate in an electron microscope. J Nucl Mater. 1984;126:170–176. https://doi.org/10.1016/0022-3115(84)90087-4
Kondal Rao N, et al. Technological aspects of UO₂ fuels: Characterisation and quality control – Indian experience. J Nucl Mater. 1979;81:171–176. https://doi.org/10.1016/0022-3115(79)90075-8
Hälldahl L, Nygren M. Thermal analysis studies of the reactions occurring during the decomposition of ammonium uranyl carbonate in different atmospheres. J Nucl Mater. 1986;138:99–106. https://doi.org/10.1016/0022-3115(86)90260-6
Marajofsky A, Pérez L, Celora J. On the dependence of characteristics of powders on the AUC process parameter. J Nucl Mater. 1991;178:143–151. https://doi.org/10.1016/0022-3115(91)90379-L
Hälldahl L, Sørensen T. Thermal analysis of the decomposition of ammonium uranyl carbonate (AUC) in different atmospheres. Thermochim Acta. 1979;29:253–259. https://doi.org/10.1016/0040-6031(79)87084-7
Hälldahl L, Nygren M. TG, DSC, X-ray and electron diffraction studies of intermediate phases in the reduction of ammonium uranyl carbonate to UO₂. Thermochim Acta. 1984;72:213–218.
Korichi S, Aoudia N, Benlmadjet H, Kaci S, Ousmaal N. Kinetic studies of isothermal decomposition of (NH₄)₄UO₂(CO₃)₃ to uranium oxide. Prog React Kinet Mech. 2020;45. https://doi.org/10.1177/1468678319888629
Korichi S, Mernache F, Benaouicha F, Aoudia N, Amrane A, Hadji S. Thermal behavior and kinetic modeling of (NH₄)₄UO₂(CO₃)₃ decomposition under non-isothermal conditions. J Radioanal Nucl Chem. 2017;314:923–934. https://doi.org/10.1007/s10967-017-5444-2
Le Page AH, Fane AG. The kinetics of hydrogen reduction of UO₃ and U₃O₈ derived from ammonium diuranate. J Inorg Nucl Chem. 1974;36:87–94. https://doi.org/10.1016/0022-1902(74)80663-9
Girgis BS, Rofail NH. Decomposition–reduction stages of ammonium uranyl carbonates under different atmospheres. Thermochim Acta. 1992;196:105–115. https://doi.org/10.1016/0040-6031(92)85010-S
Pijolat M, Brun C, Valdivieso F, Soustelle M. Reduction of uranium oxide U₃O₈ to UO₂ by hydrogen. Solid State Ionics. 1997;101–103:931–935. https://doi.org/10.1016/S0167-2738(01)00730-5
Tel H, Eral M. Investigation of production conditions and powder properties of AUC. J Nucl Mater. 1996;231:165–169. https://doi.org/10.1016/0022-3115(96)00354-6
Baran V, Vošček V. Spontaneous isothermal decomposition of the uranyl carbonate complex (NH₄)₄[UO₂(CO₃)₃] at room temperature. Part II: Infrared spectroscopy and X-ray analysis. Thermochim Acta. 1987;122(2):261–276. https://doi.org/10.1016/0040-6031(87)87047-8
Bing-Guo L, Jin-Hui P, Srinivasakannan C, Li-Bo Z, Jin-Ming H, Sheng-Hui G, Dong-Cheng K. Preparation of U₃O₈ by calcination from ammonium uranyl carbonate in microwave fields: Process optimization. Ann Nucl Energy. 2015;85:879–884.
Qingre G, Shifang K. Study of AUC thermal decomposition kinetics in nitrogen by a non-isothermal method. Thermochim Acta. 1987;116:71–77. https://doi.org/10.1016/0040-6031(87)88166-2
Ki BH, Lee YB, Prelas MA, Ghosh TK. Thermal and X-ray diffraction analysis during the decomposition of ammonium uranyl nitrate. J Radioanal Nucl Chem. 2012;292:1075–1083. https://doi.org/10.1007/s10967-011-1579-8
Gomes RP, Riella HG, Instituto de Pesquisas Energéticas e Nucleares (IPEN). Development of a reduction process of ammonium uranyl carbonate to uranium dioxide in a fluidized bed. In: Proceedings of the II CGEN – General Congress on Nuclear Energy; 1988; Rio de Janeiro, Brazil.
Cho WD, Han MH, Bronson MC, Zundelevich Y. Processing of uranium oxide powders in a fluidized-bed reactor. I. Experimental. J Nucl Mater. 2002;305:106–111. https://doi.org/10.1016/S0022-3115(02)01135-2
Patro JB, Sridharan AK, Katiyar NPS, Sampath M, Rajendran R, Sinha KK, Kondal Rao N. UO₂ fuels – Qualitative approach for characterization. *J Nucl Mater*. 1982;106:81–86. https://doi.org/10.1016/0022-3115(82)90335-X
Choi CS, Park JH, Kim EH, Shin HS, Chang IS. The influence of AUC powder characteristics on UO₂ pellets. J Nucl Mater. 1988;153:148–155. https://doi.org/10.1016/0022-3115(88)90206-1
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