Study on damage of Gd2O3-CeO2 under electronic energy loss: comparison between bulk-like and nanostructure

Physical chemistry chemical physics : PCCP(2024)

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摘要
To understand the physical phenomena responsible for radiation damage of the materials used in nuclear reactors, and thus study their operation life and/or efficiency, it is required to simulate the conditions by exposing the materials to energetic ions. Ceria (CeO2) has been proposed as one of the inert matrices for the transmutation of minor actinides in the futuristic inert matrix fuel (IMF) concept. The inert matrix should also contain burnable poison to compensate for the initial reactivity of fuel. In this context, gadolinium (Gd) is an excellent burnable poison with a high neutron absorption cross-section. In view of this, Gd2O3-CeO2 nano-powders were synthesized and sintered at 800 degrees C and 1300 degrees C to obtain different grain sizes and morphologies. FESEM and TEM were carried out to study the grain size of pristine pellets. The sintered pellets were irradiated with 80-MeV Ag ions (electronic energy loss (S-e) regime) at room temperature to emulate the effect of fission fragments. For analysis of the effect of grain size on the irradiation-induced structural degradation at different fluences, GIXRD and Raman spectroscopy were performed. Significantly large damage has been observed for the smaller grain-sized samples (sintered at 800 degrees C) as compared to the large grain-sized sample (sintered at 1300 degrees C). Neither of the samples amorphized under the present experimental conditions as indicated by the presence of the Raman-active T-2g mode (centred at 462 cm(-1)) and all the XRD peaks of fluorite cubic structure up to the highest fluence employed (1 x 10(14) ions cm(-2)). X-ray photoelectron spectroscopy results demonstrate that Ce4+ to Ce3+ and vacancy-related isolated clusters are the main defects produced in the systems. The radiation tolerance behaviour of the samples is understood with the help of thermal spike simulation, which indicates higher transient lattice temperatures with longer duration in the smaller grain-sized sample upon irradiation. Gd-doped ceria thus possesses good radiation stability in the S-e regime, indicating its potential for application in IMFs.
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