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Sorption behaviors of neptunium (V) on naturally-occurring magnetite (Fe3O4) and goethite (α-FeOOH) in 0.1M NaN03 electrolyte solution under aerobic conditions were interpreted using the surface complexation model (SCM). The surface properties of these materials were experimentally investigated by C02-free potentiometric titration, and SCM parameters for the constant capacitance model, such as protonation/deprotonation constants of the surface hydroxyl group, were determined. The number of negatively charged sorption sites of goethite rapidly increased with the increase of the bulk solution pH compared with that of magnetite and this tendency was similar to the pH dependence of neptunium sorption. This implies that the neptunyl cation, NpO2+, plays a dominant role in possible sorption reactions. Assuming that the dominant surface complex is XO-NpO2, modeling by means of SCM was carried out, and the results were found to agree with experimental data.

From the viewpoint of waste management, a quantitative evaluation of LWR nuclear fuel cycle system performance was carried out, considering both higher burn-up operation of UO 2 fuel coupled with the introduction of MOX fuel. A major parameter to quantify this performance is the number of high-level waste (HLW) glass units generated per GWd (gigawatt-day based on reactor thermal power generation before electrical conversion). This parameter was evaluated for each system up to a maximum burn-up of 70 GWd/THM (gigawatt-day per ton of heavy metal) assuming current conventional reprocessing and vitrification conditions where the waste loading of glass is restricted by the heat generation rate, the MoO 3 content, or the noble metal content. The results showed that higher burn-up operation has no significant influence on the number of glass units generated per GWd for UO 2 fuel, though the number of glass units per THM increases linearly with burn-up and is restricted by the heat generation rate. On the other hand, the introduction of MOX fuel causes the number of glass units per GWd to double owing to the increase in the heat generation rate. An extended cooling period of the spent fuel prior to reprocessing effectively reduces the heat generation rate for UO 2 fuel, while a separation of minor actinides (Np, Am, and Cm) from the high-level waste provides additional reduction for MOX fuel. However, neither of these leads to a substantial reduction in the number of glass units, since the MoO 3 content or the noble metal content restricts the number of glass units rather than the heat generation rate. These results suggest that both the MoO 3 content and the noble metal content provide the key to reducing the amount of waste glass that is generated, leading to an overall improvement in fuel cycle system performance.

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