Kimihiko Yano

Uranium Crystallization Test with Dissolver Solution of Irradiated Fuel

The crystallization process has been developed as a part of the advanced aqueous process, NEXT (New Extraction System for TRU recovery) for fast reactor (FR) cycle. In this process, a large part of U is separated from dissolver solution by crystallization as UO2(NO3)2.6H2O. The U crystallization test was carried out with real dissolver solution of irradiated FR fuel to investigate the influence of cooling rate on the crystal size and the behavior of fission product (FP) compared with that of Pu(IV). In regard to the influence of the cooling rate, it was confirmed that the crystal size was smaller as the cooling rate is faster. Although it was expectable that the decontamination performance was improved by diminishing the specific surface of the crystals, it was suggested that a large crystal produced by crystallization was not always high purity. Concerning the behavior of FPs, Eu behaved similarly to Pu(IV). Cs accompanied with U into the crystals under the condition in this test.

Experimental Study on U-Pu Cocrystallization Reprocessing Process

A new reprocessing system with a 2-stage crystallization process has been developed. In the first stage of the system, U and Pu are recovered from dissolver solution by U-Pu cocrystallization. Laboratory-scale experiments were carried out with U and Pu mixed and irradiated fuel dissolver solutions to obtain fundamental data on the U-Pu cocrystallization process. Pu(VI) was cocrystallized with U, but crystallization yields of Pu were lower than those of U. FPs were separated from U and Pu by cocrystallization, and decontamination factors of Cs and Eu to U in crystals were over 100.

Dissolution behavior of (U,Zr)O2-based simulated fuel debris in nitric acid

To explore the possibility of dissolving fuel debris into nitric acid as a potential pre-treatment for waste treatment in which the U and Pu are removed from the inventory, dissolution tests of U1−xZrxO2 and (U,Pu)1−xZrxO2 were carried out in 6 M HNO3 at 353 K. At the end of the dissolution test (after 4 h), the ratio of dissolved uranium decreased with an increase in the Zr contents, x. While the dissolution of U-rich samples was congruent, a preferential leaching of U was observed with Zr-rich samples. Taking into account these different dissolution phenomena, the dissolution rate analysis was carried out using surface-area model to calculate the instantaneous dissolution rate (IDR). The IDR decreased from 10−5 down to 10−10 mol cm−2 min−1 as x increased from 0 to 0.95. From these findings, dissolution with HNO3 is expected to be only applicable in U-rich part of fuel debris (x < 0.3) if the dissolution in 6 M HNO3 at 353 K is assumed. Application of complexing acids, such as mixture of HNO3 and HF, should be considered to increase the dissolution rate of the Zr-rich part.

Purification of uranium products in crystallization system for nuclear fuel reprocessing

Uranium crystallization system has been developed to establish an advanced aqueous reprocessing for fast breeder reactor (FBR) fuel cycle. In the crystallization system, most part of uranium in dissolved solution of spent FBR-MOX fuels is separated as uranyl nitrate hexahydrate (UNH) crystals by a cooling operation. The targets of U yield and decontamination factor (DF) on the crystallization system are decided from FBR cycle performance and plutonium enrichment management. The DF is lowered by involving liquid and solid impurities on and in the UNH crystals during crystallization. In order to achieve the DF performance (more than 100), we discuss the purification technology of UNH crystals using a Kureha Crystal Purifier (KCP). Results show that more than 90% of uranium in the feed crystals could be recovered as the purified crystals in all test conditions, and the DFs of solid and liquid impurities on the purified UNH crystals are more than 100 under longer residence time of crystals in the column of KCP device. The purification mechanism is mainly due to the repetition of sweating and recrystallization in the column under controlled temperature.

Mechanical properties of cubic (U,Zr)O2

Evaluation of fuel debris properties in the Fukushima Daiichi Nuclear Power Plant (1F) is required to develop fuel debris removal tools. In the removal of debris resulting from the TMI-2 accident, a core-boring system played an important role. Considering the working principle of core boring, hardness, elastic modulus, and fracture toughness were found to be important fuel debris properties that profoundly influenced the performance of the boring machine. It is speculated that uranium and zirconium oxide solid solution (U,Zr)O2 is one of the major materials in the fuel debris from 1F. In addition, the Zr content of the fuel debris from 1F is expected to be higher than that of the debris from TMI-2 because the 1F reactors were boiling-water reactor (BWR). In this research, the mechanical properties of cubic (U,Zr)O2 samples containing 10%¬-65% ZrO2 are evaluated. The hardness, elastic modulus, and fracture toughness are measured by the Vickers test, ultrasonic pulse echo method, and indentation fracture method, respectively. In case of the (U,Zr)O2 samples containing less than 50% ZrO2, Vickers hardness and fracture toughness increased, and the elastic modulus decreased slightly with increasing ZrO2 content. Moreover, all of those values of the (U,Zr)O2 samples containing 65% ZrO2 increased slightly compared to (U,Zr)O2 samples containing 55% ZrO2. ZrO2 content affects fracture toughness significantly in the case of samples containing less than 10% ZrO2. Higher Zr content (exceeding 50%) has little effect on the mechanical properties.

Continuous-Operation Test at Engineering Scale Uranium Crystallizer System

Uranium crystallization based on solubility difference is one of the remarkable technologies which can provide simple process to separate uranium in nitric acid solution since the process is mainly controlled by temperature and concentration of solute ions. Japan Atomic Energy Agency (JAEA) and Mitsubishi Materials Corporation (MMC) are developing the crystallization process for elemental technology of FBR fuel reprocessing.[1–3] The uranium (U) crystallization process is a key technology for New Extraction System for TRU Recovery (NEXT) process that was evaluated as the most promising process for future FBR reprocessing.[4–6] We had developed an innovative crystallizer and carried out several fundamental investigations. On the basis of the results, we fabricated an engineering-scale crystallizer and have carried out continuous operation test to investigate the stability of the equipment at steady and non-steady state conditions by using depleted uranium. As for simulating typical failure events in the crystallizer, crystal accumulation and crystal blockage were occurred intentionally, and monitoring method and resume procedure were tried and selected in this work. As the test results, no significant phenomenon was observed in the steady state test. And in the non-steady state test, process fluctuation could be detected by monitoring of screw torque and liquid level in the crystallizer, and all failure events are proven to be recovered by appropriate resumed procedures.© 2009 ASME