Improvement of plutonium proliferation resistance by doping minor actinides

This paper focuses on improving the proliferation resistance of plutonium resulting from uranium-based fuel irradiation. Intrinsic properties of plutonium isotopes with even mass numbers (²³⁸Pu, ²⁴⁰Pu and ²⁴²Pu) — in terms of their intense decay heat and high spontaneous fission neutron rates — were used as a measure to improve the proliferation resistance of plutonium itself. The present study explores MA addition effect into LEU (5%²³⁵U) and HEU (20%²³⁵U) with regard to plutonium proliferation resistance characteristics. Consideration goes beyond critical condition to examine the potential of subcritical system in enhancing the plutonium proliferation properties. Results show that even the doping level of 1% of Np, TrPu or all MA elements into low enriched uranium improves the proliferation-resistant properties of plutonium. A potential for further improvement is achieved by higher doping of minor actinides into high enriched uranium irradiated in a subcritical mode.     

A conceptual design study of proliferation-resistant PWR fuel using reprocessed uranium

A conceptual design study was carried out to enhance proliferation-resistant nature of current light water reactor fuels. Main features of the proliferation-resistant fuel design are adoption of alloy instead of oxide and utilization of enriched reprocessed uranium (10 wt% ²³⁵U). Major dimensions of the fuel assembly were not changed because of thermal-hydraulic considerations and back-fittability to current PWRs. Its smaller ²³⁸U inventory reduces generation of plutonium and ²³⁶U in the reprocessed uranium promotes generation of ²³⁸Pu that has large decay heat. The assembly calculation results of the fuel indicated that the fuel has good proliferation-resistant nature in the viewpoint of decreased plutonium generation, worse plutonium composition and increased decay heat. Neutronic analyses of an equilibrium core loaded with the proliferation-resistant fuels were carried out and calculation results indicate that variations of major core safety parameters are not very large. Therefore, basic feasibility of the proliferation-resistant fuel design using reprocessed uranium was confirmed in the course of this study.     

Adapting the deep burn in-core fuel management strategy for the gas turbine – modular helium reactor to a uranium–thorium fuel

In 1966, Philadelphia Electric has put into operation the Peach Bottom I nuclear reactor, it was the first high temperature gas reactor (HTGR); the pioneering of the helium-cooled and graphite-moderated power reactors continued with the Fort St. Vrain and THTR reactors, which operated until 1989. The experience on HTGRs lead General Atomics to design the gas turbine – modular helium reactor (GT-MHR), which adapts the previous HTGRs to the generation IV of nuclear reactors. One of the major benefits of the GT-MHR is the ability to work on the most different types of fuels: light water reactors waste, military plutonium, MOX and thorium. In this work, we focused on the last type of fuel and we propose a mixture of 40% thorium and 60% uranium. In a uranium–thorium fuel, three fissile isotopes mainly sustain the criticality of the reactor: ²³⁵U, which represents the 20% of the fresh uranium, ²³³U, which is produced by the transmutation of fertile ²³²Th, and ²³⁹Pu, which is produced by the transmutation of fertile ²³⁸U. In order to compensate the depletion of ²³⁵U with the breeding of ²³³U and ²³⁹Pu, the quantity of fertile nuclides must be much larger than that one of ²³⁵U because of the small capture cross-section of the fertile nuclides, in the thermal neutron energy range, compared to that one of ²³⁵U. At the same time, the amount of ²³⁵U must be large enough to set the criticality condition of the reactor. The simultaneous satisfaction of the two above constrains induces the necessity to load the reactor with a huge mass of fuel; that is accomplished by equipping the fuel pins with the JAERI TRISO particles. We start the operation of the reactor with loading fresh fuel into all the three rings of the GT-MHR and after 810 days we initiate a refueling and shuffling schedule that, in 9 irradiation periods, approaches the equilibrium of the fuel composition. The analysis of the k_eff and mass evolution, reaction rates, neutron flux and spectrum at the equilibrium of the fuel composition, highlights the features of a deep burn in-core fuel management strategy for a uranium–thorium fuel.     

Fast Reactor Operating on Uranium–Plutonium Oxide Fuel in a Self-Regulatable Regime

Mathematical simulation is used to show that it is possible to develop a fast reactor operating on uranium–plutonium oxide fuel (UO₂)_1–x (PuO₂) _x , the same for all fuel elements in the core, and with uranium carbide in breeding elements with heavy coolant (PbBi eutectic). A self-regulatable regime is obtained in the reactor. This enhances safety while minimizing control. Tailings uranium with 0.1% ²³⁵U and a mixture of plutonium isotopes, which is obtained from spent fuel, making it possible to conduct operation in an actinide-closed fuel cycle, is used in the fuel and uranium carbide. ²³⁸U is actually consumed in the reactor, but most fission products are produced from ²³⁹Pu.     

A study of the generation of 232U in UO2 and MOX fuels

To clarify the generation pathway of ²³²U, an important nuclide for dose evaluation at various stages in the reuse of uranium, concentrations of ²³²U generated through various pathways were evaluated for UO₂ and mixed oxide (MOX) fuels. Burnup calculation was conducted with ORIGEN2.2 code adopting ORLIBJ40 library, a set of cross-section libraries based on JENDL-4.0. It was found that differences in ²³²U concentrations in UO₂ and MOX fuels mainly arise from differences in the initial compositions of ²³⁴U, ²³⁵U, and ²³⁶U. It was also found that the contribution of plutonium and americium isotopes in MOX fuels is small compared with that of uranium isotopes. The results clarified that the capture cross sections of ²³⁰Th, ²³¹Pa, ²³⁵U, and ²³⁶U, as well as the (n,2n) cross sections of ²³⁷Np and ²³⁸U, have a large effect on the generation of ²³²U. Additional investigation showed that ²³²U concentration is strongly affected not only by time after irradiation but also by time before irradiation.     

Effect of Transplutonium Doping on Approach to Long-life Core in Uranium-fueled PWR

The present paper advertises doping of transplutonium isotopes as an essential measure to improve proliferation-resistance properties and burnup characteristics of UOX fuel for PWR. Among them ²⁴¹Am might play the decisive role of burnable absorber to reduce the initial reactivity excess while the short-lived nuclides ²⁴²Cm and ²⁴⁴Cm decay into even plutonium isotopes, thus increasing the extent of denaturation for primary fissile ²³⁹Pu in the course of reactor operation. The doping composition corresponds to one discharged from a current PWR. For definiteness, the case identity is ascribed to atomic percentage of ²⁴¹ Am, and then the other transplutonium nuclide contents follow their ratio as in the PWR discharged fuel. The case of 1 at% doping to 20% enriched uranium oxide fuel shows the potential of achieving the burnup value of 100GWd/tHM with about 20% ²³⁸Pu fraction at the end of irradiation. Since so far, americium and curium do not require special proliferation resistance measures, their doping to UOX would assist in introducing nuclear technology in developing countries with simultaneous reduction of accumulated minor actinides stockpiles.     

Burn up extension with slightly enriched uranium and plutonium fuel in CANDU reactors

A study of fuel burn-up and concentrations of uranium and plutonium isotopes for the three fuel cycles of a CANDU reactor are carried out in the present work. The infinite and effective multiplication factors are calculated as a function of fuel burn up for the natural UO₂ fuel, 1.2% enriched UO₂ fuel and for the 0.45% PuO₂-UO₂ fuel. The amount of ²³⁵U and ²³⁸U consumed and ²³⁹Pu, ²⁴⁰Pu and ²⁴¹Pu produced in the three fuel cycles are also calculated and compared.     

Performance of the gas turbine-modular helium reactor fuelled with different types of fertile TRISO particles

Preliminary studies have been performed on operation of the gas turbine-modular helium reactor (GT-MHR) with a thorium based fuel. The major options for a thorium fuel are a mixture with light water reactors spent fuel, mixture with military plutonium or with with fissile isotopes of uranium. Consequently, we assumed three models of the fuel containing a mixture of thorium with ²³⁹Pu, ²³³U or ²³⁵U in TRISO particles with a different kernel radius keeping constant the packing fraction at the level of 37.5%, which corresponds to the current compacting process limit. In order to allow thorium to act as a breeder of fissile uranium and ensure conditions for a self-sustaining fission chain, the fresh fuel must contain a certain quantity of fissile isotope at beginning of life; we refer to the initial fissile nuclide as triggering isotope. The small capture cross-section of ²³²Th in the thermal neutron energy range, compared to the fission one of the common fissile isotopes (²³⁹Pu, ²³³U and ²³⁵U), requires a quantity of thorium 25–30 times greater than that one of the triggering isotope in order to equilibrate the reaction rates. At the same time, the amount of the triggering isotope must be enough to set the criticality condition of the reactor. These two conditions must be simultaneously satisfied. The necessity of a large mass of fuel forces to utilize TRISO particles with a large radius of the kernel, 300 μm. Moreover, in order to improve the neutron economics, a fuel cycle based on thorium requires a low capture to fission ratio of the triggering isotope. Amid the common fissile isotopes, ²³³U, ²³⁵U and ²³⁹Pu, we have found that only the uranium nuclides have shown to have the suitable neutronic features to enable the GT-MHR to work on a fuel based on thorium.     

Irradiation analysis of U, Am samples irradiated in experimental fast reactor “Joyo” for protected plutonium production in fast breeder reactor blanket

Americium is a key element to design the FBR based nuclear fuel cycle, because of its long-term high radiological toxicity as well as a resource of even-mass-number plutonium by its transmutation in reactors, which contributes the enhancement of proliferation resistance. The present paper summarizes analysis of the individual Am and U samples irradiation in Joyo to re-evaluate the results of Pu isotopes in the measure of proliferation resistance, and to combine the results for the prediction of DU-Am irradiation especially in the production of Pu isotopes. By the prediction of DU-Am oxide fuel in fast reactor environment with detail fuel irradiation analysis, it was confirmed that neutron moderation and fuel size affects the produced Pu isotope and its vector due to the very high sensitivity of ²³⁸U resonance capture reaction, the larger diameter fuel is more preferable in the case of moderated neutron spectrum environment for denaturing Pu in fast reactor blanket. Finally proliferation resistance of all the Pu produced in U, Am sample irradiation and DU-Am fuel irradiation prediction were evaluated based on decay heat and spontaneous fission neutron rate, and it was confirmed ²⁴¹Am produces un-attractive Pu to abuse from the beginning to the end of irradiation, and more than 2% of ²⁴¹Am doping is required to enhance the proliferation resistance of Pu to MOX grade and Kessler’s proposal in moderated neutron spectrum environment in fast reactor.     

Research and Development of Minor Actinide-containing Fuel and Target in a Future Integrated Closed Cycle System

Research and development of minor actinide-containing fuels and targets, i.e., (Pu,Am)O₂–MgO, (Pu,Np)O₂–MgO, (U,Pu,Np)O₂, (U,Pu,Np)N and (Pu,Np,Zr)N, for use in a future integrated closed cycle system that includes fast reactor and accelerator driven sub-critical system is underway. The present statuses of fabrication test and property measurements are given. Design concept of the oxide target is described in detail together with a screening of the support material. A new apparatus for the measurement of mechanical properties at the elevated temperature is installed for use in evaluating the fuel-cladding mechanical interaction. Development histories with future prospects of two types of Np-containing fuels for the fast reactor are mentioned. Preliminary test results for a new nitride target for the accelerator driven sub-critical system are given. Finally, an irradiation test plan in the experimental fast reactor JOYO is briefly described.     

Comparative Studies of JENDL-3.3, JENDL-3.2, JEFF-3, JEF-2.2 and ENDF/B-6.8 Data Libraries on the Monte Carlo Continuous Energy Modeling of the Gas Turbine-Modular Helium Reactor Operating with Thorium Fuels

One of the major benefits of the Gas Turbine-Modular Helium Reactor is the capability to operate with several different types of fuel; either Light Water Reactors waste, military plutonium or thorium represent valid candidates as possible types of fuel. In the present studies, we performed a comparison of various nuclear data libraries by the Monte Carlo Continuous Energy Burnup Code MCB applied to the Gas Turbine-Modular Helium Reactor operating on a thorium fuel. A thorium fuel offers valuable attractive advantages: low fuel cost, high reduction of actinides production and the possibility to enable the reactor to act as a breeder of fuel by the neutron capture of fertile ²³²Th. We evaluated the possibility to mix thorium with small quantities, about 3% in atomic composition, of ²³⁹Pu, ²³³U and ²³⁵U. The mass of thorium must be much larger than that one of plutonium or uranium because of the low capture cross section of thorium compared to the fission one of the fissile nuclides; at the same time, the quantity of the fissile isotopes must grant the criticality condition. These two simultaneous constraints force to load a huge mass of fuel in the reactor; consequently, we propose to allocate the fuel in TRISO particles with a large radius of the kernel. For each of the three different fuels we calculated the evolution of the fuel composition by the MCB code equipped with five different nuclear data libraries: JENDL-3.3, JENDL-3.2, JEFF-3, JEF-2.2 and ENDF/B.     

Effect of minor actinides doping on plutonium produced in large-scale FBR blanket

The present study focuses on the effect of minor actinides (MAs) addition into the FBR blanket as ways of increasing fraction of even-mass-number plutonium isotopes, especially ²³⁸Pu, aiming at enhancing the proliferation resistance of plutonium produced in the blanket. The MA loading potential to enhance the proliferation resistance of plutonium is investigated, with considering actual design constraints on the fuel decay heat from the fuel handling and fabrication points of view, as MAs considerably generate decay heat. It reveals that depending on doping quantity of MAs, it is possible to denature produced plutonium by MA transmutation. MA addition in the blanket gives a significant increment in ²³⁸Pu fraction of generated plutonium but less effect on other even-mass-number plutonium isotopes. However, it is important that MA compositions should be adequately controlled to satisfy both the proliferation resistance requirements and the decay heat constraints for fuel handling.     

Feasibility of Reprocessed Uranium in LWR Fuel Cycle for Protected Plutonium Production

Protected plutonium production (PPP) is an intrinsic measure to enhance the proliferation resistance of Pu by raising the ²³⁸Pu isotopic concentration, which denatures Pu on account of the high spontaneous fission neutron (SFN) rate and large decay heat (DH). This study is aimed at examining the feasibility of reprocessed uranium (RepU) with or without the addition of minor actinide (MA) in LWR fuel cycle for PPP and to make a tentative economic assessment of RepU possessing the PPP feature. It was analytically clarified that RepU enriched to 5% ²³⁵U by centrifugation produced denatured Pu at higher burnup than about 40GWd/t. By the addition of more than 0.5% MA to RepU and natural uranium both enriched to 5%, Pu generated in the uranium fuel with MA added could be denatured up to 40 GWd/t at least. A diagram designed with functions of SFN rate and DH explicated the PPP features of re-enriched RepU and enriched natural uranium with or without MA addition. The economic assessment indicated that the cost of fuel cycle applying re-enriched RepU would be comparable to that of the conventional fuel cycle, if the cost of the source RepU is low. In addition, the LWR fuel cycle applying RepU for PPP was discussed.     

Plutonium credit in the low enriched uranium fuel of PARR-1

The amount of plutonium (Pu) isotopes and the resultant savings of ²³⁵U due to their production were calculated in the low enriched uranium (LEU) fuel, being utilized in Pakistan Research Reactor-1 (PARR-1). Further the importance map and relative importance map for different isotopes of Pu were also determined. Equilibrium PARR-1 core was achieved for these calculations. MTR-PC26 package was used to generate the microscopic cross-sections data for 45 elements including fissile/structural materials and also the fission products. Finite difference reactor core analysis code CITATION was employed for the fuel management analysis and static depletion calculations.The results indicated that PARR-1 core has attained its equilibrium state after eleven cycles with each cycle of duration about forty full power (10 MW) days. Further, the results showed that at the beginning of equilibrium cycle (BOEC) of the PARR-1 core, net reactivity addition due to all isotopes of Pu was 4.86 × 10⁻³Δk/k. Amount of ²³⁵U equivalent to this value of reactivity was found to be 15.58 ± 0.021 g. Plots of importance and relative importance maps predicted higher isotopic concentrations of Pu in the fuel elements located in the vicinity of central water box.     

Application of fluoride volatility method to the spent fuel reprocessing

ABSTRACT

An advanced reprocessing system has been developed to treat various SF (spent fuels): spent UO₂ and MOX (mixed oxide) fuels from LWR (light water reactor) and MOX fuel from FR (fast reactor). The system consists of SF fluorination to separate most U (uranium) as volatile UF₆, dissolution of solid residue containing Pu (plutonium), FP (fission products), MA (minor actinides) and partial U by nitric acid, and Pu+U separation from FP and MA by conventional solvent extraction. Gaseous UF₆ is purified by the thermal decomposition and the adsorption of volatile PuF₆ and adsorption of other impurities. This system is a hybrid process of fluoride volatility and solvent extraction and called FLUOREX. Fluorination of most U in the early stage of the reprocessing process is aimed at sharply reducing the amount of SF to be treated in the downstream aqueous steps and directly providing purified UF₆ for the enrichment process without conversion. The FLUOREX can flexibly adjust the Pu/U ratio, rapidly separate UF₆ and economically treat aqueous Pu+U. These features are especially suitable for the transition period fuel cycle from LWR to FR. This paper summarizes the feasibility confirmation results of FLUOREX.     

Short-term irradiation behavior of minor actinide doped uranium plutonium mixed oxide fuels irradiated in an experimental fast reactor

A fuel irradiation program is being conducted using the experimental fast reactor ‘Joyo’. Two short-term irradiation tests in the program were completed in 2006 using a uranium and plutonium mixed oxide fuel which contains minor actinides (MA-MOX fuel). The objective of the tests is the investigation of early thermal behavior of MA-MOX fuel such as fuel restructuring and redistribution of minor actinides. Three fuel pins which contained MA-MOX: 2% neptunium and 2% americium doped uranium plutonium mixed oxide (Am,Pu,Np,U)O_2−x fuel were supplied for testing. The first test was conducted with high-linear heating rate of approximately 430 W cm⁻¹ for only 10 min. After the first test, one fuel pin was removed for examinations. Then the second test was conducted with the remaining two pins at nearly the same linear power for 24 h. In these tests, two oxygen-to-metal molar ratios were used for fuel pellets as a test parameter. Non-destructive and destructive post-irradiation examinations results are discussed with early on the behavior of the fuel during irradiation.     

Minor actinide transmutation in fast reactor metal fuels irradiated for 120 and 360 equivalent full-power days

An irradiation experiment on uranium–plutonium–zirconium (U–Pu–Zr) alloys containing 5 wt% or less minor actinides (MAs) and rare earths was carried out in the Phénix fast reactor. The isotope compositions of the fuel alloys irradiated for 120 and 360 equivalent full-power days (EFPDs) were chemically analyzed by inductively coupled plasma–mass spectrometry after 3.3–5.3 years of cooling. The results of chemical analysis indicated that the discharged burnups of the fuel alloys irradiated for 120 and 360 EFPDs were 2.1–2.5 and 5.3–6.4 at%, respectively. The changes in the isotopic abundances of plutonium, americium, and curium during the irradiation experiment were assessed to discuss the transmutation performance of MA nuclides added to U–Pu–Zr alloy fuel. Multigroup three-dimensional diffusion and burnup calculations accurately predicted the changes in these isotopic abundances after fuel fabrication. An evaluation of the MA transmutation ratio based on the results of chemical analysis revealed that the quantity of MA elements in the U–19Pu–10Zr–5MA (wt%) alloy decreased by about 20% during the irradiation experiment for 360 EFPDs.     

Neutronics and material attractiveness for PWR thorium systems using monte carlo techniques

Thorium (Th) oxide fuel offers a significant advantage over traditional low-enriched uranium and mixed uranium/plutonium oxide (MOX) fuel irradiated in a Light Water Reactor. The benefits of using thorium include the following: 1) unlike depleted uranium, thorium does not produce plutonium, 2) thorium is a more stable fuel material chemically than LEU and may withstand higher burnups, 3) the materials attractiveness of plutonium in Th/Pu fuel at high burnups is lower than in MOX at currently achievable burnups, and 4) thorium is three to four times more abundant than uranium. This paper quantifies the irradiation of thorium fuel in existing Light Water Reactors in terms of: 1) the percentage of plutonium destroyed, 2) reactivity safety parameters, and 3) material attractiveness of the final uranium and plutonium products. The Monte Carlo codes MCNP/X and the linkage code Monteburns were used for the calculations in this document, which is one of the first applications of full core Monte Carlo burnup calculations. Results of reactivity safety parameters are compared to deterministic solutions that are more traditionally used for full core computations.Thorium is fertile and leads to production of the fissile isotope ²³³U, but it must be mixed with enriched uranium or reactor-/weapons-grade plutonium initially to provide power until enough ²³³U builds in. One proposed fuel type, a thorium-plutonium mixture, is advantageous because it would destroy a significant fraction of existing plutonium while avoiding the creation of new plutonium. ²³³U has a lower delayed neutron fraction than ²³⁵U and acts kinetically similar to ²³⁹Pu built in from ²³⁸U. However, as with MOX fuel, some design changes may be required for our current LWR fleet to burn more than one-third a core of Th/Pu fuel and satisfy reactivity safety limits. The calculations performed in this research show that thorium/plutonium fuel can destroy up to 70% of the original plutonium per pass at 47 GWd/MTU, whereas only about 30% can be destroyed using MOX. Additionally, the materials attractiveness of the final plutonium product of irradiated plutonium/thorium fuel is significantly reduced if high burnups (∼94 GWD/MTU) of the fuel can be attained.     

Radial redistribution of actinides in irradiated FR-MOX fuels

The redistributions of neptunium, plutonium and americium during two kinds of short-term irradiation tests for 10 min and 24 h at high linear heating rate around 430 W cm⁻¹ were studied in the uranium and plutonium mixed oxide fuel containing Am and/or Np. It was found in the irradiation test for 24 h that the concentrations of Pu and Am increased toward the central void, but there was no change in the concentration of Np. The obtained experimental redistributions of Am and Pu were analyzed, based on both pore migration and thermal diffusion models. As a result, the calculated redistributions of Pu and Am showed good agreements with the experimentally obtained ones.     

Advanced U–Np–Pu fuel to achieve long-life core in heavy water reactor

The objective of this paper is to look at the possibility of approaching the long-life core comparable with reactor life-time. The main issues are centered on U–Np–Pu fuel in a tight lattice design with heavy water as a coolant. It is found that in a hard neutron spectrum thus obtained, a large fraction of ²³⁸Pu produced by neutron capture in ²³⁷Np not only protects plutonium against uncontrolled proliferation, but substantially contributes in keeping criticality due to improved fissile properties (its capture-to-fission ratio drops below unit). Equilibrium fuel composition demonstrates excellent conversion properties that yield the burn-up value as high as 200 GWd/t at extremely small reactivity swings.