Application of CANDLE Burnup to Block-Type High Temperature Gas Cooled Reactor for Incinerating Weapon Grade Plutonium

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1 GENES4/ANP2003, Sep , 2003, Kyoto, JAPAN Paper 1079 Application of CANDLE Burnup to Block-Type High Temperature Gas Cooled Reactor for Incinerating Weapon Grade Plutonium Yasunori Ohoka * and Hiroshi Sekimoto Research Laboratory for Nuclear Reactors, Tokyo Institute of Technology, O-okayama, Meguro-ku, Tokyo , Japan The CANDLE burnup strategy is a new reactor burnup concept, where the distributions of fuel nuclide densities, neutron flux, and power density move with the same constant speed along the core axis from bottom to top (or from top to bottom) of the core and without any change in their shapes. In the present study, the incineration of weapon grade plutonium (93.8%Pu-239) is investigated by applying the CANDLE burnup to the block-type high temperature gas cooled reactor. The natural gadolinium is used as the burnable poison. With the oxide fuel of weapon grade plutonium, natural gadolinium concentration of 27.2% and fuel pin pitch of 10.4cm, the CANDLE burnup is realized with the core average burnup of the heavy metal of 65% (Pu-239 of 89%) and burning region speed of 60cm/year. KEYWORDS: CANDLE burnup, block-type high temperature gas cooled reactor, burnable poison, weapon grade plutonium I. Introduction 1. Pu-burning in Block-type High Temperature Gas Cooled Reactor The disposal method of the weapon grade plutonium of the surplus produced for the purpose of use to the military in the United States and Russia at the time of cold war is currently discussed all over the world 1). It appears that the incineration processing by using the fuel of block-type high temperature gas cooled reactor becomes the high processing characteristic for the safety and the economy from the following features 2) ; (1) Burning of weapon grade plutonium with efficient generation of electric power. In addition, use of waste heat can be performed as a high temperature energy source. (2) The graphite of main structural material of core possesses high heat capacity, slow thermal response and structural stability. (3) The helium of coolant material is inert of chemical reaction and nuclear reaction. (4) The coated fuel particle endures deep burnup, and it is capable of burning up to 90% or more of the initially loaded Pu-239. (5) Due to the usage of the coated fuel particle, the diversion to the other purposes of plutonium is difficult, that is excellent in the resistance of nuclear proliferation. 2. CANDLE Burnup A new burnup strategy CANDLE (Constant Axial shape of Neutron flux, nuclide densities and power shape During Life of Energy producing reactor) is proposed 3). In this burnup strategy, the fission region moves along the core axis from bottom to top (or from top to bottom) of the core as shown in Fig. 1. The reactor core may be divided roughly to three regions; fresh fuel region, burning region and spent fuel region. In the burning region, the fissile material burns and produces neutrons and energy. In the front side of the burning region, the produced neutrons leak to the fresh fuel region, and in the backside of the burning region the fission products (FPs) are accumulated by fission reactions of the fissile materials. Then the fissile materials in the fresh fuel region start the fission reaction, and the fission reaction rate of the burning region finally decreases. By this way, the burning region moves to the fresh fuel region. Start Burnup Finish Fresh fuel region Burning region Spent fuel region Fig. 1 Concept of the CANDLE burnup strategy * Corresponding author, Tel , Fax , yohoka@nr.titech.ac.jp

2 3. Application of CANDLE Burnup to Block-type High Temperature Gas Cooled Reactor In the case of application of CANDLE burnup to high-temperature gas cooled reactor, the burnable poison is used 4) as shown in Fig. 2. The initial fuel is adjusted to the sub-criticality by the burnable poison. If this region goes into a burning region, the burnable poison burns up in a much shorter time, and then the fissile material starts the fission reaction. The distribution of each nuclides density in the upper part of the core is axially uniform, but it is complicated in the burning region. It may be difficult to construct the ignition region for this burnup strategy. However, the setup of the succeeding core configuration is very easy. The burning region at the end of reactor life can be used as the ignition region of the succeeding core as shown in Fig. 3. Since this reactor core consists of block fuels, this refueling strategy can be easily employed. The CANDLE burnup strategy has the following general merits; (1) Burnup reactivity control mechanism is not required, because the excess burnup reactivity becomes zero. (2) Reactor characteristics do not change with burnup. The estimation of core condition becomes very easy and reliable. Therefore, the reactor operation becomes simple. (3) The reactor core height is proportional to a reactor core life. Therefore, design of long-life reactor core becomes easier. (4) Infinite neutron multiplication factor of fresh fuel is less than unity. Therefore, the risk for criticality accident is small. The transportation and storage of fresh fuels become simple and safe. Neutron flux Burnup region move direction (axial direction) BP Fissile FP Neutron flux Burnup BP Fissile BP: Burnable poison, FP: Fission Products Fig. 2 Distribution of neutron flux and each nuclide densities of CANDLE burnup strategy at high temperature gas cooled reactor FP Fresh fuel charge Burnup Spent fuel discharge Fresh fuel region Burning region Spent fuel region Fig. 3 Concept of the CANDLE burnup and refueling strategy The reactor that has merits of both the CANDLE burnup strategy and the high temperature gas cooled reactor is attractive. In the present work, the feasibility of such a reactor core is investigated, and try to make high burnup of Pu-239 is by changing core parameters. II. Calculation Scheme and Conditions The CANDLE burnup for the block-type high temperature gas cooled reactor was analyzed using the steady state CANDLE burnup analysis code system. The steady state is the state where time has fully passed from the ignition, and the CANDLE condition is satisfied in the strict meaning. The burning region moving speed, distributions of the nuclide density, neutron flux, and power density are obtained by solving the simultaneous equations of nuclides burnup and neutron diffusion. In the CANDLE burnup strategy, the burnup equation takes into account the movement of burning region. In this analysis, the calculation method is similar to the PREC method 5) that is developed for analysis of the pebble-bed reactor. This is the method of moving viewpoint on the burning region. The detailed description is given in the reference 3,4). The cell calculation employs a double heterogeneity model for treating TRISO coated fuel particles. In the present analysis, the cell calculation is performed for the fuel cell like the HTTR of JAERI 6). This fuel cell geometry is shown in Fig. 4. The fuel compact region consists of TRISO coated fuel particle and graphite matrix, which is treated as the micro heterogeneity cell. The cell calculation is performed using the collision probability routine of SRAC code system 7) with JENDL-3.2 nuclear data library 8).

3 Pitch Low Density PyC High Density PyC SiC Kernel He Fig. 4 Fuel Cell Model Fuel compact Graphite sleeve Cooled material, He Graphite block The design parameters of the analyzed reactor core are shown in Table 1. A cylindrical core (r-z coordinate system) is considered. Setting the core height to infinity is impossible in the actual calculation, so it is set at 800cm. The z=800cm side is for the spent fuel region, and the z=0cm side is for the fresh fuel region. The energy group structure is shown in Table 2. The natural gadolinium is used as the burnable poison whose isotope composition fraction is shown in Table 3. Only 155 Gd and 157 Gd are effective as the burnable poison, but 154 Gd, 155 Gd, 156 Gd, 157 Gd and 158 Gd are included in the burnup chain as shown in Fig. 5. This chain is a part of the fission products chain. Table 1 Design Parameters Thermal power [MW th ] 30 Coated fuel particle TRISO coated PuO 2 fuel particle Kernel / particle diameter [mm] / Coating material thickness [mm] density [g/cm 3 ] PyC / PyC / SiC / PyC / / / / / / Packing fraction [%] 30.0 Compact inner /outer diameter [cm] 1.00 / 2.60 Sleeve outer diameter / block inner diameter [cm] 3.40 / 4.10 Core diameter / height [cm] 400 / 800 Radial reflector thickness [cm] 50 Table 2 Neutron Energy Group Structure Group number Upper Energy [ev] Lower 1 Fast E E+05 2 Slowdown E E+01 3 Resonance E E+00 4 Thermal E E-05 Table 3 Isotope Composition Fraction of Natural Gadolinium Isotope Composition Fraction [%] fission 153 Eu 154 Eu 155 Eu 156 Eu (n, γ) 154 Gd 155 Gd 156 Gd 157 Gd 158 Gd β decay Fig. 5 Gadolinium nuclides in the FP burnup chain

4 III. Calculation Results and Discussions concentration, when the pitch increases, the neutron At application of the CANDLE burnup to the high spectrum becomes softer, but the fuel material becomes temperature gas cooled reactor, the thermal absorption cross diluter gradually. Therefore, the effective neutron section of burnable poison nuclides is important. If the microscopic cross section is too small, the fresh fuel region is critical, or the core is sub-critical. Therefore, the neutron flux distribution on reactor core axis is too wide. And if the cross section is larger, the burnup of spent fuel is higher 4). multiplication factor increases until the pitch of 10.6cm, and then decreases. At the natural gadolinium concentration of 27.2%, the peak value of multiplication factor becomes just unity. If the concentration becomes more than it, the multiplication factor becomes less than unity for any pitch. The condition that the core is critical and that the Pu-239 burnup of spent fuel is as large as possible is investigated by changing parameters such as the burnable poison concentration and the fuel cell pitch. The change of the effective neutron multiplication factor for different the fuel cell pitch at each natural gadolinium concentrations is shown in Fig. 6, where the effective multiplication factor is shown only near unity. At each The relation between the Pu-239 core average burnup, the burning region move speed and the fuel cell pitch is shown in Fig. 7, where the gadolinium concentration is adjusted to make the effective neutron multiplication factor unity. When the pitch is wider, the speed becomes faster. The maximum value of Pu-239 burnup of core central part 98.1% and core average 86.2% are obtained at pitch of 10.4cm and gadolinium concentration of 27.2%. k eff Gd 24.0% Gd 25.0% Gd 26.0% Gd 27.1% Gd 27.2% Gd 27.3% Gd 27.0% Pitch [cm] Fig. 6 Relation between the pitch and the effective neutron multiplication factor (k eff ) in each concentration 239 Pu Burnup [%- 239 Pu] % % Burnup 26.9% % % % Speed % % Pitch (k eff = 1) [cm] Speed [cm/year] Fig. 7 Relation between the Pu-239 bunrup, the burning region move speed and the pitch in each concentration at k eff =1

5 Table 4 Effects of different reflector thickness Refrector thicknesss [cm] Effective neutron multiplication factor Burning region move speed [cm/year] Heavy metal average burnup [%(HM)] Pu-239 Central part Burnup [%] Core average Pu Burnup [%- 239 Pu] reflector thickness 50cm 60cm 70cm 80cm 90cm 100cm 50cm 100cm r [cm] Fig. 8 Pu-239 burnup distributions for reflector thickness (on the reactor core radius) In addition, the radial reflector thickness is increased every 10cm for the purpose of the big difference between core central part and core average of Pu-239 burnup is smaller. The analysis result is shown in Table 4 and the radial direction distribution of Pu-239 burnup is shown in Fig. 8. The burnup at the reflector boundary are increased by the reflector effect, and the core average burnup is increased gradually with increasing the reflector thickness. Furthermore rise of the Pu-239 burnup, the core radius is decreased every 5cm at the radial reflector thickness of 100cm. The analysis result is shown in Table 5 and the radial direction distribution of Pu-239 burnup is shown in Fig. 9. The core average burnup becomes larger with decreasing the core radius, but the effective neutron multiplication factor becomes smaller. At the radius of less than 180cm, the core becomes sub-critical. At the radius of 185cm, the Pu-239 core average burnup attains about 89.1% under the criticality condition. Table 5 Effects of different core radius at reflector thickness of 100cm Core radius [cm] Effective neutron multiplication factor Burning region move speed [cm/year] Heavy metal average burnup [%(HM)] Pu-239 Burnup Central part [%(Pu-239)] Core average

6 Pu Burnup [%- 239 Pu] core radius 180cm 185cm 190cm 195cm 200cm 180cm 200cm r [cm] Fig. 9 Pu-239 burnup distributions for core radius (on the reactor core radius) At this condition, core radius of 185cm, radial reflector thickness of 100cm, natural gadolinium concentration of 27.2% and pitch of 10.4cm, the infinite neutron multiplication factor and the neutron flux distributions are shown in Figs. 10 and 11, respectively. For either figure the horizontal axes denotes the axial position, where the z=0cm side is for the fresh fuel region and the z=800cm side is for the spent fuel region. Fig. 10 shows that the infinite multiplication factor is less than unity in both fresh fuel and spent fuel region, but more than unity in the burning region. Fig. 11 shows that the flux distribution has a sharp peak in the burning region and negligibly small in the other regions. Hence, the CANDLE burnup strategy can be considered to be established for the present design of the high temperature gas cooled reactor k inf z [cm] r [cm] Fig. 10 Infinite neutron multiplication factor distribution

7 8.E+13 7.E+13 Neutron flux [cm -2 s -1 ] 6.E+13 5.E+13 4.E+13 3.E+13 2.E+13 1.E+13 0.E z [cm] r [cm] Fig. 11 Neutron flux distribution Nuclide density [cm -3 ] 1.E+21 1.E+20 1.E+19 1.E+18 1.E+17 1.E+16 8.E+13 Neutoron flux FP(include Gd) Pu-239 Gd-157 Pu-240 Pu-241 Burnup 0.E z [cm] Fig. 12 Distribution of neutron flux and each nuclide densities on the reactor core axis 6.E+13 4.E+13 2.E+13 Neutron flux [cm -2 s -1 ] The distribution of the neutron flux and each nuclides densities on the reactor core axis are shown in Fig. 12. The left-hand axis denotes the nuclide densities in logarithmic scale, and right-hand axis denotes the neutron flux distribution in linear scale. As mention above, FP exists from the fresh fuel region, since some gadolinium nuclides are included in FP nuclides. When the neutron flux becomes higher, Gd-157 will decrease by absorption for a short time. After then, the number density of Pu-239 decreases and Pu-240, 241 and FP increases by the nuclear reaction of Pu-239. IV. Conclusion In this study, the incineration performance of weapon grade plutonium for the block-type high temperature gas cooled reactor is investigated by applying the CANDLE burnup. The obtained results are shown in the followings: (1) The feasibility is confirmed by using the natural gadolinium as the burnable poison and adjusting its concentration and the cell pitch. (2) For increasing burnable poison concentration, the spent fuel burnup of Pu-239 increases. However, if the concentration becomes too high, the reactor core becomes sub-critical.

8 (3) The burnup of Pu-239 can be raised by adjusting the reflector thickness and core radius. With natural gadolinium concentration of 27.2%, fuel pin pitch of 10.4cm, core radius of 185cm and reflector thickness of 100cm, the core average burnup of the Pu-239 reaches about 89%. The feasibility of the CANDLE burnup to the weapon grade plutonium fueled block-type high temperature gas cooled reactor is investigated, and this strategy was appeared to be effective for the incineration process of weapon grade plutonium. Acknowledgment The present study is supported partly by the JAERI s Nuclear Research Promotion Program. References 1) E. R. Merz and C. E. Walter, Advanced Nuclear Systems Consuming Excess Plutonium; NATO ASI Series, Partnership Sub-Series, 1. Disarment Technologies, Kluwer Academic Publishers, Netherland, 1(1997) 2) A. I. Kiryushin, N. G. kodochigov, N. G. kouzakov, Project of the GT-MHR high-temperature helium reactor with gas turbine, Nucl. Eng. Design., 173, 119(1997) 3) H. Sekimoto, K. Ryu and Y. Yoshimura, A New Burnup Strategy CANDLE, Nucl. Sci. Engin., 139, 306(2001). 4) Y. Ohoka and H. Sekimoto, Application of CANDLE Burnup to Block-type high Temperature Gas Cooled Reactor, Proc. Int. Conf. On Nucl. Engin., Tokyo, Japan, April 20-23, 2003, ICONE (2003). 5) H. Sekimoto, T. Obara, S. Yukinori, et al., New Method to Analyze Equilibrium Cycle of Pebble-Bed Reactors,, J. Nucl. Sci. Technol., 24, 765(1987). 6) K. Yamashita, R. Shindo, I. Murata, et al., Nuclear Design of the High-Temperature Engineering Test Reactor (HTTR), Nucl. Sci. Engin., 22, 212 (1996). 7) K. Okumura, K. Kaneko and K. Tsuchihashi, SRAC95; General Purpose Neutronics Code System, JAERI-Data/Code , Japan Atomic Energy Research Institute (JAERI), (1998). 8) T. Nakagawa, K. Shibata, S. Chiba, et al., Japanese Evaluated Nuclear Data Library Version 3 Revision-2: JENDLE-3.2, J. Nucl. Sci. Technol., 32, 1259 (1995).

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