Effects of Water Vapor on Tritium Release Behavior from Solid Breeder Materials

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1 Effects of Water Vapor on Tritium Release Behavior from Solid Breeder Materials T. Kinjyo a), M. Nishikawa a), S. Fukada b), M. Enoeda c), N. Yamashita a), T. Koyama a) a) Graduate School of Engineering Science, Kyushu University, Fukuoka , Japan b) Department of Applied Quantum Physics and Nuclear Engineering, Kyushu University, Fukuoka , Japan c) Naka Establishment, Japan Atomic Energy Agency, Ibaraki , Japan ABSTRACT Tritium release model was developed by present authors. Tritium diffusion in bulk of grain, transfer at interfacial layer of grain, surface reactions such as water adsorption/desorption, isotope exchange reaction with hydrogen in gas phase, isotope exchange reaction with water vapor in gas phase and water generation reaction were considered in the tritium release model. Tritium release curves estimated by the tritium release model gave good agreements with experimental curves under humid condition obtained at Japan Atomic Energy Agency (JAEA) and it became clear that water in gas phase or on grain surface affects tritium release behavior from solid breeder materials. In this study the tritium release behavior under humid, dry or dry purge gas with hydrogen condition is discussed considering effect of water vapor in gas phase or on grain surface, and chemical form of release tritium is evaluated with experimental data obtained at JAEA. Finally tritium release behavior under various conditions is estimated assuming ITER-TBM conditions designed by JAEA or commercial reactor. Corresponding Author: Tomohiro Kinjyo Graduate School of Engineering Science, Kyushu University Hakozaki 6-1-1, Higashi-ku Fukuoka city, Fukuoka, , Japan Tel: , Fax: Address:

2 Introduction Tritium release model considering tritium migration in bulk of crystal grain, in interfacial layer or reactions between grain surface and gas phase has been developed by present authors. Estimation of tritium release behavior from various solid breeder materials under humid purge gas condition was done by the model and it gave good agreement with experimental data [1]. To control of water vapor in is too difficult especially less than several Pa order. It will be impossible to get out water vapor from perfectly, and several Pa of water vapor exists in called as dry. By the way, some of water vapor is generated by water formation reaction in case solid breeder material is located in dry purge gas with hydrogen at above 6 o C. The water formation reaction was reported previously [2]. The water vapor in might give large effects to tritium release behavior from solid breeder materials, such as tritium release rate from solid breeder materials, chemical form of released tritium or tritium inventory in solid breeder materials, because concentration of released tritium under out-pile experiment condition carried out in this study or ITER-TBM condition is smaller than water vapor mixed in. In this study, the effects of water vapor on tritium release behavior is evaluated by out-pile tritium release experiment or numerical calculation using the tritium release model developed by present authors. Experiment Drying operation to get rid of surface water from solid breeder materials: The Li 4 SiO 4 (Forschungszentrum Karlsruhe, FzK), TiO 3 (France Atomic Energy Commission, CEA or Kawasaki Heavy Industry, KHI), ZrO 3 (Mitsubishi Atomic Power Industry, MAPI (now Mitsubishi Heavy Industry, MHI)) or LiAlO 2 (Japan Atomic Energy Agency, JAEA) pebbles located in quartz tube were heated from room temperature to 8 C and the temperature was kept at 8 C for 8 hours in dry He atmosphere. Neutron irradiation: Pebbles of Li 4 SiO 4, TiO 3, ZrO 3 or LiAlO 2 were irradiated by the thermal neutron at the Japan Research Reactor 4 (JRR-4) in JAEA under the conditions of He atmosphere. The neutron flux was 4.E13 cm -2 s -1 and irradiation time was 1 min. Tritium release experiment: Release curves of bred tritium from pebbles of breeder material pebbles were obtained applying the out-pile temperature programmed desorption (TPD) techniques. Details of Experimental apparatus and experimental methods were explained in the previous paper [3]. Results and discussion Figure 1 shows estimated tritium release curves with experimental data obtained under 1, Pa, 1 Pa or 1 Pa of humid condition. Estimated tritium release curve under

3 1, Pa or 1 Pa of water vapor condition gave a good agreement with experimental data but Estimated tritium release curve under 1 Pa of water vapor condition did not give a good agreement with experimental data. It was possible that more than 1 Pa of water vapor existed in set up as 1 Pa of water vapor condition. Several Pa of water vapor initially exists in gas vessels and the water vapor is got out by cold trap including molecular sieve 5A at C to get dry, but several Pa of water vapor must be remained in purge gas after getting through the cold trap. It is too difficult to control partial pressure of water vapor in especially low partial pressure condition. Figure 2 shows the estimated tritium release curves with experimental data obtained as dry condition. The estimated release curves gave a good agreement with experimental curve when partial pressure of water vapor in was assumed to be around 1 Pa. Figure 3 shows the estimated tritium release curves with experimental data from Li 4 SiO 4 obtained as dry with 1, Pa of hydrogen condition. The estimated release curves gave a good agreement with experimental curve when partial pressure of water vapor in purge gas was assumed to be 1 Pa. When hydrogen is added to the, water vapor is generated by water formation reaction above 7 C. Therefore there are two types of water vapor in the when hydrogen is added to the, one is back ground water exists in gas vessels initially, another is the water vapor generated by water formation reaction. The water vapor will accelerate isotope exchange reaction between tritium in surface water on grain surface and water in gas phase, and tritium released gas phase as water form is increased. Even though hydrogen is added to the, two chemical form of tritium are released to. Tritium release behavior including decision of chemical form under various condition in the out-pile experiment carried out present authors can be explained by the tritium release model developed by present authors as a basic step. Then tritium release behavior under ITER-TBM condition designed by Japan Atomic Energy Agency is estimated using the model. Simplified TBM model is shown in figure 4. Purge gas flow rate in breeder layer closer to plasma is set to be 27.3 L/min. and flow is assumed to be plug flow for simplification of numerical calculation. Temperature of the breeder layer is heated from 32 C to 95 C with neutron irradiation, and the neutron irradiation condition is 4 sec. irradiation and 14 sec. break time. Tritium inventory in the breeder layer closer to plasma packing TiO 3 pebbles is estimated as figure 5. Tritium inventory in bulk of grain is much smaller then that in interfacial layer or in surface water. Tritium inventory in LiAlO 2 bed is estimated as figure 6. The tritium diffusivity of LiAlO 2 is the smallest among the solid breeder candidates but tritium inventory in bulk of grain is smaller then that in interfacial layer or in surface water. This result indicates that tritium diffusivity in bulk of grain does not give large effect to tritium inventory in TBM. On the other hand, increasing of grain diameter might be effective to

4 decrease tritium inventory in TBM because of decreasing of tritium inventory in interfacial layer or in surface water. Figure 7 shows chemical form of released tritium from TiO 3 under ITER-TBM condition. Large amount of water vapor generated by water formation reaction is mixed to dry even though perfect dry is introduced to TBM when hydrogen is added to the dry. According to the mixing of water vapor, much amount of tritium is released to gas phase as water form. If it is preferred to recover tritium as hydrogen form, suitable recovery system must be considered which can deal with HT and HTO. Figure 8 shows tritium inventory in TiO 3 bed under humid condition. Steady state is gotten rapidly compared with that under dry with hydrogen condition because isotope exchange reaction 2 with water vapor is faster than isotope exchange reaction 1 with hydrogen between neutron shots. The tritium inventory in surface water is smaller than that under dry with hydrogen condition. To select humid might be effective to reduce tritium inventory in solid breeder bed, to unify chemical form of released tritium in gas phase and to accelerate tritium release rate to gas phase. Figure 9 shows estimated tritium release curves with water vapor in generated by water formation reaction from various candidates under dry with 1 Pa hydrogen condition assuming commercial reactor condition. Temperature of breeder materials is set to be 1, K. Partial pressure of water vapor in from Li 4 SiO 4 or LiAlO 2 decreases with operation time and ratio of released HT from Li 4 SiO 4 or LiAlO 2 increases, but ratio of released HT from TiO 3 does not change until 3 hours. The cause is as follows, the capacity of water formation reaction for TiO 3 is the largest among the solid breeder candidates and mass transfer coefficient of isotope exchange reaction 1 with hydrogen decreases above 4 C [4, 5]. By the way, time getting steady state of tritium release is about 1 hours for TiO 3, 16 hours for Li 4 SiO 4 or 3 hours for LiAlO 2. If period using breeder materials in commercial reactor is several months or a year, difference of the time getting steady state is not serious problem. With this concept LiAlO 2 might be good materials for solid breeder material because the capacity of water formation reaction is the smallest among the candidates and stability of grain surface under hydrogen atmosphere above 6 C is comparatively better than other candidates. Conclusion The tritium release behavior was estimated using model developed by present authors. To control partial pressure of water vapor in is important to unify chemical form of released tritium. Tritium release behavior might be affected by the water vapor in. Because concentration of released tritium to is smaller than partial pressure of water

5 vapor mixed in by water formation reaction. (T2 conc. is about.1 Pa under Kyushu-U experiment condition, or 1 Pa under ITER-TBM condition.) The tritium release behavior under ITER-TBM condition was estimated in this study. It was estimated that some amount of tritium might be released as water form even though hydrogen was added to the dry. If humid is selected as, chemical form of released tritium is unified and we might get steady state of tritium release faster than that under dry with hydrogen condition. References [1] T. Kinjyo, M. Nishikawa, T. Tanifuji, M. Enoeda, Introduction of tritium release step at surface layer of breeder grain for modeling of tritium release behavior from solid breeder materials, Fusion Eng. Des., 81 (26) [2] Y. Kawamura, M. Nishikawa, T. Shiraishi, K. Okuno, Formation of water in lithium ceramics bed at hydrogen addition to, J. Nucl. Mater., 23 (1996) [3] T. Kinjyo, M. Nishikawa, Tritium release behavior from Li 4 SiO 4, Fusion Sci. and Technol., 46 (24) [4] T. Kawagoe, M. Nishikawa, A. Baba, S. Beloglazov, Surface inventory of tritium on TiO 3, J. Nucl. Mater., 297 (21) [5] K. Hashimoto, M. Nishikawa, N. Nakashima, S. Beloglazov, M. Enoeda, Tritium inventory in TiO 3 blanket, Fusion. Eng. Des., (22) [6] T. Kinjyo, M. Nishikawa, M. Enoeda and S. Fukada, Tritium diffusivity in crystal grain of TiO 3 and tritium release behavior under several conditions, Fusion Eng. Des., in press.

6 Tritium concentration [µci/cc] Li 4 SiO 4 (FzK).2 [g] 1, Pa H 2 O/N 2 1 Pa H 2 O/N 2 1 Pa H 2 O/N 2 Temperature Pa H 2 O/N Temperature [ C] Time [hour] Figure 1 Tritium release curves in case partial pressure of water vapor is changed Tritium concentration [ µci/cc] Dry N 2 in JAERI experiment TiO 3 (CEA) Li 4 SiO 4 (FzK) Temperature ZrO 3 (MAPI) LiAlO 2 (JAERI) Temperature [ C] Time [hour] Figure 2 Estimated tritium release curves with experimental data obtained as dry condition

7 Tritium concentration [µci/cc].2.1 Tritium supply to interfacial layer Temperature Li 4 SiO 4 (FzK).1 g 1, Pa H 2 and 1 Pa H 2 O/N Temperature [ C] Time [hour] Figure 3 Estimated tritium release curve with experimental data obtained as dry with hydrogen condition Neutron flux 27.3 [L/min] First breeder layer Out put in A = 9.E-3 [m 2 ] V = 11.9E-3 [m 3 ] out V = 22.8E-3 [m 3 ] 52.7 [L/min] 25.4 [L/min] Second breeder layer Tritium generation rate First layer 17.E-6 [mol/m 3 sec] 133 A = 17.2E-3 [m 2 ] Second layer 8.3E-6 [mol/m 3 sec] T 2 partial pressure 1 [Pa] Purge gas flow rate First layer 27.3 [L/min] Second layer 25.4 [L/min] Linear velocity First layer 5.5 [cm/sec] Second layer 2.45 [cm/sec] Figure 4 Simplified ITER test blanket module designed by Japan Atomic Energy Agency

8 Tritium inventory [mol], or [mol/sec] TiO kg Bed length 133 mm Flow rate 27.3 L/min 1Pa (1,ppm) H 2 and T in surface water [mol] Pa (ppm) H 2 O in He T in interfacial layer [mol] T in bulk [mol] T to [mol/sec] T from bulk to interface [mol/sec] Time [second] 6.x1-7 5.x1-7 4.x1-7 3.x1-7 2.x1-7 1.x1-7 Figure 5 Estimated tritium inventory in TiO 3 under dry with 1 Pa hydrogen condition Tritium supply to interfacial layer [mol/sec] Tritium inventory [mol], or [mol/sec] 1 2 LiAlO kg 1 Bed length 133 mm Flow rate 27.3 L/min 1Pa (1,ppm) H 2 and T in surface water [mol] Pa (ppm) H 2 O in He T in interfacial layer [mol] T in bulk [mol] T to [mol/sec] T from bulk to interface [mol/sec] Time [second] 6.x1-7 5.x1-7 4.x1-7 3.x1-7 2.x1-7 1.x1-7 Figure 6 Estimated tritium inventory in LiAlO 2 under dry with 1 Pa hydrogen condition Tritium supply to interfacial layer [mol/sec]

9 Tritium concentration [µci/cc] 4 2 TiO kg Bed length 133 mm Flow rate 27.3 L/min 1Pa (1,ppm) H 2 and Pa (ppm) H 2 O in He Time [second] Released tritium in gas phase Released as HT Amount of HT + HTO Patrial pressure of H 2 O in Partial pressure of H 2 O in gas phase [Pa] Figure 7 Estimated chemical form of released tritium from TiO 3 under dry purge gas with 1 Pa hydrogen condition Tritium inventory [mol], or [mol/sec] TiO kg Bed length 133 mm Flow rate 27.3 L/min Pa (ppm) H 2 and 1Pa (1,ppm) H 2 O in He T in bulk [mol] T in surface water [mol] T in interfacial layer [mol] T to [mol/sec] T from bulk to interface [mol/sec] Time [second] 6.x1-7 5.x1-7 4.x1-7 3.x1-7 2.x1-7 1.x1-7 Figure 8 Estimated tritium inventory in TiO 3 under dry with 1 Pa water vapor condition Tritium supply to interfacial layer [mol/sec]

10 Tritium concentration [µci/cc] Commercial reactor condition Bed length 133 mm, Flow rate 27.3 L/min Temperature 1 K 1 Pa (1,ppm) H 2 and Pa (ppm) H 2 O in N 2 TiO 3HT Time [hour] Li 4 SiO 4HT LiAlO 2HT HT + HTO H 2 O HT + HTO H 2 O HT + HTO H 2 O Partial pressure of H 2 O in gas phase [Pa] Figure 9 Estimated tritium release curves under dry with 1 Pa hydrogen condition assuming commercial reactor

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