Analogies of experience in the United States Transuranium Element Production Program with partitioning and transmutation of transuranic actinides in commercial used fuels Abstract ACTINIDE AND FISSION PRODUCT PARTITIONING AND TRANSMUTATION, ISBN 978-92-64-99174-3, OECD 212 1
Introduction Figure 1: Vision of a unified heavy element production programme Vision of a Unified Heavy Element Production Programme The field of new transuraniumelements is entering an era where the participating scientists in this country cannot go much further without some unified national effort which can only be authorised and co-ordinated by the Atomic Energy Commission itself. The future progress in this area depends on substantial weighable quantities (say milligrams) of berkelium, californium and einsteinium. The acquiring of this depends upon our country s entrance into a two-fold programme. The irradiation of substantial quantities of 239 as reactor fuel element, and the reirradiation of the products to form hundred gram amounts of 244 and higher curium isotopes The irradiation of the curium in the suggested very high flux reactor. Z 94 93 Np N G.T. Seaborg Berkeley, 24 October 1957 96 95 Np 237 Am 242 98 97 Bk 238 239 24 241 242 243 244, ( n,f) Np 238 99 Fm Am 241 Am 242 Am 243 Am 244 Am 245 Am 246 Es 249 25 251 252 253 254 Bk 249 243 244 245 246 247 248 249 25 245 246 Bk 25 Bk251, ( n,f), (n,f), (n,f), SF - SF -, EC - - - -, (n,f) - - - Fm 254 Fm 255 Fm 256 Es 253 Es 254 Es 255, -, EC -, (n,f), (n,f), SF -, ( n,f) - - - SF SF Fm 257 Transplutonium element yields Heavy element production 2 ACTINIDE AND FISSION PRODUCT PARTITIONING AND TRANSMUTATION, ISBN 978-92-64-99174-3, OECD 212
Figure 2: Transplutonium-element yield and fission loss during thermal neutron irradiation of plutonium 239 36% 24 241 1% 26% 242 243 243 Am 244 Am 244 246 248 249 Bk 25 252 245 247 249 25 Bk 251.3% 8.5% 1.5%.8%.4% 64% 239 242 244 252 242 244 252 257 Fm 3n, 9% fission loss 2n, ~1% fission loss 8n, ~8.7% fission/decay loss 5n, ~.3% fission/decay loss Figure 3: Heavy element production for DOE research programmes and 252 neutron sources Recycle - Am - Feed Material 242, 243 Am, Target Preparation Reactor Irradiation Hot Cell Separations Product Shipment SRS REDC HFIR 1 st Campaign in 1967.34 mg 5.6 mg 14 µg 249 Bk Product 252 Product 253 Es Product Recent Campaign in 23 45 mg 35 mg 1.7 mg Bk ( 249 Bk) ( 252 ) Es ( 253 Es, 254 Es) Fm ( 257 Fm) 249 Bk 253 252 255 Es 249 253 Es 248 255 Fm ACTINIDE AND FISSION PRODUCT PARTITIONING AND TRANSMUTATION, ISBN 978-92-64-99174-3, OECD 212 3
/Absorption Figure 4: Production rate for 252 252 Produced (mg/8 g Target) 1 2 1 1 1 1-1 1-2 1-3 Heavy Curium Target (22% 244, 51% 246, 11% 248 ) 244 Target 243 Am Target 242 Target 1-4 1 2 3 4 5 6 7 8 9 1 11 12 13 14 15 HFIR Irradiation Cycles (23 d per cycle) Comparison of actinide consumption in thermal and fast spectrum irradiations Figure 5: Comparison of fission versus absorption in a pressurised water reactor (PWR) and a sodium fast reactor (SFR) DOE Spent Nuclear Fuel Recycling Program Plan March 26 1..9.8 PWR SFR.7.6.5.4.3.2.1 U235 U238 Np237 238 239 24 241 242 Am241 Am243 244 4 ACTINIDE AND FISSION PRODUCT PARTITIONING AND TRANSMUTATION, ISBN 978-92-64-99174-3, OECD 212
Figure 6: Transplutonium-element yield and fission loss during irradiation of plutonium Thermal Neutron Irradiation 239 24 241 242 243 243 Am 244 Am 244 245 246 247 248 249 249 Bk 25 Bk 25 251 252 1% 8.5% 1.5%.3% 36% 26%.8%.4% 64% Fast Neutron Irradiation 239 24 241 242 243 Am 244 245 246 247 2.2% 1.4%.8%.12%.6% 23% 14% 9% 11.8%.8%.6%.7%.6% 77% Actinide partitioning-transmutation modelling studies ACTINIDE AND FISSION PRODUCT PARTITIONING AND TRANSMUTATION, ISBN 978-92-64-99174-3, OECD 212 5
Figure 7: Transplutonium-element yield and fission loss during irradiation of 242 TRU Actinide Yield and Loss During Thermal Neutron Irradiation of 242 242 243 Am 244 245 246 247 12% 7% 5% ~% ~% 92% 8% 8% 242 TRU Actinide Yield and Loss During Fast Neutron Irradiation of 242 243 Am 244 245 246 247 5% 2.5% 34% 65% 58% 2.5% 29% 7% 24% 35% Figures 8(a) and 8(b): P-T scenarios evaluated U to Re-enrichment FR Used Fuel LWR UO 2 Used Fuel 3-4 y Cooled 2 MT/y Separations U-TRU-Zr Fuel Fab Fast Reactor Irradiation ~3 y Low Heat FP Waste to Repository Irradiated MA Target Storage MOX Used Fuel Storage U to Re-enrichment U--Np MOX Fuel Fab LWR Irradiation 4.5-6 y LWR UO 2 Used Fuel 3-4 y Cooled 2 MT/y Separations Low Heat FP Wastes to Repository U-Am- Targets LWR Irradiation 4.5-6 y 6 ACTINIDE AND FISSION PRODUCT PARTITIONING AND TRANSMUTATION, ISBN 978-92-64-99174-3, OECD 212
Total Destruction (%) Figure 9: Burn-up of TRU actinides in one P-T cycle irradiation 9 9 9 8 8 8 7 6 5 4 3 Total 241 Am Destruction (%) 7 6 5 4 3 241 Am 237 Np Destruction (%) 7 6 5 4 3 237 Np 2 2 2 1 1 1 Core Burn-up (%) Core Burn-up (%) Core Burn-up (%) 241 Am 242 Am 242 242 238 239 Summary ACTINIDE AND FISSION PRODUCT PARTITIONING AND TRANSMUTATION, ISBN 978-92-64-99174-3, OECD 212 7
Quantit y (MT/year) Quantit y (MT/year) Quantit y (MT/year) Figure 1: Comparison of total TRU and element inventories in the total recycle from each cycle during multiple P-T cycles 7 6 LWR, 3-Year Decay Total TRUs 7 6 FR.25CR, 5 -Year Decay Total TRUs 7 6 -Np in FR/.25CR Am- in LWR, 5 -Year Decay Total TRUs 5 4 5 4 5 4 3 3 3 2 2 2 1 Am Np 1 2 3 4 5 P -T Cycle Number 1 Am Np 1 2 3 4 5 P -T Cycle Number 1 Am Np 1 2 3 4 5 P -T Cycle Number References 8 ACTINIDE AND FISSION PRODUCT PARTITIONING AND TRANSMUTATION, ISBN 978-92-64-99174-3, OECD 212