From fuel to fuel: Dissolution, Partitioning and fuel manufacturing - PowerPoint PPT Presentation

From fuel to fuel: Dissolution, Partitioning and fuel manufacturing ASGARD, SACSESS, GENIORS Stéphane.Bourg@cea.fr Christian Ekberg

INTRODUCTION THE 3 PROJECTS EDUCATION AND TRAINING CEA | 10 AVRIL 2012 | PAGE 3

INTRODUCTION CEA | 10 AVRIL 2012 | PAGE 4

Nuclear Energy Today – open fuel cycle Does not preserve natural resource depleted U 430 TWh e (0.2 – 0.5% 235 U) 8300t/a  Natural U is a limited resource Uranium Spent ore Although present everywhere, U-ores of reasonable fuel 1200t/a 1200t/a ~9500t/a economic interest are limited (260$/kg U) (Once-through) Minimum lifespan ~135 years (with current ~9t/a 235 U 56t/a 235 U ~1122t/a 236+238 U consumption 56kt/y) ∆ U ~70t/a 1144t/a 238 U ~14t/a Pu Need for preserving U-resource Efficiency~0.7% ~55t/a FP+AM Rough estimates derived from French Fuel cycle assuming no recycling  Global efficiency is currently very low: ~0.7% 300 Estimated lifespan (years) 250 ~70t from the initial ~9500t Uore 200 150 100  Need for improving U-efficiency 50 0 coal gas oil uranium D irection de l’ E nergie N ucléaire - Marcoule FISA D épartement de Recherche sur les Procédés pour la M ine et le R ecyclage du C ombustible June 2019, Pitesti

Nuclear Energy Today – Once through fuel cycle (French fuel cycle) Spent fuel 9500 t Up to - 15 to 20% of French 0,76% odd Pu 93.0% 238 U 8000 t -20% electricity yearly 0,41% even Pu 0.75% 235 U 1200t 1200t supplied by recycled 0.54% 236 U Uranium ore materials fuel FP 4.55% Depleted 1% 95% - ~1500t uranium ore uranium MOX fuels 4% yearly preserved 10 - 15/a Per 120 m 3 ERU Enriched Rep. U fuels reactor Recycling plants HLW - No significant SNF interim storage  risk reduced La Hague MELOX >2 000tHM of MOX fuel produced >33 000 tHM reprocessed D irection de l’ E nergie N ucléaire - Marcoule FISA 6 D épartement de Recherche sur les Procédés pour la M ine et le R ecyclage du C ombustible June 2019, Pitesti

GEN4 systems with fast neutrons FR MOx (450 t) σ fission / σ capture Fission /capture 6,00 Used MOx REL LWR 5,00 FNR (450 t) RNR FNR Fuel 4,00 3,00 Manufacturing Plutonium (# 70 t) Waste 2,00 1,00 (50 t) Depleted Uranium (U ret # 320 t) Recycling 0,00 U (# 50 t) 238Pu 239Pu 240Pu 241Pu 242Pu plant With fast neutron reactors With thermal reactors 50 Gtoe 1GWe ~ 1GWe ~ COAL GAS 150t U nat /y 1t U nat /y COAL 160 Gtoe 7500 Gtoe OIL 420 Gtoe OIL 230 Gtoe U=6% world energy potential U=90% world energy potential Very significant improvement of natural uranium efficiency D irection de l’ E nergie N ucléaire - Marcoule FISA 7 D épartement de Recherche sur les Procédés pour la M ine et le R ecyclage du C ombustible June 2019, Pitesti

Recycling the minor actinides (transmutation): a potential contribution for decreasing the waste burden 10 4 10000 Relative radiotoxicity  Waste toxicity dominated by MA 10 3 1000 Recycling MA  decrease waste lifetime Radiotoxicité relative 10 2 100 and toxicity 10 10 U-ore 1  Preserve the valuable repository 1 Time 0,1 resource 0,1 10 10 10 2 100 10 3 1000 10 4 10000 100000 1000000 10 5 10 6 Temps (années)  of the heat load   density of the Am recycling repository HLW: 160 ha HLW: 1200 ha With Am recycling, reduction of the Residual heatpower (W/t HM ) repository volume by a factor up to 8 Very significant increase of the repository "lifespan" D irection de l’ E nergie N ucléaire - Marcoule FISA 8 D épartement de Recherche sur les Procédés pour la M ine et le R ecyclage du C ombustible June 2019, Pitesti

Anticipated beneficial impact of recycling activities Actinides recycling significantly improve the nuclear energy environmental footprint Ch. Poinssot, S. Bourg et al., Energy 2014, 6, 199–211 J.Serp, Ch Poinssot, S. Bourg, Energies 2017, 10, 1445. D irection de l’ E nergie N ucléaire - Marcoule FISA 9 D épartement de Recherche sur les Procédés pour la M ine et le R ecyclage du C ombustible June 2019, Pitesti

A significant Improvement of the nuclear waste management Interim storage time: 120 years • Relative decrease of HLW vs. ILW while total volume of waste ~ constant +/- 20% • Decrease of thermal power due to Pu-recycling  significant gain for the repository volume • Decrease of radiotoxicity & lifetime • Am transmutation: save the repository surface by a factor about 3 compared to SFR D irection de l’ E nergie N ucléaire - Marcoule FISA 10 D épartement de Recherche sur les Procédés pour la M ine et le R ecyclage du C ombustible June 2019, Pitesti

GEN IV Fast Neutron Reactors + ADS in Europe MSR MYRRHA Reference fuel: carbide, nitride… Reference fuel: MOX D irection de l’ E nergie N ucléaire - Marcoule FISA 11 D épartement de Recherche sur les Procédés pour la M ine et le R ecyclage du C ombustible June 2019, Pitesti

Potential Future Fuel Cycles DISSOLUTION Specific Reprocessing SEPARATION SEPARATION U, Pu (, MA) MA DISSOLUTION CONVERSION, FABRICATION ADS IRRADIATION FNR D irection de l’ E nergie N ucléaire - Marcoule FISA 12 D épartement de Recherche sur les Procédés pour la M ine et le R ecyclage du C ombustible June 2019, Pitesti

Different separation process options developed worldwide for different fuel cycle strategies But before, we need to dissolve the fuel, and after, we have to re-manufacture it! D irection de l’ E nergie N ucléaire - Marcoule FISA 13 D épartement de Recherche sur les Procédés pour la M ine et le R ecyclage du C ombustible June 2019, Pitesti

ASGARD FROM FUEL TO FUEL NON MOX CEA | 10 AVRIL 2012 | PAGE 14 16 juillet 2019

Christian Ekberg, Stephane Bourg, Eva deVisser-Tynova, Andreas Geist, Frodo Klaassen, Teodora Retegan, Mark Sarsfield and Janne Wallenius D irection de l’ E nergie N ucléaire - Marcoule FISA 15 D épartement de Recherche sur les Procédés pour la M ine et le R ecyclage du C ombustible June 2019, Pitesti

Consortium  Budget: 9365 kEuro (EC 4.9 kEuro)  Duration: 20120101- 20151231 (4 years)  Extended to 20150630 D irection de l’ E nergie N ucléaire - Marcoule FISA D épartement de Recherche sur les Procédés pour la M ine et le R ecyclage du C ombustible June 2019, Pitesti

Rationale of ASGARD  Focus on the behaviour of novel nuclear fuels ranging through production, dissolution, conversion and refabrication  Novel fuels considered are An (Am) bearing oxides, CERMET (Mo- based), CERCER (Mg based)´, nitrides and carbides  Provide extensive training and education concerning handling of nuclear material from the whole fuel D irection de l’ E nergie N ucléaire - Marcoule FISA D épartement de Recherche sur les Procédés pour la M ine et le R ecyclage du C ombustible June 2019, Pitesti

CERMET fuels- Dissolution of Mo PuO 2 /Mo dissolution CeO 2 /Mo dissolution (Pu 0.8 Am 0.2 )O 2 / Mo dissolution  1 and 3 mol/L HNO ₃ and 1 mol/L  CeO 2 /Mo (60/40wt.%) pellets  Irradiated at HFR Petten (HELIOS pin 5) HNO ₃ /0.2 mol/L Fe(NO ₃ ) ₃ , RT dissolved in 20 and 100 mL  2 steps process: 1 mol/L HNO 3 without or with • dissolution of Mo -matrix HNO 3 (8 M)  Mo dissolution – faster with Fe (III) Fe(lll) • dissolution of actinides oxides HF or Ag(II)  Pu (Am) dissolution much slower in  CeO 2 separated from the matrix  Samples taken during dissolution for ICP presence of Fe(III) measurements  PuO 2 could be separated from Mo matrix  Black residue remained – PuO 2 CeO 2 Fresh fuel Irradiated fuel D irection de l’ E nergie N ucléaire - Marcoule FISA D épartement de Recherche sur les Procédés pour la M ine et le R ecyclage du C ombustible June 2019, Pitesti

CERCER fuels- Dissolution of MgO  Experiments in 2.5 mol/L HNO 3 at 30 ºC.  Agitation speed has no effect on dissolution rate, i.e. dissolution rate is surface controlled  The acid volume has no effect on dissolution rate.  A two-stage reaction equation for the dissolution of MgO was postulated based on XRD measurements and literature review.  The dissolution (2 M HNO 3 , RT) of MgO/CeO 2 (60/40 wt.%) – MgO completely dissolved, CeO 2 remained as powder  Actinides can be separated from the magnesia matrix D irection de l’ E nergie N ucléaire - Marcoule FISA D épartement de Recherche sur les Procédés pour la M ine et le R ecyclage du C ombustible June 2019, Pitesti

Conversion from solution to oxide precursors Sol – gel methods Impregnation of solid Photochemical conversion matrixes  Amberlite IRC-86 and Lewatit Two methods  UO 2 , ThO 2 , ThO 2 -UO 2 , CeO 2 , TP-207 resins tested for • Internal gelation Eu 2 O 3 , (Ce,U)O 2 , Eu 2 O 3 -UO 2 fabrication of UO 2 /Nd materials prepared • Complex Sol-Gel Process microspheres  Fuel pellets made  UO 2 /Nd microspheres prepared & characterized  Amberlite IRC-86 successful  processes studied &optimised D irection de l’ E nergie N ucléaire - Marcoule FISA D épartement de Recherche sur les Procédés pour la M ine et le R ecyclage du C ombustible June 2019, Pitesti