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Actinide Transmutation in Nuclear Reactors

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Actinide Transmutation in Nuclear Reactors JAMÜARY 1995 ECN-R--95-004 fcl<f$W439 energy innovation ACTINIDE TRANSMUTATION IN NUCLEAR REACTORS J.H. BULTMAN The [Netherlands Energy Research Foundation ECN Het Energieonderzoek Centrum Nederland (ECN) is is the leading institute in the Netherlands for energy het centrale instituut voor onderzoek op energie­ research. ECN carries out basic and applied research gebied in Nederland. ECN verricht fundamenteel en in the fields of nuclear energy, foss-1 fuels, renewable toegepast onderzoek op het gebied van kernenergie, energy sources, policy studies, environmental aspects fossiele-energiedragers, duurzame energie, beleids­ of energy supply and the development and application studies, milieuaspecten v«.n de energievoorziening en of new materials. de ontwikkeling en toepassing van nieuwe materialen. ECN employs more than 900 staff. Contracts are Bij ECN zijn ruim 900 medewerkers werkzaam. De obtained from the government and from national and opdrachten worden verkregen van de overheid en van foreign organizations and industries. organisaties en industrieën uit binnen- en buitenland. ECN's research results are published in a number of De resultaten van het ECN-onderzoek worden neer­ report series, each series serving a different public, gelegd in diverse rapportenseries, bestemd voor ver­ from contractors to the international scientific world. schillende doelgroepen, van opdrachtgevers tot de internationale wetenschappelijke wereld. The R-series is for research reports that make the results of ECN research available to the international De R-serie is de serie research-rapporten die de technical and scientific world. resultaten van ECN-onderzoek toegankelijk maken voor de internationale technisch-wetenschappelijke wereld. Netherlands Energy Research Foundation ECN Energieonderzoek Centrum Nederland P.O. Box 1 Postbus l NL-1755ZG Petten 1755 ZQ Petten the Netherlands Telefoon : (02246) 49 49 Telephone : +31 2246 49 49 Fax : (02246) 44 80 Fax :+31 2246 44 80 Dit rapport is te verkrijgen door het overmaken van This report is available on remittance of Dfl. 35 to: f35,-- op girorekening 3977703 ten name van: ECN, General Services. ECN. Algemene Diensten Petten, the Netherlands te Petten Postbank account No. 3977703. onder vermelding van het rapportnummer. Please quote the report number. © Netherlands Energy Research Foundation ECN <D Energieonderzoek Centrum Nederland JAMÜARY 1995 ECN-R--95-004 KS001922914 R: FI DE0O8071410 •DE008071410» ACTINIDE TRANSMUTATION IN NÜCLEAR REACTORS J.H. BULTMAN THIS REPORT HAS ALSO BEEN PÜBIJSHED AS A PHD THESIS, ISBN 90-9007889-4 DEFENDED AT THE TECHNICAL UNIVERSITY DELFT, JANUARY 17TH, 1995 / Abstract This report has also been published as a PhD thesis. It discusses the reduction of the transuranics part of nuclear waste. Requirements and criteria for efficient burning of transuranics are developed. It is found that a large reduction of transuranics produced per unit of energy is possible when the losses in reprocessing are small and when special transuranics burner reactors are used at the end of the nuclear era to reduce the transuranics inventory. Two special burner reactors have been studied in this thesis. In chapter 3, the Advanced Liquid Metal Reactor is discussed. A method has been developed to optimize the burning capability while complying to constraints imposed on the design for safety, reliability, and economics. An oxide fueled and metallic fueled ALMR have been compared for safety and transuranics burning. Concluded is that the burning capability is the same, but that the higher thermal conductivity of the metallic fuel has a positive effect on safety. In search for a more effective waste transmuter, a modified Molten Salt Reactor was designed for this study. The continuous refueling capability and the molten salt fuel make a safe design possible without uranium as fuel. A four times faster reduction of the transuranics is possible with this reactor type. The amount of transuranics can be halved every 10 years. The most important conclusion of this work is that it is of utmost importance in the study of waste transmutation that a high burning is obtained with a safe design. In future work, safety should be the highest priority in the design process of burner reactors. i Ui Contents Abstract i Summary vi Nomenclature ix List of Symbols x List of Definitions xi List of Abbreviations xv 1 Introduction 1 1.1 Nuclear Energy and Waste 1 1.2 Motivation to Perform this Work 4 1.3 What this Thesis Covers 7 2 Nuclear Waste and Nuclear Waste Reduction 9 2.1 Introduction 9 2.2 Waste Parameters 10 2.3 Waste Production and Reduction Factors 13 2.3.1 Fuel and Waste Amounts and Flows 13 2.3.2 Definitions to Evaluate Waste Production and Reduction 16 2.4 On Reducing LWR Waste by Recycling in LWRs 17 2.4.1 Introduction 17 2.4.2 Calculational Method 19 iv CONTENTS 2.4.3 Plutonium Recycling in LWRs 20 2.4.4 Transuranics Recycling in LWRs 22 2.4.5 Uranium Recycling in LWRs 24 2.4.6 Transuranics Waste Produced by Equilibrium LWRs . 26 2.5 Energy Scenarios and Waste Production 26 2.5.1 Energy Scenarios 28 2.5.2 Reactor Designs 29 2.5.3 Waste and Energy Production 31 2.6 Physics Aspects of Burner Design 36 2.6.1 Burner Design Objective 36 2.6.2 Waste and Enrichment 37 2.6.3 Transmutation Efficiency of a Transuranics Fueled Reactor 39 2.7 Conclusions 41 3 LWR Waste Reduction with ALMR Burners 43 3.1 Introduction 43 3.2 The ALMR system 45 3.3 Design Approach .. 48 3.4 Calculational Methods 51 3.4.1 Multigroup Cross Section Generation 52 3.4.2 Flux Solution and Burnup Calculations 54 3.4.3 Reactivity Control Requirement and Control Rod Worth Calculation 55 3.4.4 Void Worth and Reactivity Parameters 55 3.5 Influence of Design Parameters on Actinide Burning 57 3.5.1 Introduction 57 3.5.2 Partial Derivatives of the Performance Parameters to the Design Parameters 58 3.5.3 Correlations between the Coefficients for Cycle Length and Number of Batches 61 3.5.4 Burner Optimization within Performance Constraints . 62 3.6 Metallic and Oxide Fueled ALMR Burners 69 CONTENTS v 3.6.1 Optimization Process and Core Description 69 3.6.2 Comparison of the Metallic and Oxide Fueled Burners 71 3.6.3 Reactivity Control 73 3.6.4 Void Worth and Reactivity Parameters of the Optimized Burner Designs 74 3.6.5 Safety Parameters 79 3.7 Conclusions 86 4 Molten Salt D*ansmuter 89 4.1 Introduction 89 4.2 History of the Molten Salt Reactor Development 92 4.3 Systems Description 93 4.3.1 Core 93 4.3.2 Reprocessing 94 4.3.3 Materials b4 4.3.4 Cooling 96 4.4 Calculational Methods 96 4.4.1 Neutron Balance 96 4.4.2 Calculation of Fission Product Densities 97 4.4.3 Calculation of the Actinide Densities 98 4.4.4 Core Calculation 100 4.4.5 Calculation of Reactivity Coefficients 100 4.5 Design of the Molten Salt Transmuter 100 4.5.1 Role of Fission Products 100 4.5.2 Flux Dependence 102 4.5.3 Fuel Volume Fraction Dependence 107 4.5.4 Transuranics Salt Fraction Dependence Ill 4.5.5 Startup of the Molten Salt Transmuter 114 4.5.6 Discussion of the Results 114 4.6 Influence of Uncertainty in Actinide Cross Sections 115 4.6.1 Adjoint Calculational Method 115 vi CONTENTS 4.6.2 Method Verification 117 4.6.3 Reactivity and Core Size 118 4.7 Conclusions 121 5 Final Conclusions and Recommendations 123 REFERENCES 130 A EQUI: Calculation of Equilibrium Actinide Densities 131 A.1 Calculational Method 131 A.2 Cross Section and Decay Data 134 A.3 Program Description 135 A.4 Verification of EQUI 137 A.4.1 Nuclide Densities 137 A.5 Conclusions 139 Acknowledgement 140 V» Summary The reduction of the transuranics part of nuclear waste is discussed in this thesis. Only the transuranics and not the fission products are discussed, because they represent the highest environmental hazard in the long term. A huge amount of 1,000 tonne of transuranics is already produced worldwide, and annually about 80 tonne of transuranics is added. This material can be used for nuclear energy production, for instance, as fuel for Advanced Liquid Metal Reactors (ALMRs), but to reduce this amount will be rather difficult as only 1.2 kg/MWey can be fissioned maximally. To stabilize the amount of transuranics, one has to operate about 70 GWe in burners; that is an increase of about 20% in installed nuclear power worldwide. One can reduce the production of transuranics by recycling in the reactor which produces them. As is shown in chapter two of this thesis, only the plutonium iso­ topes can be recycled in Light Water Reactors (LWRs), because recycling of other transuranics will lead to a high production of short-lived and spontaneously fission­ ing actinides. These actinides make the reprocessing of fuel, which is necessary when recycling is applied, impossible with current techniques. The production of transuranics can be reduced by maximally a factor of four by recycling plutonium isotopes in LWRs. Another approach to reduce transuranics is the use of special burners. In chapter two, we show that nuclear energy can be produced without an increase of the transuranics amount currently produced. For low reprocessing losses in the order of 0.1 %, energy can be produced in this way for many centuries. The physics of transuranics transmutation is rather simple: reduce the production rate of transuranics by removing uranium from the fuel. Also, the time to reduce a certain amount of transuranics should be small, which can be accomplished by a high specific power. All other design criteria are related to issues of safety and technology.
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