Closing
the
CANDU
Fuel
Cycle
with
Modified
PUREX
Recycling CANDU Spent Fuel
Authors
Juhx Pellazar Jinah Kim
Alexander Koven Sameena Mulam (Presenter) Marty Tzolov Leon Wu
WiN – Canada
Conference
•
Need for Processing
•
The Modified PUREX Process
•
Benefits
•
Future Work
1Closing the CANDU Fuel Cycle with Modified
PUREX
Recycling CANDU Spent Fuel• Canada’s radioactive nuclear used fuel inventory and the cost of managing it is a growing, long‐term
concern
Rationale
for
Processing
Nuclear Fuel Waste Inventory, 2010 and Projection to 2050 [1]
How long
before
something
is done
about it?
2CANDU
Fuel
• Fresh CANDU nuclear fuel consists of 88% uranium atoms (U), mostly U‐238
• Spent CANDU fuel with a burn‐up of 190MWh/kg U is composed of 0.57% fission products (FP)*
• Considered “unusable” waste
• BUT, processing it can unlock the carbon‐free energy in the 99.43% actinides, decrease
stored waste and storage time
3
*Hart D and Lush D
(http://www.nwmo.ca/uploads_managed/MediaFiles/645_ 4‐4TheChemicalToxicityPotentialofCANDUSpentFuel.pdf) [2]
• To design a process to convert spent fuel into: 1) Mixed Oxide Fuel (MOX) for CANDU
2) Metallic actinide for Fast Neutron Reactors (FNR) fuel replenishment
• To maximize the purity of the FP stream and the fuel streams
Research
Objectives
Traditional PUREX Process Modified PUREX Process
• Liquid‐liquid extraction using
Tributyl Phosphate (TBP)
• Liquid‐liquid extraction using
TBP, plus compatible agents
• Selective separation plus
purification of U and Pu
• Co‐extraction of Pu with U
• Large amounts of liquid
waste
• Crystallization used to
decrease liquid load
• No separation of long‐lived
minor actinides (MA) from
short‐lived FPs
• Minor actinides and FPs
separated
• Limited recycling options for
fuelling other reactors
• Spent fuel recycled as
metallic and MOX fuel
Need
for
PUREX
Modifications
Spent Fuel Partition U & Pu Dissolution in Acid Extract U & Pu U Fission
Products & Minor
Actinides
Pu
Traditional PUREX Process Modified PUREX Process
• Liquid‐liquid extraction using
Tributyl Phosphate (TBP)
• Liquid‐liquid extraction using
TBP, plus compatible agents
• Selective separation plus
purification of U and Pu
• Co‐extraction of Pu with U
• Large amounts of liquid
waste
• Crystallization used to
decrease liquid load
• No separation of long‐lived
minor actinides (MA) from
short‐lived FPs
• Separation of minor
actinides and FPs
• Limited recycling options for
fuelling other reactors
• Recycling of spent fuel as
metallic and MOX fuel
Need
for
PUREX
Modifications
7 CANDU Spent Fuel Bundle Metallic FNR Fuel Mixed Oxide CANDU Fuel 7 Feed Preparation
Separation and Partitioning
8 CANDU Spent Fuel Bundle Metallic FNR Fuel Mixed Oxide CANDU Fuel FP Storage Preparation 8 Dissolution 99.43 % Ln Storage % Actinide of Feed
Separation and Partitioning
9 CANDU Spent Fuel Bundle Metallic FNR Fuel Mixed Oxide CANDU Fuel FP Storage Preparation 9 Dissolution 99.43 % other U 69.52 % Ln Storage U Crystallization % Actinide of Feed Fuel Preparation
10 CANDU Spent Fuel Bundle Metallic FNR Fuel Mixed Oxide CANDU Fuel FP Storage Preparation 10 Dissolution 99.43 % U/Pu/Np 29.90 % MA/FP/Ln Ln Storage 0.01 % % Actinide of Feed other U 69.52 % Extraction U Crystallization Fuel Preparation
11 CANDU Spent Fuel Bundle Metallic FNR Fuel Mixed Oxide CANDU Fuel FP Storage Preparation 11 Dissolution 99.43 % Extraction SETFICS B Ln MA/Ln FP MA 0.01 % MA Ln Storage <0.01 % <0.01 % U Crystallization % Actinide of Feed U/Pu/Np 29.90 % U 69.52 % MA/FP/Ln other SETFICS A TRUEX Fuel Preparation
12 CANDU Spent Fuel Bundle Metallic FNR Fuel Mixed Oxide CANDU Fuel FP Storage Preparation 12 Dissolution Electrolytic Reduction Ln Storage % Actinide of Feed 99.43 % Extraction SETFICS B Ln MA/Ln FP MA 0.01 % MA <0.01 % <0.01 % U Crystallization U/Pu/Np 29.90 % U 69.52 % MA/FP/Ln other SETFICS A TRUEX Oxidation
Overall
Efficiency
Metallic actinide stream 99.99%<0.01% Actinides FP Final FP stream 97.26% FP <0.01% Actinides 13Waste Type Waste Proposed Treatment
Solid Zircaloy Fuel
Cladding
Reused as alloying material for
FNR bundle High Level
Liquid
Waste
Organic Reused after alkaline washing
Aqueous Calcination and Ceramic
immobilization Effluent
Gases
NOx Nitric acid formation with
absorption column
Waste
Management
Criticality
Issues
Parameter Subcritical Limit for Fissile Solute 235UO 2(NO3)2 239Pu(NO3)4 Concentration of fissile nuclide (g/L) 11.6 7.3 235UO
2(NO
3)
2= 0.01 g/L
239Pu(NO
3)
4=
0.01
g/L
[3]Subcritical limits were compared to the guidelines
in the CNSC Guidance document GD‐327, Guidance
for Nuclear Criticality Safety, section 2.4.1.
• Recycle fuels from CANDU, FNR, LWR, etc.
• U crystallization leads to decreased liquid waste
– Depleted U can be used in FNRs
• Actinides separated from fission products
– Concentrated to ~1.21% fissile content, reused as fuel in CANDU
• Minimizes stored waste and storage time
• Proliferation mitigated by not separating Pu from U
Benefits
of
Modified
PUREX
• Strategically separate out already stable, valuable fission products (rhodium and ruthenium)
• Recycle waste streams and multiple cycles to increase recovery of all actinides
• Development of an implementation strategy
• Optimization of spent fuel storage times and volumes of used nuclear fuel constituents
• Transition plan for FNRs in Canada
Future
Recommendations
18
[1] Low‐Level Radioactive Waste Management Office, "Inventory of Radioactive Waste in Canada,"
Government of Canada, Ottawa, 2012.
[2] Hart D and Lush D, http://www.nwmo.ca/uploads_managed/MediaFiles/645_4‐
4TheChemicalToxicityPotentialofCANDUSpentFuel.pdf
[3] http://nuclearsafety.gc.ca/eng/lawsregs/guidancedocuments/published/html/gd327/