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(1)

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 

(2)

Need for Processing

The Modified PUREX Process

Benefits

Future Work

1

Closing the CANDU Fuel Cycle with Modified

PUREX 

Recycling CANDU Spent Fuel

(3)

• 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?

2

(4)

CANDU

 

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]

(5)

• 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

(6)

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

(7)

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

(8)

7 CANDU Spent Fuel Bundle Metallic  FNR Fuel Mixed  Oxide  CANDU Fuel 7 Feed Preparation

Separation and Partitioning

(9)

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

(10)

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

(11)

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

(12)

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

(13)

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

(14)

Overall

 

Efficiency

Metallic actinide  stream 99.99%<0.01% Actinides FP Final FP stream 97.26% FP <0.01% Actinides   13

(15)

Waste 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

(16)

Criticality

 

Issues

Parameter Subcritical Limit for Fissile Solute 235UO 2(NO3)2 239Pu(NO3)4 Concentration of fissile  nuclide (g/L) 11.6 7.3 235

UO

2

(NO

3

)

= 0.01 g/L

239

Pu(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.

(17)

• 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

(18)

• 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

(19)

18

(20)

[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/

References

References

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