Impact of Partitioning, Transmutation and Waste Reduction
Technologies on the Final Nuclear Waste Disposal
Werner von Lensa, Forschungszentrum Jülich
Co-authors:
L. Boucher (CEA-France), E. Gonzales (CIEMAT, Spain), D. Greneche (AREVA-NC, France), D. Westlen, J. Wallenius (KTH, Sweden),
J. Marivoet (SCK•CEN, Belgium), R. Nabbi, M. Rossbach & R. Odoj (FZJ-Germany), C.H. Zimmerman (Nexiasolutions, United Kingdom)
IGD-TP / SNETP Exchange Forum, Prague, 29-30 October 2013
RED-IMPACT
2
Partners of RED-IMPACT
Research50%
Waste Agencies
18%
Nuclear Industry &
Utilities32%
23 partners + 2 subcontractors KTH-Sweden: Coordinator FZJ-Germany: Co-Coordinator Belgium: BN; SCK-CEN Czech Republic: NRI; RAWRA EC: ITU-Karlsruhe France: Areva ANP, CEA; COGEMA Germany:FANP; GRS; IER; KKP Netherlands: NRG Romania: CITON Slovakia: DECOM, VUJE Spain: CIEMAT; EA; ENRESA UK: NexiaSolutions; NIREX; UC
EC CONTRACT NO. FI6W-CT-2004-002408
Duration: March 2004 – September 2007
3
Working procedure
1. Definition of fuel cycle 2. Heavy Metal mass flow 3. Neutronic calculations 4. Mass flow in reprocessing units Actinide losses: 0.1% in HLW, 0.02% in ILW Volatile Activation + Fission Products
• I: 1% in HLW, 1% in ILW • 14C: 10% in HLW • Cl: 1% in HLW, 0.2% in ILW
5. Waste inventories 6. Waste disposal analyses 7. Estimation of environmental, economic and
social indicators
4
Investigated Fuel Cycles
• Industrial scenarios – Scenario A1: (reference) : once through open cycle with Gen-II / III reactors
– Scenario A2 : mono-recycling of plutonium in Gen-III reactors (+ variants e.g. Th-MOX, IMF, PWR vs. BWR etc.)
– Scenario A3 : Multirecycling of Pu (only) in Sodium Fast Reactors (EFR)
• Innovative scenarios – Scenario B1 : Multi-recycling of Pu & MA in Sodium Fast Reactors (EFR)
plus advanced PUREX
– Scenario B2 : multi-recycling of plutonium in Gen-III reactors and burning of Minor Actinides in ADS plus advanced PUREX & PYRO
– Scenario B3 : mono-recycling of plutonium in Gen-III reactors + burning of plutonium in Gen-IV fast reactors + burning of Minor Actinides in ADS including advanced PUREX and PYRO (reduced efforts)
Cradle-to-Grave
5 A1: 5.354 spent fuel assemblies / TWhel B1: 1.644 canisters / TWhel (HLWvitr.)
6
Performance indicators
The indicators have been divided into two major groups:
• “Technical” indicators related to waste management issues: – composition of the waste; number of SF-assemblies, number of canisters, – size of the repository; gallery length (influenced by heat load) – long-term performance of the repository system:
• individual annual dose; • radiotoxicity flux released into the biosphere; • integrated radiotoxicity flux released into the biosphere.
– Inclusion of ILW
• Economic, Environmental and Societal sustainability (EES) indicators – Production cost & external cost – Fuel import dependencies, resource consumptions – Proliferation and terrorist attack resistance – Health impacts on workers & public in normal operation & accidents – etc.
7
Priorities
1,E+02
1,E+03
1,E+04
1,E+05
1,E+06
1,E+07
1,E+08
1,E+09
1 10 100 1000 10000 100000 1000000time (years)
Sv p
er to
n H
M
Grand totalPlutoniumAmericiumCuriumUraniumNeptuniumFission Products
Plutonium Management has strongest Impact ! Focus on most important MA !!!
U-Equilibrium
8
Thermal output and length of disposal galleries (Clay)
Scenario Clay: allowable
thermal output at disposal time
Total needed gallery length
Relative needed gallery length
(W/m) (m/TWhe) (-) A1 354 5.922 1 A2 332 / 376 5.743 0.970 A3 365 3.479 0.587 B2 379 2.895 0.489 B1 379 1.882 0.318 B1-separation of Sr 1.273 0.215 B1- separation of Cs and Sr (Cs-waste disposed after 100 a)
0.439 0.0741
Reduction by a Factor of 3 (A1 vs. B1)
Removal of Cs & Sr would allow further reduction
A1: LWR-open A2: LWR-Mono A3: SFR-Multi-Pu B1: SFR-Multi-Pu&MA B2: SFR+ADS B3: LWR, SFR+ADS
9
Repository in granite Concept: Enresa, Spain
• Bentonite saturated after 20 a, corrosion starts
• Sequential failure of canisters from 1300 to 10000 a
• Average time for H2O to reach biosphere 8400 a
• Diffusion and sorbtion retards the transport of many nuclides
• Release to river (106 m3/a), exposed group use river water
10
Long-Lived Fission Products dominate Doses (A1 granite)
1,E-14
1,E-13
1,E-12
1,E-11
1,E-10
1,E-09
1,E-08
1,E+03 1,E+04 1,E+05 1,E+06 1,E+07
Time (years)
Dos
e (S
v/yr
-TW
h(e)
)
I129
Se79Sn126
C14
Cl36
Cs135
Ra226-Th230
TOTAL
Pa231Th229
135Cs
11
Granite: calculated doses (all scenarios, Enresa)
1.E-14
1.E-13
1.E-12
1.E-11
1.E-10
1.E-09
1.E-08
1.E+03 1.E+04 1.E+05 1.E+06 1.E+07
Time (years)
Dos
e (S
v/yr
-TW
h(e)
)
Scenario A1
Scenario B2Scenario A3
Scenarios A3 & B1
Scenario A2
Scenario B2
Scenarios A3 & B1
Differences mainly due to Iodine removal during reprocessing !!!
A1: LWR-open A2: LWR-Mono A3: SFR-Multi-Pu B1: SFR-Multi-Pu&MA B2: SFR+ADS B3: LWR, SFR+ADS
12
Calculated doses in Clay (all scenarios, SCK•CEN)
1.0E-17
1.0E-16
1.0E-15
1.0E-14
1.0E-13
1.0E-12
1.0E-11
1.0E-10
1.0E+02 1.0E+03 1.0E+04 1.0E+05 1.0E+06 1.0E+07
Time after canister failure (years)
Dos
e (r
iver
pat
hway
) (Sv
/a/T
Whe
)
A1A2 hlwA2 spf-moxtotal A2A3B1B2 hlw-uoxB2 hlw-moxB2 hlw-adstotal B2
A1: LWR-direct A2: LWR-Mono A3: LWR-Multi B1: SFR-Multi B2: SFR+ADS
13
Variant scenarios of B1 (calculated e.g. for Granite)
Impact of waste matrix lifetime
1.E-14
1.E-13
1.E-12
1.E-11
1.E-10
1.E-09
1.E+03 1.E+04 1.E+05 1.E+06 1.E+07
Time (years)
Dos
e (S
v/yr
-TW
h(e)
)
Se79
Sn126
C14
Cs135
I129
Ca41Cl36
Se79
I129
C14
Cs135
Ca41
Sn126
72.000yr glass
720.000yr glass
7.2 million yr glass
RN
RN
C14
I129
Cs135
Se79
RN
Actinides& daughters (overlapped)
Sn126
14
Thorium: Reduction of MA
Uranium
0,7 %
Actinides: Long-term Radiotoxicity !!!
Secondary Fuels
Thorium (3 x more)
Th/Pu MOX: 2x better Pu/MA consumption !!!
15
Human intrusion doses (all scenarios, Nirex)
1E-061E-051E-041E-031E-021E-011E+001E+011E+021E+031E+04
1E+02 1E+03 1E+04 1E+05 1E+06
Time (yr)
Dos
e (S
v)
Scenario A1Scenario A2 VHLWScenario A2 MOXScenario A3Scenario B1Scenario B2 ADSScenario B2 MOXScenario B2 UOXCigar Lake Natural AnalogueLower ICRP Intervention LevelUpper ICRP Intervention Level
16
ILW-Packages
Source: • Structural Parts of Fuel Assemblies
– End-fittings, chopped claddings, grids etc. – Core & Blanket
• Reprocessing of ADS-Fuel (Zr-Nitride) – C-14, Cl-36, Nb-94 contents – Noble metals from Pyro-processing
• ADS core components – Pb-Bi, core support, window, accelerator
tube
A1 0 m3/TWeh A2 2,5 m3/TWeh A3 5,3 m3/TWeh B1 5,3 m3/TWeh B2 3,3 m3/TWeh
For granite repository:
• Waste matrix less retention
• Direct access of ground water
• doses start earlier
• ILW dominates till 20.000 y
17
Calculated doses for ILW in Granite (scenario A2, Enresa)
1.E-14
1.E-13
1.E-12
1.E-11
1.E-10
1.E-09
1.E-08
1.E+03 1.E+04 1.E+05 1.E+06 1.E+07
Time (years)
Dos
e (S
v/yr
-TW
h(e)
)
Se79
C14
Cl36
TOTALI129
Mo93
Ra226Th230
Cs135
18
Doses for HLW + ILW in Granite
1.E-14
1.E-13
1.E-12
1.E-11
1.E-10
1.E-09
1.E-08
1.E+03 1.E+04 1.E+05 1.E+06 1.E+07
Time (years)
Dos
e (S
v/yr
-TW
h(e)
)
Scenario A1
Scenario A2
Scenarios A3 & B1
Scenario B2
Scenarios A3 & B1
Enresa calculation
19
Conclusions (1)
• P&T Impact on repository dimensions (heat load) – reduction of gallery length with a factor 3 – a factor 5 in case of Sr separation – a factor 10 (or more) in case of Cs and Sr separation
• P&T Impact on dose: HLW disposal – limited: due to mobile fission and activation products
(14C, 36Cl, 79Se, 99Tc, 129I, 135Cs, 126Sn) – depends on amount of disposed 129I, 14C, 36Cl vs.
discharged volatile isotopes during reprocessing – ADS-specific waste to be considered in more detail
• P&T Impact on Human Intrusion dose: significant • Impact of more stable matrix on dose: significant
20
Conclusions (2)
• ILW Impact on dose: – Granite: ILW doses > HLW doses consider use of low activation materials, add barriers (C-14)
– Clay: ILW doses < HLW doses • Reduced generation of MA: Th-MOX, IMF vs. Pu-MOX
• Hetereogeneous recycling & other reactors (BWR, HWR, HTR etc.)
• Improved Partitioning / Reprocessing: LLFP, volatile FP • Partitioning & Conditioning (P&C): viable option • Cost / Benefit Evaluations: science / industry dialog • Repository/waste package adaptation to P&T waste Transition to advanced reprocessing/conditioning: ASAP
21
Thanks for your attention
22
Assumptions
• A1: reference scenario: open cycle • Burn-up 50 GWd/tHM, UOX : 235U enrichment 4.2%
– HLW: 5.354 spent fuel assemblies / TWhel • B1: Fast neutron Gen IV & advanced PUREX
• Burn-up: core 136 GWd/tHM (axial 15, radial 24) • MOX: 23.2% Pu + 2.7% MA
– Vitrified HLW: 1.644 canisters / TWhel • HLW disposal in 3 host formations
– Granite: ENRESA (Spain), NRI (Czech Republic) – Clay: SCK•CEN (Belgium) – Salt: GRS (Germany)
23
Evolution of temperature
0
20
40
60
80
100
120
0.01 0.1 1 10 100 1000time (years)
T (°
C)
interface A1interface A2 HLWinterface A2 MOXinterface A3interface B1interface B2 UOXinterface B2 MOXinterface B2 ADS A1: LWR-open
A2: LWR-Mono A3: LWR-Multi B1: SFR-Multi B2: SFR+ADS
24
Radiological impact
• Safety functions of repository system – Engineered containment
• Container lifetime (2000 a)
– Slow release of RNs • Waste matrix degradation (100 000 a) • Solubility limitation (reducing conditions)
– Very slow transport • Diffusive transport through buffer (and clay formation) • Sorption on (clay) minerals
• Small releases of radionuclides into biosphere
25
Radiotoxicity Fluxes for Clay
1.0E-12
1.0E-11
1.0E-10
1.0E-09
1.0E-08
1.0E-07
1.0E-06
1.0E-05
1.0E-04
1.0E-03
1.0E-02
1.0E-01
1.0E+02 1.0E+03 1.0E+04 1.0E+05 1.0E+06 1.0E+07
Time after canister failure (years)
RT
Flux
to N
eoge
ne (S
v/a/
TWhe
)
C14
Cl36
Ni59
Se79
Zr93
Nb94
Tc99
Pd107
Sn126
I129
Cs1351.0E-12
1.0E-11
1.0E-10
1.0E-09
1.0E-08
1.0E-07
1.0E-06
1.0E-05
1.0E-04
1.0E-03
1.0E-02
1.0E-01
1.0E+02 1.0E+03 1.0E+04 1.0E+05 1.0E+06 1.0E+07
Time after canister failure (years)
RT
Flu
x to
Neo
gen
e (S
v/a/
TW
he)
Se79
Zr93
Tc99
Pd107
Sn126
I129
Cs135
A1 B1 Significant impact of long-lived fission products !
Minor Actinides strongly immobilised ! Strong dependence on solubility limits !
26
Human intrusion doses (scenario A1, Nirex)
0.000001
0.00001
0.0001
0.001
0.01
0.1
1
10
100
1000
10000
100 1000 10000 100000 1000000
Time (yr)
Dos
e
Cl_36
Sr_90
Tc_99
I_129
Cs_137
Po_210
Pb_210
Rn_222
Ra_226
Ac_227
Th_228
Th_229
Th_230
Th_232
Pa_231
U_234
U_235
U_238
Pu_238
Pu_239
Pu_240
Pu_241
Am_241
Am_242m
Am_243
Total
Pu-240
Am-241
Pu-238Cs-137
Total
Pu-239 Rn-222
Th-229
Ra-226
Th-230
, Sv
MA dominate Human Intrusion Scenarios
27
Human intrusion: required isolation times
Comparator
HLW/SF Types
Cigar Lake natural
analogue
ICRP 10 mSv intervention
level
ICRP 100 mSv intervention
level Radiotoxicity
Scenario B1: HLW ~200,000 a ~40,000 a ~1000 a ~300 a Scenario B2: HLW
from ADS fuel > 1 Ma ~70,000 a ~13,000 a ~300 a
Scenario A3: HLW > 1 Ma > 1 Ma ~70,000 a ~24,000 a Scenario A1: spent
UOX fuel > 1 Ma > 1 Ma ~100,000 a ~200,000 a
Scenario A2: spent MOX fuel > 1 Ma > 1 Ma ~200,000 a ~90,000 a
28
ILW: calculated doses in Clay (scenario A3, SCK•CEN)
1.0E-16
1.0E-15
1.0E-14
1.0E-13
1.0E-12
1.0E-11
1.0E-10
1.0E+02 1.0E+03 1.0E+04 1.0E+05 1.0E+06 1.0E+07
Time after canister failure (years)
Dos
e (r
iver
pat
hway
) (Sv
/a/T
Whe
)
C14
C14 (R=2)
Cl36
Se79
Tc99
Sn126
I129
TOTAL
29
Doses for HLW + ILW in Clay (all scenarios, SCK•CEN)
1.0E-17
1.0E-16
1.0E-15
1.0E-14
1.0E-13
1.0E-12
1.0E-11
1.0E-10
1.0E+02 1.0E+03 1.0E+04 1.0E+05 1.0E+06 1.0E+07
Time after canister failure (years)
Dos
e (r
iver
pat
hway
) (Sv
/a/T
Whe
)
A1 sfA2 hlw and sf-moxA2 ilwtotal A2A3 hlwA3 ilwtotal A3B1 hlwB1 ilwtotal B1B2 hlwB2 ilwtotal B2
SF, HLW and ILW