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SPent fuel characterisation Program for the Implementation of Repositories WP2 & WP4 Development of measurement methods and techniques to characterise spent nuclear fuel Henrik Widestrand and Peter Schillebeeckx 25 – 26 October 2016, Cordoba, Spain IGD-TP 7 th Exchange forum
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SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

Apr 30, 2020

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Page 1: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

SPent fuel characterisation Program for the

Implementation of Repositories

WP2 & WP4

Development of measurement methods and

techniques to characterise spent nuclear fuel

Henrik Widestrand and Peter Schillebeeckx

25 – 26 October 2016, Cordoba, Spain

IGD-TP 7th Exchange forum

Page 2: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

Interim storage or final disposal of spent nuclear fuel

Characterisation of Spent Nuclear Fuel (SNF) is required for a safe, secure and

economic storage and disposal.

Main observables of interest:

• Decay heat

• Neutron and gamma-ray emission

• Reactivity

Page 3: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

Quality of predicted observables depends on:

• Quality of the calculation methods (codes + nuclear data)

• Quality of the irradiation history + engineering details of the SNF

Optimum design of storage conditions: theoretical predictions

1 10 100 100010-1

100

101

102

Dec

ay h

eat /

mW

Time / year

Ptot

1 10 100 100010

100

1000

Total

Neu

tron

em

issi

on r

ate

/ s-1

Time / year

PWR UO2 pellet235U/U = 4.8 %

m(U) = 4.4 g

Burnup = 44 GWd/tU

Page 4: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

Present status : e.g. decay heat

Experiments on PWR at CLAB (1998)

Different codes (cal3 = SIEMENS)

200 400 600 800 1000 12000.85

0.90

0.95

1.00

1.05

1.10

1.15 P

cal1/P

exp = 1.03 +/- 0.06

Pcal2

/Pexp

= 0.97 +/- 0.03

Pcal3

/Pexp

= 0.91 +/- 0.03

Pexp

/ W

Pca

l / P

exp

Calorimeter at CLAB

Page 5: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

Present status : e.g. decay heat

Experiments at CLAB (2003 - 2004)

Calculations: ORIGEN-S

0 200 400 600 8000.85

0.90

0.95

1.00

1.05

1.10

1.15 BWR P

cal/P

exp = 1.00 +/- 0.04

PWR Pcal

/Pexp

= 1.02 +/- 0.02

Pexp

/ W

Pca

l / P

exp

Calorimeter at CLAB

Page 6: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

Present status : e.g. decay heat

Experiments at CLAB (1998 and 2003 - 2004)

Calculations: ORIGEN-S

0 200 400 600 8000.85

0.90

0.95

1.00

1.05

1.10

1.15 P

cal / P

exp (1998) = 0.97 +/- 0.03

Pcal

/ Pexp

(2003 - 2004) = 1.02 +/- 0.02

Pexp

/ W (2003- 2004)

Pca

l / P

exp

Calorimeter at CLAB

Page 7: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

Objective :

Develop innovative Non Destructive Analysis (NDA) techniques and improve

existing ones for the characterization of Spent Nuclear Fuel (SNF), to:

• Reduce bias effects and uncertainties of experimental data

• Validate & improve theoretical models (including nuclear data)

• Verify irradiation histories and improve incorrect data

• Define correlation procedures between observables

e.g. gamma-ray ⇔ heat

Separation between WP2 & WP4 : logistic reasons

WP2 : radionuclide sealed sources and reference materials

WP4 : highly radioactive irradiated nuclear material

WP2 & WP4

Page 8: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

• Develop, improve and validate NDA techniques to directly measure

− decay heat

− neutron emission

− gamma-ray emission

− reactivity

− nuclide vector

avoiding complex and time consuming chemical analysis

• Make use of other efforts:

− Next Generation Safeguards Initiative (NGSI) of DOE/NNSA

− EURATOM/DOE/SKB agreement (Action Sheet -50)

− JAEA/JRC collaboration agreement (characterisation of melted fuel by NDA)

− FP7 project: First Nuclides

− International projects: ARIANE, MALIBU, REGAL

WP2 & WP4

Page 9: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

Example: decay heat

Improve fundamental understanding of measurement process

Identify the main metrological parameters, e.g. source terms

1 10 100 10000.0

0.2

0.4

0.6

0.8

1.0

Pi /

Pto

t

Time / year

Am-241 Ba-137m Ce-144 Cm-242 Cm-244 Co-60 Cs-134 Cs-137 Eu-154 Kr-85 Nb-95 Pm-147 Pr-144 Pu-238 Pu-239 Pu-240 Pu-241 Rh-106 Ru-106 Sr-90 Y-90 Y-91 Zr-95

Decay heat : Pi

1 10 100 100010-2

10-1

100

101

102

Decay heat : Pi

Dec

ay h

eat /

mW

Time / year

Am-241 Ba-137m Ce-144 Cm-242 Cm-244 Co-60 Cs-134 Cs-137 Eu-154 Kr-85 Nb-95 Pm-147 Pr-144 Pu-238 Pu-239 Pu-240 Pu-241 Rh-106 Ru-106 Sr-90 Y-90 Y-91 Zr-95 total

PWR UO2 pellet235U/U = 4.8 %

m(U) = 4.4 g

Burnup = 44 GWd/tU

Page 10: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

1 10 100 100010-2

10-1

100

101

102

Decay heat : Pi

Dec

ay h

eat /

mW

Time / year

Am-241 Ba-137m Ce-144 Cm-242 Cm-244 Co-60 Cs-134 Cs-137 Eu-154 Kr-85 Nb-95 Pm-147 Pr-144 Pu-238 Pu-239 Pu-240 Pu-241 Rh-106 Ru-106 Sr-90 Y-90 Y-91 Zr-95 total

1 10 100 10000.0

0.2

0.4

0.6

0.8

1.0

Pi /

Pto

t

Time / year

Am-241 Ba-137m Ce-144 Cm-242 Cm-244 Co-60 Cs-134 Cs-137 Eu-154 Kr-85 Nb-95 Pm-147 Pr-144 Pu-238 Pu-239 Pu-240 Pu-241 Rh-106 Ru-106 Sr-90 Y-90 Y-91 Zr-95

Decay heat : Pi

Example: decay heat

Cooling time : 5 y < t < 50 y (β- decay of FP)

• Fission yields

• Specific heat FP: e.g. 90Sr/Y and 137Cs/Ba

Nuclide Specific power

µW/GBq

Ramthun (1973)

(experimental)

Collé (2007)

(theoretical)

Libraries

JEF-2.2 JEFF-3.1.1 ENDF/B-VII.1 90

Sr 31.4 27.2 27.9 31.4 90

Y 150.0 148.0 149.5 149.6 90

Sr/90

Y 183.0 ± 2.7 181.4 175.2 177.4 181.0

Page 11: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

1 10 100 10000.0

0.2

0.4

0.6

0.8

1.0

Pi /

Pto

t

Time / year

Am-241 Ba-137m Ce-144 Cm-242 Cm-244 Co-60 Cs-134 Cs-137 Eu-154 Kr-85 Nb-95 Pm-147 Pr-144 Pu-238 Pu-239 Pu-240 Pu-241 Rh-106 Ru-106 Sr-90 Y-90 Y-91 Zr-95

Decay heat : Pi

1 10 100 100010-2

10-1

100

101

102

Decay heat : Pi

Dec

ay h

eat /

mW

Time / year

Am-241 Ba-137m Ce-144 Cm-242 Cm-244 Co-60 Cs-134 Cs-137 Eu-154 Kr-85 Nb-95 Pm-147 Pr-144 Pu-238 Pu-239 Pu-240 Pu-241 Rh-106 Ru-106 Sr-90 Y-90 Y-91 Zr-95 total

Example: decay heat

Nuclide Specific power

µW / GBq

241Am 900.3 ± 3.5

238Pu 896.2 ± 0.5

239Pu 840.4 ± 1.1

240Pu

843.1 ± 1.1

Cooling time : 10 y < t (241Am and 238,239,240Pu)

• Production: σσσσ(n,γγγγ) and σ(n,f)

• Specific heat

Page 12: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

Identify metrological parameters of the measurement process

Example: neutron emission

1 10 100 100010

100

1000

Neu

tron

em

issi

on r

ate

/ s-1

Time / year

Total (s.f) (α,n)

238Pu, 241Am,244Cm

242Cm

244Cm

246Cm

PWR UO2 pellet235U/U = 4.8 %

m(U) = 4.4 g

Burnup = 44 GWd/tU

Page 13: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

NDA methods: improve & refine existing NDA technique

Fuel assemblies • Decay heat

– Calorimetry

– Gamma-ray spectrum

• Gamma-ray emission

– Tomography

– Gamma-ray spectrometry

• Reactivity (collaboration with LANL, Action Sheet-50)

– Differential Die-Away (DDA) ,

– Differential Die-Away Self-Interrogation (DDSI)

Page 14: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

• Radiation hard neutron detector (Diamond technology)

– Miniature detector (control channels)

– Stand-alone

– Integrated in e.g. DDA, DDSI, SINRD

• Gamma-ray detectors: LaBr, CeBr, CZT

– Spectrometry

– Tomography

• Reactivity

– Self-Interrogation Neutron Resonance Densitometry (SINRD)

(SCK•CEN)

NDA methods: innovative NDA techniques

Fuel assemblies

0.1 1100

101

102

103

104

0.0

0.2

0.4

0.6

0.8

1.0

Tot

al c

ross

-sec

tion

(b)

Neutron energy (eV)

239Pu

1% 239Pu4% 239Pu

Tra

nsm

issi

on

Page 15: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

• Direct NDA measurement of observables (outside hot cell)

– Heat , neutron, gamma-ray, nuclide vector

– Transport sample from hot cell to device

⇒ Avoid chemical analysis

• Use of well-characterised samples with documented history

– FP7 : First Nuclides

– REGAL project organised by SCK•CEN

NDA methods: innovative NDA techniques

Small samples

Page 16: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

• Proof- of-principle: neutron output

– Direct related to Cm-quantity

• Final objective

– Neutron and gamma-ray emission

– Heat by calorimetry (including existing solutions)

– Nuclide vector by Neutron Resonance Transmission Analysis (NRTA)

NDA methods: innovative NDA techniques

Small samples

0 5 10 15 20 25 30 35 40

0.000

0.005

0.010

Texp

Tcal

Neutron energy / eV

238U 238U238U

235UTra

nsm

isso

n235U

Page 17: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

Facilities

Small samples Fuel assemblies

SCK•CEN • NPP Preussen Elektra

• CLAB –Sweden

Page 18: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

Facilities: SCK•CEN (Mol, Belgium)

Small samples • Small sample objective

– Test calculation models on well-defined samples

– Measurement of nuclear data (specific heat)

• Samples from previous & ongoing projects

– Profit from the FP7 “First Nuclides” project

– Well-known radiation history

– Radio-chemically analysed

– Sliced pellet sample available

– Solute samples available

Page 19: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

Facilities: SCK•CEN (Mol, Belgium)

Small samples • Analysis of encapsulated spent fuel samples (e.g. 3 pellets)

Page 20: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

NDA methods: improve & refine existing NDA technique

Fuel assemblies

Measurements on a wide variety of SFA (BU, IE, CT)

• Define realistic performance values (uncertainties)

• Define correlation schemes between different observables

• Use NDA results to improve irradiation histories

Page 21: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

Facilities: Preussen Elektra (NPP-site, Germany)

• Fuel pool inside reactor building holds ∼ 700 fuel

assemblies in each plant

Fuel assemblies

Page 22: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

Facilities: Preussen Elektra (NPP-site, Germany)

• Fuel is loaded into dry storage casks after about 5 - 10

years of shutdown cooling for interim storage

Fuel assemblies

Page 23: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

Facilities: Preussen Elektra (NPP-site, Germany)

• Example plant 1

(18x18) spent fuel

inventory in pool

• MOX and UOX

• BU: 50-60 MWd/kgU

• CT ∼ 1 -15 y

Page 24: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

Facilities: Preussen Elektra (NPP-site, Germany)

• Example plant 2

(16x16) spent fuel

inventory in pool

• UOX

• BU: 45-53 MWd/kgU

• CT ∼ 1 -15 y

Page 25: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

Facilities: CLAB (Oskarshamn, Sweden)

Fuel assemblies • Central Interim Storage Facility for Spent Nuclear Fuel

• LWR fuel assemblies (~ 6300 t BWR and PWR fuel stored)

• Service pool with fuel handling machine

• Calorimeter (BWR and PWR fuel)

• γ-spectrometry scan equipment with collimator

• Experiences from earlier projects

• Approximate fuel properties:

– 7 fuel types BWR

– 7 fuel types PWR

– BU range 10 - 55 GWd/tU

– CT range (2) 5 - 30 y

– IE range 2-5%

Page 26: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

SKB: business case example

Encapsulation plant • Optimisation of canister packing

– Maximum decay heat criteria ( ∼ 1 700 W)

– Max. mean decay heat per assembly if equally

distributed:

• PWR ∼ 425 W,

• BWR ∼ 142 W

– ∼ 6 000 canisters

• Cast iron inserts for

– 4 PWR or

– 12 BWR assemblies

Page 27: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

SKB: business case example

T

Pmax

T

T

T

T

T

T

T

Reduction in bias and uncertainty of decay heat will

improve packing efficiency and reduce empty positions

• Cost per canister

– ∼ 1 M€

• SKB 50 decay heat

– BWR: mean CT= 17 y mean decay heat = 165 W

– PWR: mean CT= 18 y mean decay heat = 590 W

• Example

– 1% increase in number of canisters: 50 M€ in increased costs

Page 28: SP entfuel characterisation Program for the€¦ · SP entfuel characterisation Program for the Implementation of Re positories WP2 & WP4 Development of measurement methods and techniques

Thanks for your attention