H2/D2 Sieverts solubility constant in LiPb eutectic from

G. ALBERRO, P.M. MARTINEZ, E. WIRTH, S. MOREAU, N. MORAL, I. PEÑALVA, A. SARRIONANDIA-IBARRA, F. LEGARDA,

G. A. ESTEBAN, L. SEDANOSeptember - 2010

H2/D2 Sieverts solubility constant in LiPb eutectic from two independent Isovolumetric Desorption Tests

INDEX

1. Introduction2. Task execution historic 3. IDE measurement technique & facility 4. Difficulties, parasitic effects and corrective actions5. Mathematical model description6. Absorption/desorption runs examples7. Ks and D absorption/desorption results8. PCTPRO2000®9. PCTPRO2000® absorption measurements: Ks and D 10. Discussion

• LiPb QA• LiPb convection • Ks results and other values in the field´s literature• D results and other values in the field´s literature

11. Conclusions12. Near term prospected (proposed) activities

INDEX

1. Introduction2. Task execution historic 3. IDE measurement technique & facility 4. Difficulties, parasitic effects and corrective actions5. Mathematical model description6. Absorption/desorption runs examples7. Ks and D absorption/desorption results8. PCTPRO2000®9. PCTPRO2000® absorption measurements: Ks and D 10. Discussion

• LiPb QA• LiPb convection • Ks results and other values in the field´s literature• D results and other values in the field´s literature

11. Conclusions12. Near term prospected (proposed) activities

• Determine the magnitude and kinetics of the induced tritium flux from the breeding region from the blanket to the helium cooling loop,

• The design (sizing and efficiency) of future tritium extraction systems of the breeding alloy or the He coolant purification system will be defined on the basis of these transport parameters.

TechniqueT

[K]p0

[Pa]Isotope

Ks0

[mol m-3Pa-1/2]D0

[m2s-1]Reference

Absorption 423 - 923 103 – 105 H 0.1185 - Aiello

Desorption 508 - 700 103 – 105 H 6.76 10-4 4.03 10-8 Reiter

Desorption 723 103 – 104 D 7.48 10-4 1.50 10-9 Fauvet

Desorption 573 - 723 104 – 105 T 2.99 10-2 - Katsuta

Absorption 573 - 773 Up to 104 H 1.30 10-2 - Chan

Absorption 850 - 1040 1 - 10 D 1.75 10-2 - Wu

Experimental Hydrogen Sieverts’ constants and diffusivities of eutectic LiPb

Unacceptable data scattering in the literature.

INDEX

1. Introduction2. Task execution historic3. IDE measurement technique & facility 4. Difficulties, parasitic effects and corrective actions5. Mathematical model description6. Absorption/desorption runs examples7. Mathematical model description8. Ks and D absorption/desorption results9. PCTPRO2000®10.PCTPRO2000® absorption measurements: Ks and D 11. Discussion

• LiPb QA• LiPb convection • Ks results and other values in the field´s literature• D results and other values in the field´s literature

11. Conclusions12. Near term prospected (proposed) activities

early 90´s

• Key upgrades and investments: - vacuum pumps and advanced seals, - pressure heads, - quartz components and W sample holder, - data acquisition improvement,

2003-2005

• Improvement/expertise of I(A-D)E measurement technique for LiPb eutectic

> 2006

• Facility recovered at EHU/Bilbao with regional and national programme support.

by 2002

• Reiter conceived (as sole facility in the world able to produce reversible I(A-D) measurements in liquids), developed and exploited at JRC-Ispra (I)

• Identifications of a large set of parasitic effects in the measurement: key for reproducibility

today • A unique EU R&D FT capability fully operational.• Sensitivity for other low H-absorbing materials and

much lower absorbing gases (He)

INDEX

1. Introduction2. Task execution historic 3. IDE measurement technique & facility 4. Difficulties, parasitic effects and corrective actions5. Mathematical model description6. Absorption/desorption runs examples7. Ks and D absorption/desorption results8. PCTPRO2000®9. PCTPRO2000® absorption measurements: Ks and D 10. Discussion

• LiPb QA• LiPb convection • Ks results and other values in the field´s literature• D results and other values in the field´s literature

11. Conclusions12. Near term prospected (proposed) activities

H2 (D2) Supply

Filter

LNT

To

compressed

air

UHV1

OVEN

UHV2

Turbomolecular

pump

Rotative pump

LV1

LV2

MV

QMS

P1

BAG

G2

P3

V2

V1

F

T3

T1, T2

Turbomolecular

pump

Rotative pump

P2

G1

V3

P3

BAG Bayard-Alpert Gauge MV Manually actuated magnetic valve

F Furnace P1, P2 Capacitive manometers

G1 Electropneumatic gate valve P3 Spinning rotor gauge

UHV Ultra high vacuum pumping units QMS Quadrupole mass spectrometer

G2 Manually actuated gate valve V1 Experimental chamber

T1, T2 Thermocuples V2, V3 Expansion volumes

T3 Pt-Resistance Thermometers LV1,2 Manually actuated leak valves

INDEX

1. Introduction2. Task execution historic 3. IDE measurement technique & facility 4. Difficulties, parasitic effects and corrective actions5. Mathematical model description6. Absorption/desorption runs examples7. Ks and D absorption/desorption results8. PCTPRO2000®9. PCTPRO2000® absorption measurements: Ks and D 10. Discussion

• LiPb QA• LiPb convection • Ks results and other values in the field´s literature• D results and other values in the field´s literature

11. Conclusions12. Near term prospected (proposed) activities

Parasitic absorptions

LiPb boiling at pumping phase

Li-segregation in hyper-eutectic LiPb

LiPb oxidation with highly absorbing Li2O formation, as floating debris

Li vapor pressure effect on pressure heads

LiPb solved impurities

LiPb convection

W/quartz crucible and blank tests for Li attacks to quartz

Cooled intermediate glassy serpentine for Li vapor trap

Sample as received Not way to correct

Prevent LiPb oxidationFlushing Ar & pumping

Quantified (minimum impact)

Quantified (marginal effect in the test)

Assessed. Effect on increasing D

INDEX

1. Introduction2. Task execution historic 3. IDE measurement technique & facility 4. Difficulties, parasitic effects and corrective actions5. Mathematical model description6. Absorption/desorption runs examples7. Ks and D absorption/desorption results8. PCTPRO2000®9. PCTPRO2000® absorption measurements: Ks and D 10. Discussion

• LiPb QA• LiPb convection • Ks results and other values in the field´s literature• D results and other values in the field´s literature

11. Conclusions12. Near term prospected (proposed) activities

t

p(t)

τp τrτl

Loading ReleasePumping

pl

pf

PbLi

H2

W

crucible

x = 0

x = a

x

c(x)

c0

(H)

a)(x)n(en

cctxc

n

atnDn

2/12cos)12(

)1(4),(

0

)4/()12(001

222

)4/()12(

0

)4/()12(02

222222

1)2/()12(cos)12(

)1(4),(

anD

n

atnDn

Leaxnen

ctxc

)4/()12()4/()12(

0

)4/()12(03

222222222

1)2/()12(cos)12(

)1(4),(

anDanD

n

atnDn

LP eeaxnen

ctxc

)4/()12()4/()12()4/()12(

022

2/1222222222

11)12(

18)()(

anDanDatnD

n

sLsN

NLP eee

nVpK

V

RTtp

0

)4/()12(

22

2/1

,

222

)12(

181)(

n

atnD

sLsN

LNN en

VpKV

RTptp

Absorption

Desorption

INDEX

1. Introduction2. Task execution historic 3. IDE measurement technique & facility 4. Difficulties, parasitic effects and corrective actions5. Mathematical model description6. Absorption/desorption runs examples7. Ks and D absorption/desorption results8. PCTPRO2000®9. PCTPRO2000® absorption measurements: Ks and D 10. Discussion

• LiPb QA• LiPb convection • Ks results and other values in the field´s literature• D results and other values in the field´s literature

11. Conclusions12. Near term prospected (proposed) activities

t

p(t)

p rl

Loading ReleasePumping

pl

pf

0

0,02

0,04

0,06

0,08

0 5000 10000 15000 20000 25000 30000 35000 40000

t [s]

pn

[m

ba

r]

NO SAMPLE

SAMPLE

NET

523 K

0

0,04

0,08

0,12

0,16

0 5000 10000 15000 20000 25000 30000 35000 40000

t [s]

pn

[m

bar]

NO SAMPLE

SAMPLE

NET

773 K

0

0,04

0,08

0,12

0 5000 10000 15000 20000 25000 30000 35000 40000

t [s]

pn

[m

ba

r]

NO SAMPLE

SAMPLE

NET

613 K

0

0,04

0,08

0,12

0,16

0 5000 10000 15000 20000 25000 30000 35000 40000

t [s]

pn

[m

ba

r]

NO SAMPLE

SAMPLE

NET

703 K

INDEX

1. Introduction2. Task execution historic 3. IDE measurement technique & facility 4. Difficulties, parasitic effects and corrective actions5. Mathematical model description6. Absorption/desorption runs examples7. Ks and D absorption/desorption results8. PCTPRO2000®9. PCTPRO2000® absorption measurements: Ks and D 10. Discussion

• LiPb QA• LiPb convection • Ks results and other values in the field´s literature• D results and other values in the field´s literature

11. Conclusions12. Near term prospected (proposed) activities

Experimental measurements in 2007 at the UPV-EHU:

• Technique: Desorption• Temperature range: T = 532 – 753 [K]• Pressure range: p = 105 [Pa]• Isotope: H

In 2008 :

• Technique: Absorption• Temperature range: T = 523 – 703 [K]• Pressure range: p = 10 - 102 [Pa]• Isotope: H

In 2009 :

• Technique: Desorption• Temperature range: T = 523 – 773 [K]• Pressure range: p = 104 [Pa]• Isotope: H

Difusividad

1.00E-10

1.00E-09

1.00E-08

1.00E-07

1.00E-06

1.00E-05

1.2 1.3 1.4 1.5 1.6 1.7 1.8 1.9 2

1000/T [K-1

]

D [

m2 s

-1]

UPV-EHU (2007)

UPV-EHU (2008)

UPV-EHU (2009)

INDEX

1. Introduction2. Task execution historic 3. IDE measurement technique & facility 4. Difficulties, parasitic effects and corrective actions5. Mathematical model description6. Absorption/desorption runs examples7. Ks and D absorption/desorption results8. PCTPRO2000®9. PCTPRO2000® absorption measurements: Ks and D 10. Discussion

• LiPb QA• LiPb convection • Ks results and other values in the field´s literature• D results and other values in the field´s literature

11. Conclusions12. Near term prospected (proposed) activities

3 pressures: 0.1, 0.5, 1 (bar); 3 temperatures: 300, 350 and 400 (ºC), 2

types of lead-lithium (Stachow, IPUL)

• Quite similar to the “classic” one.

• Fully automatised calibration and vacuum as a major QA point

Absorption/desorption curves

Stachow, LiPb

IPUL, LiPb

Sievert´s behavior evidenced

INDEX

1. Introduction2. Task execution historic 3. IDE measurement technique & facility 4. Difficulties, parasitic effects and corrective actions5. Absorption/desorption runs examples6. Mathematical model description7. Ks and D absorption/desorption results8. PCTPRO2000®9. PCTPRO2000® absorption measurements: Ks and D10. Discussion

• LiPb QA• LiPb convection • Ks results and other values in the field´s literature• D results and other values in the field´s literature

11. Conclusions12. Near term prospected (proposed) activities

Ks values

D values

1.00E-09

1.00E-08

1.00E-07

1.00E-06

1.00E-05

1.00E-04

1.45 1.5 1.55 1.6 1.65 1.7 1.75 1.8

1000/T [K-1]

D [

m2/s

] Ciemat-UPM Diff IPUL H

Ciemat-UPM Diff IPUL D

Ciemat-UPM Diff Stachow D

Ciemat-UPM Diff Stachow H

Ciemat-UPM Diff IPUL H

Ciemat-UPM Diff IPUL D

Ciemat-UPM Diff Stachow D

Ciemat-UPM Diff Stachow

INDEX

1. Introduction2. Task execution historic 3. IDE measurement technique & facility 4. Difficulties, parasitic effects and corrective actions5. Mathematical model description6. Absorption/desorption runs examples7. Ks and D absorption/desorption results8. PCTPRO2000®9. PCTPRO2000® absorption measurements: Ks and D 10. Discussion

• LiPb QA• LiPb convection • Ks results and other values in the field´s literature• D results and other values in the field´s literature

11. Conclusions12. Near term prospected (proposed) activities

Ingot BJost‐Hinrich Stachov Metahandel Spec: 18.8 ± 4.1 ‐ 19.4 ± 3.5 %at Li

Ingot ALatvia Univ., (IPUL)Spec: 15.8 ‐ 16.1 ± 0.2 %at Li

0 2 4 6 8 10

10

20

30

40

50

Lingote A - Pico seleccionado

ThermoX ELAN

6Li

7Li

Li total

co

nc.

Li

/

g·d

m-3

muestra

0 2 4 6 8 10

10

20

30

40

50

Lingote B - Pico seleccionado

ThermoX ELAN

6Li

7Li

Li total

co

nc.

Li

/

g·d

m-3

muestra

(TIMS analysis, Ciemat)

INDEX

1. Introduction2. Task execution historic 3. IDE measurement technique & facility 4. Difficulties, parasitic effects and corrective actions5. Mathematical model description6. Absorption/desorption runs examples7. Ks and D absorption/desorption results8. PCTPRO2000®9. PCTPRO2000® absorption measurements: Ks and D 10. Discussion

• LiPb QA• LiPb convection• Ks results and other values in the field´s literature• D results and other values in the field´s literature

11. Conclusions12. Near term prospected (proposed) activities

Geometry(symmetry):W = 0.5*0.015mH = 0.5*0.6m

Parameters:n = 0.000001335 [m²/s]a = 0.000008901 [m²/s]Cp = 188.41 [j/molK]S= 1 [W/cc]

Boussinesq:T0 = 623.15 [K]beta = 0.001 [1/K]r0 = 9660 [kg m-3]

BB.CC.:North wall: fixed temperature 623.15KSouth wall: fixed temperature 623.15KLateral wall: fixed temperature 623.15Kaxis: axis-symmetric BC

Steady state reached for t> 90s

INDEX

1. Introduction2. Task execution historic 3. IDE measurement technique & facility 4. Difficulties, parasitic effects and corrective actions5. Mathematical model description6. Absorption/desorption runs examples7. Ks and D absorption/desorption results8. PCTPRO2000®9. PCTPRO2000® absorption measurements: Ks and D 10. Discussion

• LiPb QA• LiPb convection • Ks results and other values in the field´s literature• D results and other values in the field´s literature

11. Conclusions12. Near term prospected (proposed) activities

1.0E-09

1.0E-08

1.0E-07

1.0E-06

1.0E-05

0.8 1 1.2 1.4 1.6 1.8 2 2.2

1000/T (K-1)

KS

(at

fr/P

a1/2

)

100200300400500600700

T (ºC)

Ciemat-UPM (IPUL) H

Ciemat-UPM (IPUL) D

Ciemat-UPM (STACHOW) D

UPV-EHU H 2007

UPV-EHU H 2008

UPV-EHU H 2009

Reiter H

Reiter D

Aiello H

CH T

CH_Wu D

Katsuta H

Chan H

Fauvet H

Shumacher H

Fukada H

INL 2008 H

INL 2009 H

QRCSM

INDEX

1. Introduction2. Task execution historic 3. IDE measurement technique & facility 4. Difficulties, parasitic effects and corrective actions5. Mathematical model description6. Absorption/desorption runs examples7. Ks and D absorption/desorption results8. PCTPRO2000®9. PCTPRO2000® absorption measurements: Ks and D 10. Discussion

• LiPb QA• LiPb convection • Ks results and other values in the field´s literature• D results and other values in the field´s literature

11. Conclusions12. Near term prospected (proposed) activities

1.00E-10

1.00E-09

1.00E-08

1.00E-07

1.00E-06

1.00E-05

1.00E-04

1.2 1.3 1.4 1.5 1.6 1.7 1.8 1.9 2 2.1

1000/T [K-1]

D [

m2/s

]

Ciemat-UPM Diff IPUL H

Ciemat-UPM Diff Stachow HCiemat-UPM Diff IPUL D

Ciemat-UPM Diff Stachow DReiter Diff

Shibuya Diff TFukada Diff H

UPV-EHU H 2007UPV-EHU H 2008

UPV-EHU H 2009

INDEX

1. Introduction2. Task execution historic 3. IDE measurement technique & facility 4. Difficulties, parasitic effects and corrective actions5. Mathematical model description6. Absorption/desorption runs examples7. Ks and D absorption/desorption results8. PCTPRO2000®9. PCTPRO2000® absorption measurements: Ks and D 10. Discussion

• LiPb QA• LiPb convection • Ks results and other values in the field´s literature• D results and other values in the field´s literature

11. Conclusions12. Near term prospected (proposed) activities

• Desorption results (2009) confirm range of absorption ones (2008) showing global consistence and confirms Es of Reiter´s tests

• High Ks (compared to Reiter´s one) can be explained in terms of LiPb QA (Li in excess assessed for Stachow GmB material)

• Convection is assessed. High D derived values can be explained by convection.

INDEX

1. Introduction2. Task execution historic 3. IDE measurement technique & facility 4. Difficulties, parasitic effects and corrective actions5. Mathematical model description6. Absorption/desorption runs examples7. Ks and D absorption/desorption results8. PCTPRO2000®9. PCTPRO2000® absorption measurements: Ks and D 10. Discussion

• LiPb QA• LiPb convection • Ks results and other values in the field´s literature• D results and other values in the field´s literature

11. Conclusions12. Near term prospected (proposed) activities

• A fully operational facility providing transport data in LiPb eutectic keeps available at UPV-EHU/Bilbao for future new tasks uses:- further H/D experimental runs,- He transport measurements in LiPb

• A complementary facility, PCTPRO2000®, is developed. Changes have been made to improve measurements accuracy, and in order to avoid parasitic effects.