14
ENEA Experience in PbLi Technologies DCLL WORKSHOP- Tritium extraction technologies for EU DCLL M. Utili (ENEA) [email protected] 14-15 November 2014

ENEA Experience in PbLi Technologies · 11/15/2014  · ) ) ) E 1 - C J - p dsb abs (downstream) (2.17) 2 2 2)2G-p des (downstream) (2.18 KS,M and KS,LM are the Sieverts’ constants

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Page 1: ENEA Experience in PbLi Technologies · 11/15/2014  · ) ) ) E 1 - C J - p dsb abs (downstream) (2.17) 2 2 2)2G-p des (downstream) (2.18 KS,M and KS,LM are the Sieverts’ constants

ENEA Experience in PbLi Technologies

DCLL WORKSHOP- Tritium extraction technologies for EU DCLL

M. Utili (ENEA) [email protected]

14-15 November 2014

Page 2: ENEA Experience in PbLi Technologies · 11/15/2014  · ) ) ) E 1 - C J - p dsb abs (downstream) (2.17) 2 2 2)2G-p des (downstream) (2.18 KS,M and KS,LM are the Sieverts’ constants

DCLL BB: Tritium extraction from Pb-16Li

D. Demage , BB Project KoM Tritium Extraction Technology & Tritium Control

Tritium Extraction System (TES), scope:

to extract tritium from the flowing lithium lead alloy in a dedicated sub-system called

Tritium Extraction Unit (TEU), to remove it from the resulting gas stream by Tritium

Removal System (TRS)

to route it to the Tritium Plant for final processing.

Development and Design of Tritium Extraction System, key factors:

SAFETY-WASTE: Tritium release, Inventory Tritium/Hydrogen

INTEGRATION: Physical size, complexity, synergy with tritium measurement and accountancy

system, volume of gas to be treated

PERFORMANCE: efficiency

OPERATION: Maintainability, Flexibility,

Reliability

ECONOMICS: Cost (R&D, capital, operation)

Page 3: ENEA Experience in PbLi Technologies · 11/15/2014  · ) ) ) E 1 - C J - p dsb abs (downstream) (2.17) 2 2 2)2G-p des (downstream) (2.18 KS,M and KS,LM are the Sieverts’ constants

DCLL status 1995-2012

1st EU-US DCLL Workshop

PbLi Loops 1995

Heat

exchanger

PbLi Loops 2013

Page 4: ENEA Experience in PbLi Technologies · 11/15/2014  · ) ) ) E 1 - C J - p dsb abs (downstream) (2.17) 2 2 2)2G-p des (downstream) (2.18 KS,M and KS,LM are the Sieverts’ constants

DCLL Breeder Blanket

TES

CPS

425°C

275°C

425°C

PMP pump

H2O

H2O

46.000kg/s

Heat exchanger

1. Solution

2. Diffusion

3. Transport of dissolved metal

4. Nucleation

5. Transport of crystallites

6. Crystal growth and sintering

(plug formation)

The issue of corrosion products precipitation in cold legs or near

megntic fields. Picture from OECD NEA Handbook of HLM V 1.0, Chap 6, in

publishing.

D2Storage tank

He Line

25% of mass flow rate

Preliminary PFD PbLi loop

T production 360 g/day 16 toroidal segment: 3 OB per sector, 2 IB per

sector n. recirculation x day: 100 Total PbLi mass fow rate: ~ 46.000kg/s N. PbLi loop: 16 PbLi mass flow rate x Segment: ~ 2875kg/s

Operative Conditions:

Page 5: ENEA Experience in PbLi Technologies · 11/15/2014  · ) ) ) E 1 - C J - p dsb abs (downstream) (2.17) 2 2 2)2G-p des (downstream) (2.18 KS,M and KS,LM are the Sieverts’ constants

Vacuum Permeators

CT,l,in CT,l,out

PbLi, T

T2

PbLi, T

permeable membrane Permeated

side

Liquid Boundary Layer Membrane Gas Boundary Layer

CT,l

C*T,l

C*T,M

C*T,g

)cc(hJ *l,Tl,Tll,T

Mass Transport

typologies: tube&shell

helicoidal tube

2*g,Trg,T ckJ

0.3460.913

17LiPbT,

tubel Sc Re 0.0096 D

Dh

correlation for the mass transfer coefficient in the liquid

boundary taken from literature for fluids different from PbLi

PROS and CONS for Vacuum Permeators

• High compactness, especially in the helicoidal tube configuration

• Being the overall tritium mass transfer strongly sensitive to hl, the tritium mass

transfer coefficient in the liquid boundary layer, its value needs to beexperimentally determined under relevant conditions. Present data fromliterature refer to fluids different from PbLi

• The metallic membrane needs to have significant tritium permeability and highcompatibility with PbLi under relevant operating conditions

• The metallic membrane needs to be resistant to oxidation in case of incidentalreduction or loss of vacuum (killing issue for Nb). Possible need of a coatinglayer (Pd?) on the vacuum side to keep the membrane oxidationunder control

• Never experimentally tested, even at small scale

)( 2,2, TiTggT PPkJ

iTaTrrT PkckJ ,22*

,

IF Liquid

Bulk

Liquid

Boundary

Layer

Gas

Boundary

Layer

Gas

Bulk

CT,l CT,l* Ks(PT2,i)0.5 RT

PT 2

Gas Liquid Contactors

Different typologies:

)cc(hJ *l,Tl,Tll,T

])Pkc

4

1(

2

1c[ha 5.0

2T2S

l,T

2l,TlvT

= kr/h l

Mass Transport

packed columns

bubble columns droplet spray columns

Net Tritium flow-rate

from PbLi into gas phase per unit volume

PROS and CONS for Gas Liquid Contactors

•Need to have low value of γ (high hl) and high value of av: this last point is verydifficult to be achieved by bubble columns and droplet stray column. With packed

columnsa reasonable value of av is assured by the packing itself

• GLCs need a downstream process for tritium concentration in He before routingtritium to the further tritium processingsystems upstreamthe refuelling stage

• Packed columns are large systems especially when large liquid flow-rates have tobe processed and high extractionefficiency is required

• Robust technology with much industrial experience

• Already tested at CEA (F) on Melodie loop, with 30% of extraction efficiencyachieved

Tritium fluxes in the different

liquid and gas regions

Tritium fluxes in the different

liquid and solid regions

η=𝑐𝐻 −𝑃𝑏𝐿𝑖

𝑖𝑛 −𝑐𝐻−𝑃𝑏𝐿𝑖𝑜𝑢𝑡

𝑐𝐻−𝑃𝑏𝐿𝑖𝑖𝑛

5

Tritium extraction from Pb-16Li

Gas Liquid Contactor:

Vacuum Permeator:

Tritium Extraction System Technologies:

- Bubble columns

- Packed columns

- Spray tower

Regenerable getters: This technology uses a tritium gettering

bed of metal in which the solubility of

tritium is higher than in lead lithium

A gas and a liquid phase are brought into contact for the purpose of a

diffusion interchange between them. Facilities: Melodie loop (CEA),

TRIEX (ENEA)

based on the phenomenon of tritium

permeation through a membrane Vacuum Permeators

CT,l,in CT,l,out

PbLi, T

T2

PbLi, T

permeable membrane Permeated

side

Liquid Boundary Layer Membrane Gas Boundary Layer

CT,l

C*T,l

C*T,M

C*T,g

)cc(hJ *l,Tl,Tll,T

Mass Transport

typologies: tube&shell

helicoidal tube

2*g,Trg,T ckJ

0.3460.913

17LiPbT,

tubel Sc Re 0.0096 D

Dh

correlation for the mass transfer coefficient in the liquid

boundary taken from literature for fluids different from PbLi

PROS and CONS for Vacuum Permeators

• High compactness, especially in the helicoidal tube configuration

• Being the overall tritium mass transfer strongly sensitive to hl, the tritium mass

transfer coefficient in the liquid boundary layer, its value needs to beexperimentally determined under relevant conditions. Present data fromliterature refer to fluids different from PbLi

• The metallic membrane needs to have significant tritium permeability and highcompatibility with PbLi under relevant operating conditions

• The metallic membrane needs to be resistant to oxidation in case of incidentalreduction or loss of vacuum (killing issue for Nb). Possible need of a coatinglayer (Pd?) on the vacuum side to keep the membrane oxidationunder control

• Never experimentally tested, even at small scale

)( 2,2, TiTggT PPkJ

iTaTrrT PkckJ ,22*

,

IF Liquid

Bulk

Liquid

Boundary

Layer

Gas

Boundary

Layer

Gas

Bulk

CT,l CT,l* Ks(PT2,i)0.5 RT

PT 2

Gas Liquid Contactors

Different typologies:

)cc(hJ *l,Tl,Tll,T

])Pkc

4

1(

2

1c[ha 5.0

2T2S

l,T

2l,TlvT

= kr/h l

Mass Transport

packed columns

bubble columns droplet spray columns

Net Tritium flow-rate

from PbLi into gas phase per unit volume

PROS and CONS for Gas Liquid Contactors

•Need to have low value of γ (high hl) and high value of av: this last point is verydifficult to be achieved by bubble columns and droplet stray column. With packed

columnsa reasonable value of av is assured by the packing itself

• GLCs need a downstream process for tritium concentration in He before routingtritium to the further tritium processingsystems upstreamthe refuelling stage

• Packed columns are large systems especially when large liquid flow-rates have tobe processed and high extractionefficiency is required

• Robust technology with much industrial experience

• Already tested at CEA (F) on Melodie loop, with 30% of extraction efficiencyachieved

Tritium fluxes in the different

liquid and gas regions

Tritium fluxes in the different

liquid and solid regions

Parameters Value

T production [g/day]

360

T PbLi [°C] 475

M PbLi [kg/s] 1.000÷3.000

Droplets tower: making small droplets in the vacuum,

tritium is released and collected by

vacuum line. Kyoto University

Page 6: ENEA Experience in PbLi Technologies · 11/15/2014  · ) ) ) E 1 - C J - p dsb abs (downstream) (2.17) 2 2 2)2G-p des (downstream) (2.18 KS,M and KS,LM are the Sieverts’ constants

PAV: Permeators Against Vacuum

PAV technologies is based on the phenomenon of tritium permeation through a membrane in

contact with Pb-15.7Li toward a secondary side where vacuum or a carrier gas is present.

PAV is a first choice process candidate due to its simplicity and reliability.

2

11

2

1212 P

mdesadsp (upstream) (2.14)

11111

1 Cdsbabsp

(upstream) (2.15)

x

CCDdp

21

(bulk) (2.16)

22222

1 Cabsdsbp

(downstream) (2.17)

2

222

desp (downstream) (2.18)

KS,M and KS,LM are the Sieverts’

constants of tritium in the membrane

and liquid metal

the pipe length is strongly depending

on the tritium mass transfer

coefficient through LBL

I. Ricapitoa, A. Ciampichetti, R. Lässer, Y. Poitevin, M. Utili, FUSION SCIENCE AND TECHNOLOGY VOL. 60 OCT. 2011

Page 7: ENEA Experience in PbLi Technologies · 11/15/2014  · ) ) ) E 1 - C J - p dsb abs (downstream) (2.17) 2 2 2)2G-p des (downstream) (2.18 KS,M and KS,LM are the Sieverts’ constants

drawback when using Nb/pure iron is that at high temperature it has a strong tendency to

oxidation, requiring a very high vacuum during operation and/or a surface layer of Pd

which is more oxidation resistant. This is a point of great importance, strongly impacting

PAV design.

[A. Ibarra, 1st EU–US DCLL Workshop Fuskite PbLi loop

Karlsruhe, April 23-24th 2013]

Fuskite loop (CIEMAT):

• New size of the test section

• Scale testing of permeation against

vacuum

• Perform measurements of permeation

in gas-phase and flowing PbLi

• Analyze permeation under a number of

controlled variables (T, P, velocity,

species)

Vacuum Permeators

CT,l,in CT,l,out

PbLi, T

T2

PbLi, T

permeable membrane Permeated

side

Liquid Boundary Layer Membrane Gas Boundary Layer

CT,l

C*T,l

C*T,M

C*T,g

)cc(hJ *l,Tl,Tll,T

Mass Transport

typologies: tube&shell

helicoidal tube

2*g,Trg,T ckJ

0.3460.913

17LiPbT,

tubel Sc Re 0.0096 D

Dh

correlation for the mass transfer coefficient in the liquid

boundary taken from literature for fluids different from PbLi

PROS and CONS for Vacuum Permeators

• High compactness, especially in the helicoidal tube configuration

• Being the overall tritium mass transfer strongly sensitive to hl, the tritium mass

transfer coefficient in the liquid boundary layer, its value needs to beexperimentally determined under relevant conditions. Present data fromliterature refer to fluids different from PbLi

• The metallic membrane needs to have significant tritium permeability and highcompatibility with PbLi under relevant operating conditions

• The metallic membrane needs to be resistant to oxidation in case of incidentalreduction or loss of vacuum (killing issue for Nb). Possible need of a coatinglayer (Pd?) on the vacuum side to keep the membrane oxidationunder control

• Never experimentally tested, even at small scale

)( 2,2, TiTggT PPkJ

iTaTrrT PkckJ ,22*

,

IF Liquid

Bulk

Liquid

Boundary

Layer

Gas

Boundary

Layer

Gas

Bulk

CT,l CT,l* Ks(PT2,i)0.5 RT

PT 2

Gas Liquid Contactors

Different typologies:

)cc(hJ *l,Tl,Tll,T

])Pkc

4

1(

2

1c[ha 5.0

2T2S

l,T

2l,TlvT

= kr/h l

Mass Transport

packed columns

bubble columns droplet spray columns

Net Tritium flow-rate

from PbLi into gas phase per unit volume

PROS and CONS for Gas Liquid Contactors

•Need to have low value of γ (high hl) and high value of av: this last point is verydifficult to be achieved by bubble columns and droplet stray column. With packed

columnsa reasonable value of av is assured by the packing itself

• GLCs need a downstream process for tritium concentration in He before routingtritium to the further tritium processingsystems upstreamthe refuelling stage

• Packed columns are large systems especially when large liquid flow-rates have tobe processed and high extractionefficiency is required

• Robust technology with much industrial experience

• Already tested at CEA (F) on Melodie loop, with 30% of extraction efficiencyachieved

Tritium fluxes in the different

liquid and gas regions

Tritium fluxes in the different

liquid and solid regions

preliminary sizing of a tube and shell PAV in niobium was carried

out in the frame of the design of the DCLL (Dual Coolant Lithium

Lead) BB for Aries-CS reactor, having a tritium generation rate of

340 g/d.

Page 8: ENEA Experience in PbLi Technologies · 11/15/2014  · ) ) ) E 1 - C J - p dsb abs (downstream) (2.17) 2 2 2)2G-p des (downstream) (2.18 KS,M and KS,LM are the Sieverts’ constants

GLC: Packed Columns

The packed columns are vertical columns filled with packing or other device providing a large interfacial surface between liquid and gas phase in both counter-current and cocurrent flow.

There are two groups of packing: • the random packing like rings • the regular or structured packing like layered sheets

The main characteristics of packed columns are:

Packed Column

Liquid in Lin , xin

Liquid out Lout , xout

Gas in Gin , yin

Gas out Gout , yout

Advantages: • reliable injection system, because it is not necessary to inject small size bubbles • reliability of the functional answer because of the kinetics of mass transfer • the packing material could be manufactured with high corrosion resistance materials to

Pb-15.7Li • the Packed columns, used as tritium extraction from lead lithium, have been tested

extensively in the past in Melodie loop at CEA

𝐽𝑇 = 𝐾𝐷 𝑐𝑇,𝑙 − 𝑐𝑇,𝑒𝑞

Page 9: ENEA Experience in PbLi Technologies · 11/15/2014  · ) ) ) E 1 - C J - p dsb abs (downstream) (2.17) 2 2 2)2G-p des (downstream) (2.18 KS,M and KS,LM are the Sieverts’ constants

experimental results on Melodie loop - 800 mm height, 54 mm diameter, packing area: 750 m2/m3, T:673 K

Disadvantages: Lower rate size/η (tritium extraction efficiency for one column is 25-30%) than permeators. In any case the size of the columns is a consequence of its efficiency, and the design of the columns can be optimised.

L/G =7

Test n. LM flow-rate

(lh-1)

Ar flow-rate

(N lh-1)

PH2,in

(Pa)

(%)

10 70-90 6 1200-1350 20-22

11 30-50 6 1000-1100 29-31

12 30-50 30 975-1000 29-31

13 30-50 6 450-475 23-25

14 30-50 6 220-230 23-25

GLC: Packed Columns

Page 10: ENEA Experience in PbLi Technologies · 11/15/2014  · ) ) ) E 1 - C J - p dsb abs (downstream) (2.17) 2 2 2)2G-p des (downstream) (2.18 KS,M and KS,LM are the Sieverts’ constants

GLC – Packed column

The extractor column, used for the stripping of the hydrogen contained in the eutectic alloy Pb–16Li, is of the filled type, in counter flow. The liquid phase, represented by the Pb–16Li alloy, enters in the column from the top, passing through the filler, in hydrogen saturated conditions. The real hydrogen content is read by a hydrogen sensor in liquid metal. The gaseous phase, represented by pure argon, is injected in the column from the bottom through an appropriate system of distribution that has the function to uniform and fragment the gas bubbles.

Barelli B1 350

Material AISI 304

Tipe B1-350

Spec. surface [m2/m3] 350

Loading specific volumetric

flow[m3/m2h)] 250

Extractor:

C

B

C

B

D D

L.T.

L.S.

L.T.

L.S.

Page 11: ENEA Experience in PbLi Technologies · 11/15/2014  · ) ) ) E 1 - C J - p dsb abs (downstream) (2.17) 2 2 2)2G-p des (downstream) (2.18 KS,M and KS,LM are the Sieverts’ constants

𝜼 =𝟏

𝑳𝒗𝒐𝒍 ∗𝟏

𝑺𝑲𝑫+

𝟏𝟐𝑮𝒎𝒐𝒍𝑽𝑴𝑨𝒓

Determination of the efficiency with the partial pressures: 𝒄𝑯 = 𝒌𝑺 𝑷𝑯

𝜼 =𝒌𝑺 𝑷𝒊𝒏 − 𝒌𝑺 𝑷𝒐𝒖𝒕

𝒌𝑺 𝑷𝒊𝒏

=𝑷𝒊𝒏 − 𝑷𝒐𝒖𝒕

𝑷𝒊𝒏

0

0,02

0,04

0,06

0,08

0,1

0,12

0,14

0,16

0

5

10

15

20

25

30

35

40

11

:50

:00

10

:15

:00

08

:40

:00

07

:05

:00

05

:30

:00

03

:55

:00

02

:20

:00

00

:45

:00

23

:10

:00

21

:35

:00

20

:00

:00

18

:25

:00

16

:50

:00

15

:15

:00

13

:40

:00

12

:05

:00

10

:30

:00

08

:55

:00

07

:20

:00

05

:45

:00

04

:10

:00

02

:35

:00

Hyd

roge

n p

arti

al p

ress

ure

[b

ar]

Extr

acti

on

eff

icie

ncy

[%

]

Efficiency

TheoreticalEfficiency

GLC: Packed Columns

Page 12: ENEA Experience in PbLi Technologies · 11/15/2014  · ) ) ) E 1 - C J - p dsb abs (downstream) (2.17) 2 2 2)2G-p des (downstream) (2.18 KS,M and KS,LM are the Sieverts’ constants

Droplets and Gas-liquid counter-current extraction tower or vacuum sieve tray

By making small droplets in the vacuum, tritium released from droplets is collected by

vacuum pumping system.

A recent study at Kyoto University indicated interesting results on the vacuum sieve tray

approach

tritium release from LiPb is governed by diffusion-limited process

Fusion Engineering and

Design (2012), 87(7-8):

1014-1018

Page 13: ENEA Experience in PbLi Technologies · 11/15/2014  · ) ) ) E 1 - C J - p dsb abs (downstream) (2.17) 2 2 2)2G-p des (downstream) (2.18 KS,M and KS,LM are the Sieverts’ constants

Parameters Value

Temperature [°C] 400

P H2 [Pa] 2.5x104

Nozle radius [mm] 1

Extraction environment Vacuum

Droplet radius Rd

Experimentally obtained

values:

Rd = 0.9mm

l0 = ~20mm

Multi-stage

Mass Flow rate: 0,724 m3/s

(6.440kg/s)

Diameter: 2,1m

h= 1m

Efficiency: 45%

One - stage

Mass Flow rate:

0,724 m3/s

(6.440kg/s)

Diameter: 4,6m

h= 6-7 m

Efficiency: 90%

Droplets and Gas-liquid counter-current extraction tower or vacuum sieve tray

Fusion Engineering and Design

(2012), 87(7-8): 1014-1018

Page 14: ENEA Experience in PbLi Technologies · 11/15/2014  · ) ) ) E 1 - C J - p dsb abs (downstream) (2.17) 2 2 2)2G-p des (downstream) (2.18 KS,M and KS,LM are the Sieverts’ constants

SAFETY-WASTE: Tritium release, Inventory Tritium/Hydrogen

INTEGRATION: Physical size, complexity, synergy with tritium measurement and

accountancy system, volume of gas to be treated

PERFORMANCE: efficiency

OPERATION: Maintainability, Flexibility, Reliability

ECONOMICS: Cost (R&D, capital, operation, power required)

GLC – Packed Tower

PAV GLC- Droples

SAFETY-WASTE

INTEGRATION Volume of gas to be treated, physical size

Physical size

PERFORMANCE 30% 69%-90% 45-90%

OPERATION

• Reliability

• Maintainability

• Flexibility: floading loading condition

• Reliability

• Maintainability

• Flexibility

• Reliability

• Maintainability

• Flexibility

ECONOMICS