H2 H , D , T Hydrogen Isotope 2 Separation Process 2 T2 … · 2015. 8. 28. · Batch Cryogenic distillation column replaced by TCAP 2004 Comp.-free CTC concept developed 2006 Comp.-free

Advances in Hydrogen Isotope Separation Using Thermal Cycling Absorption Process (TCAP)

X. Steve Xiao

Contributions: L.K. Heung, H.T. Sessions, S. Redd

H2

D2

T2

H2, D2, T2 Hydrogen Isotope Separation Process

H2

D2

T2

H2

D2

T2

H2

D2

T2

H2, D2, T2 Hydrogen Isotope Separation ProcessHydrogen Isotope Separation Process

2

Hydrogen Isotope Separation Timeline

Discovery of deuterium 1931

Discovery of tritium 1934

Isotope separation in SRS

–Thermal diffusion 1957-1986

–Fractional absorption 1964-1968

–Batch Cryogenic distillation 1967-2004

–TCAP 1994-present

3

TCAP Advance ContinuesTCAP concept invented at SRL 1980Experimental TCAP achieved 97% purity (D2, H2 ) 1983Prototype TCAP achieved 99% purity (D2, H2) 1989Pilot TCAP demonstrated (production-configured) 1993Production TCAP achieved target T2/D2 separation 1994Compact TnT design tested at LANL 2001Batch Cryogenic distillation column replaced by TCAP 2004Comp.-free CTC concept developed 2006Comp.-free CTC experiment reached 4,000 cycles 2009Inverse Column achieved 2X+ capacity & higher purity 2009Micro-TCAP (batch) for LLE 2013Mini-TCAP for Shine Medical Technologies 2014CTC-TCAP with inverse column for SRS Tritium plant 2014+

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Advance 1: Inverse Column

Pd/k – PFR configuration Pd/k – Inverse Column configuration

FCV

Feed

Product

Raffinate

PCV RCV RGA

Pd/k column PFR

FCV

Feed

Product

Raffinate

PCV RCV RGA

Pd/k column PFR

FCV

Feed

Product

Raffinate

PCV RCV RGA

Pd/k column PFR

FCV

Feed

Product

Raffinate

PCV RCV RGA

Pd/k column MS column

FCV

Feed

Product

Raffinate

PCV RCV RGA

Pd/k column MS column

FCV

Feed

Product

Raffinate

PCV RCV RGA

Pd/k column MS column

5

Mini-TCAP with Inverse Column Experimental Unit

6

Throughput Doubled!Pd/k-PFR configuration vs. Pd/k-MS configuration

0.0

0.10.2

0.3

0.4

0.5

0.6

0.7

0.8

0.9

1.0

0 10 20 30 40 50 60 70 80Cycle Number

Frac

tion

D2/

(D2+

H2)

Prod Raff

Prod Raff

Cycle # Feed (sl/cycle) 1-22 1 23-34 2 35-64 3 65-77 4

1 2 3 4

Pd/k - PFR:

Pd/k - MS:

7

T2 Inventory Reduction – to 1/2

Mini-TCAP Reduces T2 Inventory by ½ & possibly more

Present TCAP

FeedT2+H2

ProductT2

RaffinateH2

Pd/kcolumn with hot/cold jacket

Plugflowreverser (passive)

Present TCAP

FeedT2+H2

ProductT2

RaffinateH2

Pd/kcolumn with hot/cold jacket

Plugflowreverser (passive)

FeedT2+H2

ProductT2

RaffinateH2

Pd/kcolumn with hot/cold jacket

Plugflowreverser (passive)

FeedT2+H2

ProductT2

RaffinateH2

Pd/kcolumn with hot/cold jacket

Plugflowreverser (passive)

Advanced TCAP

FeedT2+H2

ProductT2

RaffinateH2

Pd/kColumn with thermal cyling

MS column with thermal cycling (active)

Mini-TCAP Reduces T2 Inventory by ½ & possibly more

Present TCAP

FeedT2+H2

ProductT2

RaffinateH2

Pd/kcolumn with hot/cold jacket

Plugflowreverser (passive)

Present TCAP

Mini-TCAP Reduces T2 Inventory by ½ & possibly more

Present TCAP

FeedT2+H2

ProductT2

RaffinateH2

Pd/kcolumn with hot/cold jacket

Plugflowreverser (passive)

Present TCAP

FeedT2+H2

ProductT2

RaffinateH2

Pd/kcolumn with hot/cold jacket

Plugflowreverser (passive)

FeedT2+H2

ProductT2

RaffinateH2

Pd/kcolumn with hot/cold jacket

Plugflowreverser (passive)

FeedT2+H2

ProductT2

RaffinateH2

Pd/kcolumn with hot/cold jacket

Plugflowreverser (passive)

FeedT2+H2

ProductT2

RaffinateH2

Pd/kcolumn with hot/cold jacket

Plugflowreverser (passive)

FeedT2+H2

ProductT2

RaffinateH2

Pd/kcolumn with hot/cold jacket

Plugflowreverser (passive)

Advanced TCAP

FeedT2+H2

ProductT2

RaffinateH2

Pd/kColumn with thermal cyling

MS column

FeedT2+H2

ProductT2

RaffinateH2

Pd/kcolumn with hot/cold jacket

Plugflowreverser (passive)

Advanced TCAP

FeedT2+H2

ProductT2

RaffinateH2

Pd/kColumn with thermal cyling

MS column with thermal cycling (active)

8

Advance 2: Extremely Compact Column Design

Better heat transfer with counter-flow

Replacement of heater possible

LN2 liquid

9

Heat Load Reduction – to 25%

ComponentsHeat Load

Present Design Mini Design

Total (relative) 100 25

Packing material 10 % 24 %

Column 16 % 38 %

Jacket/Cooling tube 74 % 38 %

Mini DesignN2?

N2?

Present DesignN2?

N2?

Present DesignN2?

N2?

Present Design

10

Advance 3: Equipment & Footprint Reduction to 1/10th

Column

Jacket

Compressors RefrigerationWater/air

HeatingHot/cold N2Column

Jacket

Compressors RefrigerationWater/air

HeatingColumn

Jacket

Compressors RefrigerationWater/air

HeatingHot/cold N2

ColumnHeating

Liquid N2

Gas N2Cooling tubeHeater

CTC

ColumnHeating

Liquid N2

Gas N2Cooling tubeHeater

CTC

Present TCAP System

Compressor-free CTC-TCAP System

11

CTC-TCAP Experimental Unit

12

Advance 4: Micro-System Fits into a Small Glovebox

13

Micro-TCAP Typical T and P Cycles

14

Advance 5: Parameter Optimized with 50% Efforts

2112122812211227121221262121212511222214221122132222111211111111

D (gas to middle)

AxDBxC

AxCBxD

C (hi press)

AxBCxD

B (Delta P)

A (inventory)

TestNo.

Experimental Design via Taguchi’s methods: orthogonal arrays

15

Reduced Cycles from 20 To 10Micro-TCAP Concentration Profile (Feed V16)

0

20

40

60

80

100

0 1000 2000 3000 4000 5000Column Gas Quantity, std cc

Con

cent

ratio

n, %

D%H%

16

Summary of Benefits

Double throughput;

Reduction of tritium inventory to 1/2;

Reduction of heat load to 25%;

Footprint Reduction to 1/10th;

Miniature version fit into a small glovebox;

Reduced workload by implementing Experimental Design – potential incentive in other tritium work.

Collaboration with Dr. Walter T. Shmayda – Laboratory for Laser Energetics, University of Rochester, for Micro-TCAP development is acknowledged.