11

Radioisotope Production at Los Alamos National Laboratory

Presented at Specialization School on Health PhysicsSpecialization School on Health Physics

UniversitaUniversita’’ degli Studi di Milanodegli Studi di MilanoBy Dennis R. Phillips

Radioisotope Applications and ProductionIsotope and Nuclear Chemistry Group

March 21, 2002

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Los Alamos Neutron Science Los Alamos Neutron Science CenterCenter(LANSCE)(LANSCE)

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Beam StopLine D

Line XLine A800 MeV

Side Couple Cavity Linac805 MHz

H+

H-

TransitionRegion

Drift Tube Linac

201.25 MHz

100 MeV750 keV

H+

H-

H-

ProtonInjectors

New 100MeV Isotope Production Facility (Under Construction) Existing

Isotope ProductionStation

SCCL is 90% of accelerator length

LANSCE Accelerator Complex

Proton Storage Ring

Weapons Neutron Research Facility

Manuel Lujan, Jr. Neutron Scattering Center

LANSCE Accelerator ComplexLANSCE Accelerator Complex

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Los Alamos Hot Cell FacilityLos Alamos Hot Cell Facility

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LANSCELANSCE SpallationSpallation TargetTarget

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Historically Produced Historically Produced Spallation Spallation IsotopesIsotopes

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• SrSr--82 (t82 (t1/21/2 = 25.4 d)/= 25.4 d)/RbRb--82 (t82 (t1/21/2 = 1.26 m)= 1.26 m)• RubidiumRubidium--82 used for PET myocardial 82 used for PET myocardial

perfusion imagingperfusion imaging• Distributed byDistributed by BraccoBracco DiagnosticsDiagnostics• Manufactured first by Bristol Myers Squibb Manufactured first by Bristol Myers Squibb

until May 2001; Now by until May 2001; Now by AmershamAmersham MedicalMedical

The The CardioGenCardioGen® PET GeneratorPET Generator

88

0

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40

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120

1 11 21 31 41 51 61 71 81 91 101

Mass Number

Be-7 =1 x 1017

Na-22 =4 x 1015

Cr-51 =2 x 1015

Co-58 =2 x 1016

Se-75 =8 x 1017

Rb-83 =1 x 1018

Sr-82 =2 x 1018

Zr-88/Y-88 =5 x 1018

Tc-95m =1 x 1017

Sr-85 =3 x 1018

Yield (# of Atoms)

0 10 20 30 40 50 60 70 80 90 100

400 – 500 g Mo metal puck800 MeV protons0.6 – 1 mA beam current100, 000 – 200,000 mA-hours~10 Ci Sr-82 produced

SpallationSpallation ProductionProduction

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LANL Mo Target ProcessLANL Mo Target Processfor for SrSr--82*82*

• Dissolve target in 30% HDissolve target in 30% H22OO22

• Pass solution through cation exchange columnPass solution through cation exchange column• Wash with 10% HWash with 10% H22OO22

• Elute column 6 M HClElute column 6 M HCl• Convert to 0.1 M HClConvert to 0.1 M HCl• Load onto new cation columnLoad onto new cation column• Wash column with 0.5 M HWash column with 0.5 M H22SOSO44

• Elute SrElute Sr--82 with 1 M82 with 1 M HClHCl

*Details in: R. C. Heaton, D. J. Jamriska, W. A. Taylor: U. S. Patent Number 5,167,938 (1992).

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Virtual Isotope CenterVirtual Isotope Center

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Proton Energy (MeV)

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Sr-85Sr-84Sr-83Sr-82

Sr-81Sr-80

Sr-79Sr-78

SrSr--82 Production on 82 Production on Rb Rb Containing TargetsContaining Targets

natRb(p,xn)82Sr

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50

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Proton energy (MeV)

Cro

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Deptula et al. (1990)

Lagunas-Solar (1992)

Horiguchi at al. (1980) [X 0.7217]

NAC data (2000)

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RbRb, , RbClRbCl Yield ComparisonYield ComparisonRb(p,xn)Sr-82 (NAC experimental data)

0

0.1

0.2

0.3

0.4

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0.7

0.8

0.9

30 40 50 60 70 80 90 100

Proton Energy (MeV)

Th

ick

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mC

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Rb metal target

RbCl target

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Croft CU112C Shipping ContainerCroft CU112C Shipping Container

• CU 112C SpecificationsCU 112C Specifications– DOT/IAEA Type A DOT/IAEA Type A – 30 gal SS Drum Outer 30 gal SS Drum Outer

Assembly (17 kg)Assembly (17 kg)– SS/Lead Pot Inner SS/Lead Pot Inner

Container (328 kg)Container (328 kg)• Inner CavityInner Cavity

– 7.19 cm Diameter7.19 cm Diameter– 16.5 cm Height16.5 cm Height

1414

INR INR RbRb TargetTarget

• 50 g50 g Rb Rb • 94 94 -- 101101 MeVMeV Incident Incident

Protons, up to 130Protons, up to 130 µµAAbeam currentbeam current

• 6800 microampere hours 6800 microampere hours (2 (2 –– 3 days irradiation 3 days irradiation time, ~30 days before time, ~30 days before delivery date)delivery date)

• 15001500 mCi SrmCi Sr--82 at delivery 82 at delivery datedate

1515

INR Rb Target Process (1)*INR Rb Target Process (1)*

• Dissolve target in 2Dissolve target in 2--propanolpropanol in Argon in Argon inertedinertedatmosphereatmosphere

• Convert rubidium propoxide to RbClConvert rubidium propoxide to RbCl• Dissolve RbCl in 6 M HClDissolve RbCl in 6 M HCl• Pass through anion column to remove ironPass through anion column to remove iron• Evaporate eluate to dryness Evaporate eluate to dryness

*Details in: Radiochim. Acta 8888, 149 – 155 (2000)

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INR Rb Target Process (2)INR Rb Target Process (2)

• Dissolve RbCl in 0.1 M NHDissolve RbCl in 0.1 M NH33/NH/NH44++ buffer buffer

solution (pH 9 solution (pH 9 -- 10); filter to remove Al10); filter to remove Al• Pass filtrate through Pass filtrate through Chelex Chelex 100 ion exchange 100 ion exchange

column; column; SrSr retained, retained, Rb Rb in in eluate eluate • Wash column with buffer, then waterWash column with buffer, then water• Elute SrElute Sr--82 with 4 M HCl82 with 4 M HCl• Evaporate to drynessEvaporate to dryness• Dissolve in 0.1 M HClDissolve in 0.1 M HCl

1717

INR Target Process (3)INR Target Process (3)

• Pass through cation column (Sr retained, trace Pass through cation column (Sr retained, trace rubidium and “color” in rubidium and “color” in eluateeluate))

• Wash gradiently with 0.1, 0.5, and 1.0 M HClWash gradiently with 0.1, 0.5, and 1.0 M HCl• Elute SrElute Sr--82 from column with 4 M HCl82 from column with 4 M HCl• Evaporate eluate to drynessEvaporate eluate to dryness• Add Concentrated HNOAdd Concentrated HNO33 to residue and evaporate to residue and evaporate

to drynessto dryness• Convert back to chloride, 0.1 M HCl product Convert back to chloride, 0.1 M HCl product

solutionsolution

1818

NAC RbCl Target IrradiationNAC RbCl Target Irradiation

• 8 8 -- 9 g RbCl9 g RbCl• 66 66 -- 40 40 MeV MeV

protonsprotons• 80 microampere 80 microampere

beam currentbeam current• 5000 5000

microamperemicroampere--hourshours• 500 500 -- 700 700 mCi mCi

SrSr--82 EOB82 EOB

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NAC RbCl Target Process (1)NAC RbCl Target Process (1)

• Dissolve target in water, Evaporate to drynessDissolve target in water, Evaporate to dryness• Dissolve residue in 0.1 M NHDissolve residue in 0.1 M NH33/NH/NH44

++ buffer buffer solution (pH 9 solution (pH 9 --10)10)

• Wash column with buffer, then waterWash column with buffer, then water• Elute SrElute Sr--82 with 6 M HCl82 with 6 M HCl• Evaporate to drynessEvaporate to dryness• Dissolve in 0.1 M HClDissolve in 0.1 M HCl

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NAC RbCl Target Process (2)NAC RbCl Target Process (2)

• Pass through cation column (Sr retained)• Wash gradiently with 0.1, 0.5, and 1.0 M HCl• Elute Sr-82 from column with 4 M HCl• Evaporate eluate to dryness• Add Concentrated HNO3 to residue and

evaporate to dryness• Convert back to chloride, 0.1 M HCl product

solution

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100 100 MeVMeV Isotope ProductionIsotope ProductionFacility SchematicFacility Schematic

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IPF beam lineIPF beam line

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IPF Beam LineIPF Beam Line

Bending Magnet

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Los Alamos Neutron Science Los Alamos Neutron Science CenterCenter(LANSCE)(LANSCE)

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Components in TR into IPFComponents in TR into IPF

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IPF buildingIPF building

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IPF buildingIPF building

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IPF Hot CellIPF Hot Cell

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Target box & target cooling skidTarget box & target cooling skid

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Target boxTarget box

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100 100 MeVMeV Target BoxTarget Box

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100 100 MeV MeV Target AssemblyTarget Assembly

Proton Beam

Beam Exit WindowLow-E Target

Cooling Water

High-E Target

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100 100 MeVMeV IPF Project SummaryIPF Project Summary

1.2.1 Facility Design 10.81.2.2 SFE Design 11.71.2.3 Project Management 12.61.2.4 Facility Construction 32.81.2.4 SFE Construction 27.91.2.5 System Testing 0.0

Contingency 4.2

WBS Description Percent Project Completion: 82%BCP Approved 10/29/01UC Milestone #1 Achieved 12/19/01UC Milestone #2 Achieved 01/11/02C.P.I = 1.01; S.P.I = 0.99

Baseline Schedule Complete: September 2003

IPF TEC

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GeGe--68 Production on Gallium68 Production on Gallium(IAEA Evaluated Data)(IAEA Evaluated Data)

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ALICE Excitation Functions for ALICE Excitation Functions for Proton Reactions on NiobiumProton Reactions on Niobium

Cross sections (mbarn)

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Nb(p,6n)Mo-88

Nb(p,p5n)Nb-88

Nb(p,2p4n)Zr-88

Zr-88 yield(cumulative)Nb(p,3p3n)Y-88

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ZrZr--88 Production on Niobium88 Production on NiobiumNb-93(p,x)Zr-88 (theoretical data)

0.0001

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Nb(p,p5n)Nb-88

Nb(p,2p4n)Zr-88

Zr-88 yield (cumulative)

Nb(p,3p3n)Y-88

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GeGe--68/68/ZrZr--88 88 Integrated Target Process (1)Integrated Target Process (1)

• Place gallium target (~4 g) and niobium Place gallium target (~4 g) and niobium encapsulation (~5 g) in ~ 60 encapsulation (~5 g) in ~ 60 mLmL Conc. HFConc. HF

• Slowly add ~ 10 Slowly add ~ 10 mLmL Conc. HNOConc. HNO33 to dissolveto dissolve• Add ~15 Add ~15 mLmL Conc. HConc. H22SOSO4 4 ; reduce volume by ; reduce volume by

evaporation to ~15 evaporation to ~15 mL mL to remove HFto remove HF• Add ~120 Add ~120 mL mL Conc. Conc. HClHCl• Extract Extract GeGe into CClinto CCl44

• Back extract Back extract Ge Ge into Hinto H22OO

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GeGe--68/68/ZrZr--88 88 Integrated Target Process (2)Integrated Target Process (2)

• Pass the germanium depleted aqueous target Pass the germanium depleted aqueous target solution through 5 solution through 5 -- 15 g15 g aluminaalumina column column (equilibrated with 12 M (equilibrated with 12 M HClHCl))

• ZrZr--88/Y88/Y--88 retained on column88 retained on column• Rinse column 2x with 12 M Rinse column 2x with 12 M HCl HCl to remove to remove

gallium and niobium massgallium and niobium mass• Elute Elute ZrZr--88 from column with solution of 88 from column with solution of

1M HF/1M HCL; Y1M HF/1M HCL; Y--88 retained88 retained

3939

Representative Target StacksRepresentative Target Stacks

1st 28 day periodSTACK # 1a STACK # 2 STACK # 3a Totals

Beam Current (µA) 125 125 125 125 125 125 125 125 125 EOB DeliveryBombardment time (days) 3.50 3.50 3.50 20.50 20.50 20.50 2.00 2.00 2.00 Sr-82 3063 2661 2 targetsTarget Nb RbCl Ga NaCl Mg Ga Cr Zn W-186 Ge-68 2252 1850 2 target

Isotope Zr-88 Sr-82 Ge-68 Si-32 Na-22 Ge-68 V-48 Cu-67 Re-186 Cu-67 1068 1068Halflife (days) 83.4 25.5 270.82 62823 950.7 270.82 15.97 2.6 3.72 As-73 0 0Production rate (mCi/µAh) 0.235 0.230 0.032 0.000 0.024 0.032 1.100 0.115 0.050 Na-22 1471 1456Yield at EOB (mCi) 2432 2304 334 0.0184 1471 1917 6322 534 250 Si-32 0.0184 0.0184Decay time (days) 0.00 4.00 4.00 14.00 14.00 14.00 0.00 V-48 6322 6322Yield after decay (mCi) 2432 2066 331 0.0184 1456 1850 6322 534 250 Zr-88 2432 2432

STACK # 3b Re-186 501 501Beam Current (µA) 125 125 125Bombardment time (days) 2.00 2.00 2.00Target RbCl Zn W-186

Isotope Sr-82 Cu-67 Re-186Halflife (days) 25.5 2.6 3.72Production rate (mCi/µAh) 0.130 0.115 0.050Yield at EOB (mCi) 759 534 250Decay time (days) 9.00Yield after decay (mCi) 594 534 250

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Representative Target StacksRepresentative Target Stacks

2nd 28 day periodSTACK # 1b STACK # 2 STACK # 3b Totals

Beam Current (µA) 125 125 125 125 125 125 125 125 125 EOB DeliveryBombardment time (days) 2.00 2.00 2.00 16.50 16.50 16.50 2.00 2.00 2.00 Sr-82 3621 2942 4 targetsTarget RbCl RbCl Ge NaCl Mg Ga RbCl Zn W-186 Sr-82 5517 2577 2 targets

Isotope Sr-82 Sr-82 As-73 Si-32 Na-22 Ge-68 Sr-82 Cu-67 Re-186 Ge-68 2075 2021 2 targetsHalflife (days) 25.5 25.5 80.3 62823 950.7 270.82 25.5 2.6 3.72 Cu-67 1068 1068Production rate (mCi/µAh) 0.130 0.230 0.171 0.000 0.024 0.032 0.130 0.115 0.050 As-73 1017 1017Yield at EOB (mCi) 759 1343 1017 0.0148 1186 1551 759 534 250 Na-22 1186 1174 2630Decay time (days) 4.00 4.00 14.00 14.00 14.00 21.00 Si-32 0.0148 0.0148 0.033Yield after decay (mCi) 681 1205 1017 0.0148 1174 1496 429 534 250 V-48 0 0

STACK # 1c STACK # 3b Zr-88 0 0Beam Current (µA) 125 125 125 125 125 125 Re-186 501 501Bombardment time (days) 5.50 5.50 5.50 2.00 2.00 2.00Target RbCl RbCl Ga RbCl Zn W-186

Isotope Sr-82 Sr-82 Ge-68 Sr-82 Cu-67 Re-186Halflife (days) 25.5 25.5 270.82 25.5 2.6 3.72Production rate (mCi/µAh) 0.130 0.230 0.032 0.130 0.115 0.050Yield at EOB (mCi) 1992 3525 524 759 534 250Decay time (days) 28.00 28.00 7.00Yield after decay (mCi) 931 1647 524 628 534 250

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Operations ModelOperations ModelIPF Operating Schedule

0 1 2 3 4 5 6 7

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Week 3

Week 4

Week 5

Week 6

Week 7

Week 8

Time (days)

Stack 1a (Zr-88/Sr-82/Ge-68) Stack 1b (Sr-82/Sr-82/As-73) Stack 1c (Sr-82/Sr-82/Ge-68)Stack 2 (Si-32/Na-22/Ge-68) Stack 3a (V-48/Cu-67/Re-186) Stack 3b (Sr-82/Cu-67/Re-186)

BEAM TIME ALLOCATION (%)

7%4%

9%

66%

4%

11%

Stack 1a (Zr-88/Sr-82/Ge-68)

Stack 1b (Sr-82/Sr-82/As-73)

Stack 1c (Sr-82/Sr-82/Ge-68)

Stack 2 (Si-32/Na-22/Ge-68)

Stack 3a (V-48/Cu-67/Re-186)

Stack 3b (Sr-82/Cu-67/Re-186)

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LANL RAP TeamLANL RAP Team

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Los Alamos Hot Cell FacilityLos Alamos Hot Cell Facility

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